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AECL-8364

ATOMIC ENERGY £ 2 ^ L'ENERGIE ATOMIQUEOF CANADA LIMITED T ^ 9 DU CANADA, LIMITEE

SOIL NUCLIDE DISTRIBUTION COEFFICIENTS

AND THEIR STATISTICAL DISTRIBUTIONS

COEFFICIENTS DE REPARTITION DES NUCLIDES DANS LE SOL

ET LEUR REPARTITION STATISTIQUE

Marsha I. Sheppard, Donald I. Beals, Denis H. ThibaultPatrick O'Connor

Whiteshell Nuclear Research Etablissement de recherchesEstablishment nucleaires de Whiteshell

Pinawa, Manitoba ROE 1 LODecember 1984 decembre

\Miuiv 1 nc:i; \ ol ( I mined. ll;,s4

ATOMIC ENERGY OF CANADA LIMITED



by

Marsha I . Sheppard, Donald I . Beals, Denis H. Thibault

and Patr ick O'Connor

Whlteshell Nuclear Research EstablishmentPinawa, Manitoba ROE 1L0

1984 DecemberAECL-8364

COEFFICIENTS DE REPARTITION DES NUCLIDES DANS LE SOL

ET LEUR REPARTITION STATISTIQUE

par

Marsha I. Sheppard, Donald I. Beals, Denis H. Thibaultet Patrick O'Connor

RESUME

Les §valuations ecologiques de 1'evacuation des dSchets de combus-tible nuclSaire dans les formations de roche plutonique nScessitent uneanalyse de la migration des nuclides qui passent de 1*enceinte d1Evacuationa la biosphSre. Pour I1analyse de la migration des nuclides a travers 1'en-ceinte d'Svacuation, les matSriaux tampons et de remblayage, la roche pluto-nique et les raorts-terrains consolid§s et non consolidis, par l'entremise del'eau souterraine, on se sert de modules necessitant des coefficients derepartition (Kd) pOur decrire 1'interaction des nuclides et des materiauxgSologiques et artificiels. Ce rapport prSsente des coefficients de repar-tition dans le sol particuliers a certains elSments et leur ripartition dupoint de vue statistique, a partir d'une etude bibliographique en detail.Les elements radioactifs considers furent les suivants: actinium, ameri-cium, bismuth, calcium, carbone, cerium, cesium, iode, plomb, raolybdene,neptunium, nickel, niobium, palladium, plutonium, polonium, protactinium,radium, samarium, selenium, argent, strontium, technetium, terbium, thorium,etain, uranium et zirconium. Les el&ments stables consideres furent lessuivants: antimoine, bore, cadmium, tellure et zinc- Lorsque la disponlbi-lite des donn§es le permet, les coefficients de repartition et leur reparti-tion sont indiques pour les sols sabloneux, limoneux, argileux et organi-ques. L'utilisation de nos valeurs est recoramandee pour les evaluationseffectuSes dans le cadre du programme canadien de gestion des dSchets decombustible nuclgaire.

L'Energie Atomique du Canada, LimiteeEtablissement de recherches nuclfiaires de Whiteshell

Pinawa, Manitoba ROE 1L01984 decembre

AECL-8364



by

Marsha I. Sheppard, Donald I. Beals, Denis H. Thibaultand Patrick O'Connor

ABSTRACT

Environmental assessments of the disposal of nuclear fuel waste inplutonic rock formations require analysis of the migration of nuclldes fromthe disposal vault to the biosphere. Analyses of nuclide migration viagroundwater through the disposal vault, the buffer and backfill, the pluto-nic rock, and the consolidated and unconsolidated overburden use modelsrequiring distribution coefficients (KJ) to describe the interaction of thenuclides with ;he geological and man-made materials. This report presentselement-specific soil distribution coefficients and their statistical dis-tributions, based on a detailed survey of the literature. Radioactive ele-ments considered were actinium, americium, bismuth, calcium, carbon, cerium,cesium, iodine, lead, molybdenum, neptunium, nickel, niobium, palladium,Plutonium, polonium, protactinium, radium, samarium, selenium, silver,strontium, technetium, terbium, thorium, tin, uranium and zirconium. Stableelements considered were antimony, boron, cadmium, tellurium and zinc.Where sufficient data were available, distribution coefficients and theirdistributions are given for sand, silt, clay and organic soils. Our valuesare recommended for use in assessments for the Canadian Nuclear Fuel WasteManagement Program.

Atomic Energy of Canada LimitedWhiteshell Nuclear Research Establishment

Pinawa, Manitoba ROE 1L01984 December

AECL-8364

TABLE OF CONTENTS

3.13.23.33.43.53.63.73.83.93.103.11

ACTINIUMAMERICIUMBISMUTHLEADNEPTUNIUMPOLONIUMPLUTONIUMPROTACTINIUMRADIUMTHORIUMURANIUM

1. INTRODUCTION

2. DISTRIBUTION COEFFICIENT, Kd 2

3. DISTRIBUTION COEFFICIENTS FOR THE ACTINIDES 5558810131720202326

4. DISTRIBUTION COEFFICIENTS FOR FISSION PRODUCTS 294.1 CALCIUM 294.2 CARBON 294.3 CESIUM 304.4 IODINE 334.5 MOLYBDENUM 364.6 NICKEL 364.7 PALLADIUM 374.8 RARE EARTHS - TERBIUM, SAMARIUM AND CERIUM 384.9 SELENIUM 394.10 SILVER 394.11 STRONTIUM 414.12 TECHNETIUM 464.13 TIN 494.14 ZIRCONIUM AND NIOBIUM 50

5. DISTRIBUTION COEFFICIENTS FOR OTHER NUCLIDES 515.1 ANTIMONY 515.2 BORON 515.3 CADMIUM 515.4 TELLURIUM 545.5 ZINC 54

5. CONCLUSIONS 56

REFERENCES 58

1. INTRODUCTION

Canada has selected geological containment in a vault deep in

plutonic rock in the Precambrian Shield as the most promising method for

disposal of its nuclear fuel waste (Boulton, 1978). A stable granitic

pluton will most likely be the host rock.

Assessment of the integrity of geological containment requires

pathways analysis to determine the travel time from the vault to the

biosphere of all the nuclides associated with the waste (Mehta, 1982). The

travel time and the predicted nuclide concentrations in the biosphere will

depend upon the interaction of the nuclides with their surroundings as they

migrate from the vault. Traditionally, this interaction has been described

using a distribution coefficient, K,, for rock, unconsolidated regolith and

soil (Wuschke et al., 1981). The objective of this report is to document

these K, values, separating them according to the major soil types found on

the Precambrian Shield. These parameter values are required for the soil

model in the assessment code used in the Canadian Nuclear Fuel Waste

Management Program.

Further, since the assessment code is stochastic, the

distributions of the K, values are also needed. Preliminary work with the

K values indicates that they are lognormally, as opposed to normally,ddistributed. The lognorraal distribution parameters (log^o) are reported

here. These parameters directly represent the data presented where two or

more values were found, and have not been adjusted toward conservatism for

assessment purposes. Sections A, 5 and 6 list the soil K, values, and their

appropriate distributions, for the actinides, the radionuclides produced

from nuclear fission and the stable nuclides, respectively, that are

expected to be present in 100-year cooled nuclear fuel (Mehta, 1982). A

reference list Is included for each nuclide.

- 2 -

2. DISTRIBUTION COEFFICIENT, K3

The processes of solute migration pertinent to radionuclide

migration in soil and unconsolidated geological materials have been discus-

sed and reviewed extensively (Wheeler, 1976; Onishi et al., 1981; Miller,

1983; Gillhara and Cherry, 1979; and Arnold et al., 1982). Many computer

models have been developed to predict nuclide migration through soil (Murali

and Aylmore, 1981; Yeh and Ward, 1981; Oster, 1982; Miller, 1983; Wong et

al., 1983; van Genuchten, 1978; Duguid and Reeves, 1976; and Sheppard,

1981). These models vary in their complexity and purpose. The simplest

model of the solute transport process, expressed in one-dimensional form,

is

where C is the solute concentration in solution, i.e., mass of solute

per unit volume of soil (g.cm~3),

t is time (s),

D is the dispersion coefficient (cm2.s-i),

x is the space coordinate (cm), and

V is the average linear pore-water velocity (cm.s-i).

Since Equation (1) does not account for the interaction of the solute and

the solid phase, the distribution coefficent, K , has been introduced tod

describe this interaction. The distribution coefficient is defined as the

concentration of solute in the adsorbed phase (mass of solute per unit mass

of soil) divided by the concentration of solute in the solution phase (mass

of solute per unit volume of soil pore water). The units of K are usually

mL/g. The K, value for each nuclide represents the partitioning of the

solute between the solid and solution phases and is applicable to equilib-

rium reactions, such as ion exchange.

Typical radionuclide interactions with soil include other geochem-

ical processes, such as precipitation, coprecipitation, hydrous metal oxide

- 3 -

coraplexation, organic matter complexation, colloid formation, and microbial

effects. Empirically determined K values may or may not include these pro-

cesses.

Ion exchange is one of the most common mechanisms of radionuclide

adsorption on geological materials (Ames and Rai, 1978). Thus, the K, value

depends upon several factors, including the cation exchange capacity (CEC),

and the species and concentration of both the ion being exchanged and the

competing ions. If the nuclide is present in smaller concentrations than

the competing Ions, then the K, value will be. independent of the concentra-

tion of the nuclide, and it will be constant if all other factors remain

constant (Johnston and Gillham, 1980).

To incorporate the K, concept into the solute transport process

described by Equation (1), the dispersion coefficient (D) and the pore-water

velocity coefficient (V) become the effective dispersion coefficient (D1)

and velocity coefficient ( V ) , respectively, where

• > • • !

'•4(2)

and R is the retardation factor, defined as

R = l + ^ K d (3)

where p, is the bulk density of the soil (g/cm3)

n is the porosity (cm3/cin3), and

K is the distribution coefficient (mL/g).

The K, concept is restricted to equilibrium reactions in which the concen-

trations in the solution and solid phases are related. K, was initially

defined by Mayer and Tompkins (1947) as

(4)

- 4 -

where C is the tracer concentration in the solution before adding the

sorbent,

C is the tracer concentration in the liquid phase of a sorbent-

water suspension,

V is the volume of liquid, and

M is the mass of solid.

Despite the fact that the K, concept strictly applies only to

simple cation-exchange, K, values are reported that describe more complex

reactions. This is in response to the need for input to simple migration

models. This report does not review the soil chemistry of the nuclides

considered; this has been done adequately elsewhere (Jenson, 1980; Johnston

and Gillham, 1980; Allard et al., 1977; Friedman, 1976, Swedish Nuclear Fuel

Supply Co. Ltd., 1983; Ames and Rai, 1978). The report does list all of the

K, values by predominant soil type for the Precambrian Shield (sand, silt,

clay and organic (Beals, 1984)) and includes other pertinent information

found in the literature. Table 1 lists K. distribution parameter estimates

for some nuclides combining all soils, as reported by Baes and Sharp (1981).

Nuclide

AmCeCsNpPbPoPuSrTcThU

* From Baes* * M o a n f\f t-1

ESTIMATES OF

p.**

2.93.03.01.02.02.73.31.4

-1.54.81.6

and Sharp (1981)

TABLE 1

DISTRIBUTIONS OF K,,*

1.30.60.81.00.70.31.00.90.50.60.6

exp( \i)+

(mL/g)

8101100110011995401800270.0360 00045

VALUES

K. Range(mL/g)

1.0 to 47 00058 to 600010 to 52 0000.16 to 9294.5 to 7600200 to 110011 to 300 0000.37 to 4000.003 to 0.282000 to 510 00011 to 4400

*** Standard deviation of the logarithm (to base 10) of K+ Median value of Kj with a 0.5 cumulative probability

- 5 -

3. DISTRIBUTION COEFFICIENTS FOR THE ACTINIDES

3.1 ACTINIUM

Nothing was found in the literature on K, values or the soil chem-

istry of actinium. We recommend using the K, values for americium because

of their chemical similarity.

3.2 AMERICIUM

Americium has been studied extensively because of weapons testing

in the 1950s. The summary on americium geochemistry presented by Johnston

and Gillham (1980) indicates that

(1) the most stable form of americium in aqueous solutions is Am 31";

(2) the soil sorption of americium is correlated to cation exchange

capacity, clay content, and concentration and type of the compe-

ting ions in solution, indicating that the principal retardation

mechanism is ion exchange;

(3) at high K, values, americium adsorption is sensitive to the con-

centration of americium in solution.

Table 2 lists the K, values reported by various investigators and includes

soil information (texture, pH, competing ions, etc.) pertinent to the sorp-

tion data. The recommended K, value means, standard deviations, ranges and

distribution parameters by soil type for americiura, based on Table 2, are

given in Table 3.

SoU 7. 7.T/ne &««) Silt

Sand fine sandyfine Randyfine sandyfine sandy

7.

d a y

loanloanloanloan

lL#it loanlLght loan

coarse sand

76.C 21.291.2 7.891.6 5.494.6 1.665.2 29.083.6 12.642.6 39.460.4 19.483.4 8.849.2 20.444.0 20.064.0 14.044.0 24.066.0 11.0?38-0 32.074.0 12.074.0 12.078.0 2.04S.0 34.0?82.0 9.0

Silt allty claysilty clay

loanI o n

16.0 50.09.0 54.0

H.0 53.0day

clay

5.0 31.032 X> 32.032.0 32.010.0 34.0

2.8

1.03.0

3,85.83 .8

18.020.2

7.822.436.022.032.023.030.014.014.020.018.09.0

loailcm

34.037.016J)

64.036.036.056.0

abyssal red clay

atyssal red clay

Organic organicorganic

XOrganic

2.4

2.45.75.78.48.4

-

0.431.190.990.210.450.170.600.180.160.982.4

3.40.20.30.1

0 . 30 .10 .70.7

0 . 6

2.82.82.52.50 . 8

2.33.60 .60.6

-

0.71.02.73.2-

-

40.840.8

7.

---

---

----

------

0.4

0.37.95.20.00.60.00.20.20.7

1.720.60.7

2.4

0 .0

0.00.9-

-

pH»Saturated Paste

5.3 (4.39)5.3 (5.71)5.0 (4.58)5.0 (6.17)6.0 (5.71)6.0 (6.72)

7-8

8.1

4 . 0

6.75.28.18.48.68.48.4

7.75.75.68.38 .0

7.5o.O8.25.46.4

4.85.9 (5-41)5.9 (6.56)6.7 (6.12)6.7 (6.98)

7.82.33.6

7.8 (7.12)7.8 (8.04)

7-3

7.94.85.46.22.7

6.9

7.2 (7.14)7.2 (7.54)

(V)

-------

----------

0.410.520.430.470.450.430.440.540.490.57----

0.440.570.56

-

0.420.490.450.57-

-

--

VALUES

CEC(nsqAOO

1515151515

15-

5.942.011.790.696.144.95

15.0410.446.38

18.3620.917.513.88.2

17.56.4

5.82.97.0

3.820202525

15.516.217.4

X30-

29.620.516.034.4

-

-

6060

FOR AMER1CILM :

I Freeg) Iron Oxides

1.651.651.521.525.295.29-

--------------------

1.291.292.412.41---

1.201.20-

-----

-

1.571.57

LXISAIURE SURVEY SLMWff

CompetingCation

-

-----

tb (90S s.-it.solution.)

---------------

---

--

-

Na (90* sat.solution)

----

0.68 mlA.NaQ

0.68 mol/LN a d

-

-

Kd(mL/g)

9.635xlO3

8.063xlO3

1.549xlO3

l,82xlO2

2.187x10"1.066x10"4xlO2

7.14xlO2

4.76xlO2

4.17xlO2

2.49xlO2

1.25xlO2

8.33xlO2

3.92xlO3

4.35x10"3.7x10"1.09x10"2.5xlO3 ± 210+6.CK1O2 ± 24+3.0xl02 • 10+8.2xlO2 ± 43+1.0x!0" ± l.SxlO1*1.2xlO2 ± 7+2.3xlO2 1 5+8.2x10' ± 1+**4.0xl02 t 11+3.9xlO2 • 2O*2.98x10"1.728x10"2.387x10"2.021x10"5.9xlO3 • 230*l.SxlO3*"1.6xlO3 • 190+3.563x10"4.723x10"5x10"

5.2xlO3 1 97C*2.6xlO3 1 47O1"9.2xlO2 • 79+2.9xlO3 t 1800+25.1

4.0xl05

7.266xlO3

5.529xlO3

Soil Locationor Inscription

rtilMs (Louisiana)btelbis (Louisiana)Lyaan (Milne)Lyman (Milne)Alken (California)Alken (California)(Netherlands)

(Rlchland, Washington)Fuquay (Bamuell, SC) O-5 enfcquay (Barmtll, SC) 5-15 oFuquay (Bamuell, SC) 15-50 cmftnf ord AHanf ord BIdaho AIdaho BIdaho CIdaho DColorado A (Bodty Flats)Colorado B (Sugar Loaf)Idaho BIdahoCIdaho Dttuhlngton A (Hanf ord)Uishlngton B (Itanford)S. Carolina (Bamuell)New Ifexico (Los ALaK*)Arkansas BSharpaburg (loua)Shafpsburg ( low)Yolo (California)Yolo (California)Idaho AArkansas CIllinoisHoltsvilleIbltsvllle(tetherLands)

Colorado C (Rocky Flats)Tennessee (Ok Ridge)New York (Vfest Valley)Arkansas A—

EgbertEgbert

Reference

NLshlta e t a l . 1979Nlshlta et a l . 1979Nishlta e t a l . 1979Nlshlta et a l . 1979Nlshlu e t a l . 1979Nlshlta et a l . 1979Hamcra 4 Verkerk, 1977

Azs I Rai, 1978Ana & Rai, 1978tees 4 ft.1, 1978a m & Rai, 1978A K S & Rai, 1978ABES 6 Rai, 1978

fees & Rai, 1978tees & Rai, 1978tuna 4 Rai, 1978tees & Rai, 1978Glover et a l . , 1976Glover et a l . . 1976Glover e t a l . , 1976Glover e t a l . , 1976Clover et a l . , 1976Glover et a l . , 1976Glover et a l . , 1976Glover et a l . , 1976Glover et a l . , 1976Glover et a l . , 1976Nlahitaet a l . , 1979Nlshlta et a l . , 1979.Vlshiu et a l . , 1979Nlshlta et a l . , 1979Glover et a l . , 1976Glover et a l . , 1976Glover et a l . , 1976NLshita et a l . , 1979KLshlta et a l . , 1979H n t r a I Verkerk, 1977

Glover et a l . , 1976Glover et al>, 1976Glover et a l . , 1976Glover e t a l . , 1976Erlckson, I960

Erlckson. 1980

NLshita et a l . , 1979NL.<hlta et a l . , 1979

* e n the value la bracketed, i t i s the ffl of the extract.S. Carolina subsoil K values for anerlclun w.r.t- calclvm and sodlun as competing ions over two orders of negnituJe are reported In Routson et a l .Kd value determined with init ial aDeridun concentration of 10"10 tnol/L.Sanrf, s i l t and clay percentages exceed 100X In original report.

1975.

- 7 -

TABLE 3

K, FOR AMERICIUM—a

SoilType

S.D."1

(mL7g)K, Range(mL/g)

LognormalDistribution*

Sand 6.146xlO3 1.1159x10** 27 82 to 4.35x10** 3.105 0.8172

Silt 1.4351x10** 1.1282x10** 7 1.6x103 to 2.98x10** 3.946 0.5382

Clay 6.0501x10** 1.29xl05 9 25.1 to 4.0xl0b 3.832 1.23

Organic 6.398x103 1.228x103 2 5.529x103 to 7.266x103 3.802 0.0839

* K = mean of K, valuesd d

"*" S.D. = standard deviation of K., valuesd

* Base 10 logarithms here and in all subsequent tables

Baes and Sharp (1981) suggested a mean value of 2.9 for the

logjgKj f° r ainericium, combining all soil types, and a corresponding stan-

dard deviation of 1.3 (see Table 1). Allard et al. (1977) reported K,d

values for clay/mud of 2 x 10 2 to 1.6 x 10 4 mL/g and for granite of

5.0 x 10 3 to 1.6 x 10 *• mL/g. Vandergraaf (198?) recommended a range of

1 x 103 to 2 x 10** mL/g for granite- The values for granite should be simi-

lar to those for coarse-textured soil (sand).

Americium References

Allard, B., H. Kipatsi and J. Rydberg. 1977. Sorption of long-lived radio-nuclides in clay and bedrock. Part 1. Determination of distributioncoefficients. ICBS Technical Report 55.

Ames, L.L. and D. Rai. 1978. Radionuclide interactions with soil and rock,media, Volume 1. U.S. Environmental Protection Agency Report, EPA520/6-78-007.

Baes III, C.F. and R.F. Sharp. 1981. Predicting radionuclide leachingfrom root zone soil for assessment applications. Trans. Am. Nucl. Soc.38, 111-112.

Erickson, K.L. 1980. Radionuclide sorption studies on abyssal red clays.In: Scientific Basis of Nuclear Waste Management Vol. 2. Plenum Press,ed. C.J.M. Northrup.

- 8 -

Glover, P.A., F.J. Miner and W.L. Polzer. 1976. Plutonium and americiumbehaviour in the soil/water environment. I. Sorption of plutonium andamericium by soils. In: Proceedings of the Actinide-Sediment Reac-tions Working Meeting at Seattle, Washington on 1976 Feb. 10-11. Bat-telle Pacific Northwest Laboratories Report, BNWL-2117, pp. 225-254.

Harastra, J. and B. Verkerk. 1977. Review of Netherlands program for geo-logic disposal of radioactive waste. Ini Nuclear Power and its FuelCycle. International Atomic Energy Agency Report, IAEA-CN-36/289.

Johnston, H.M. and R.W. Gillham. 1980. A review of selected radionuclidedistribution coefficients of geologic materials. Atomic Energy ofCanada Limited Technical Record, TR-90*.

Nishita, H., A. Wallace, E.M. Romney and R.K. Schulz. 1979. Effect of soiltype on the extractability of 237Np, 239Pu, 241Am and 244Cm as a func-tion of pH. NUREG/CR-0997 UCLA 12-1192. 32 pp.

Routson, R.C., G. Jansen and A.V. Robinson. 1975. Sorption of 99Tc, 23^Jpand 2LflAm on two subsoils from differing weathering intensity areas.Battelle Pacific Northwest Laboratories Report, BNWL-1889.

Vandergraaf, T.T. 1982. A compilation of sorption coefficients for radio-nuclides on granites and granitic rocks. Atomic Energy of Canada Lim-ited Technical Record, TR-120*.

3.3 BISMUTH

Nothing was found in the literature on soil K, values for

bismuth, but bismuth should behave similarly to polonium because of their

proximity in the Periodic Table.

3.4 LEAD

Lead is a heavy-metal cation of general environmental concern in

most industrial areas. Consequently, considprgi-.le information exists about

its environmental behaviour (Gerritse et al., 1982; Wolf et al., 1977; Sol-

datini et al., 1976; Abd-Elfattah and Wada, 1981). Unfortunately, not much

K, information is available (see Table 4).

The recommended K, value means, standard deviations, ranges and

distribution parameters for lead by soil type, based on Table 4, are given

in Table 5-

Unrestricted, unpublished report, available from SDDO, Atomic Energy ofCanada Limited Research Company, Chalk River, Ontario KOJ 1J0.

K, VALUES FOR LEAD : LnBJAlUBE SUKVBf SIMWg

Sill X I X *Type Sand Stlt day Organic , Saturated Paslte (V)

CKC % Free(mcqAOO g) I ron ( M d e s

OpnpetingQatlon

Soil locationor Description

OrRanlc

0

0

20

inpol lutedorganic soil

unpolluted peat

unpolluted peat

polluted peatsphagnm pea:sphagnim peat

3.5

3.5

2.5

90

>90

>90

>90--

4.5-5.0

4.5-5.0

7.5-8.0

4.5

4-5

4-5

6.24-54-5

22

22

16

-

-

-

_

--

[ C a * J -O-0.015 HDI/L

[Ca21-)-0-0.015 nol/L

[&«•!-

0-0.015 m>L/L-

[ C a » ] -0-0.015 nol/L

[ & « • ] .O-0.015 molA.

--

2.8ilO2

1.3xlO3

3.5riO3

2.52x10^

1.8xl02

6.3X1O1*

2.34X101*61IO"

Soil C

SoU C

Soil D

SoU A

Feat A

Peat A

Soil 8

Iteference

Gerrttse et a i . , 1982

Gerrltse et a l . , 1982


GerrltM et a l . , 1982

Gerrttoe et a l . , 1982

Gerrltse »t a l . , 1982

Gerrltse et a l . , 1982Vfolf e t a l . , 1977tolf e t a l . , 1977

I

I

- 10 -

TABLE 5

SoilType

Sand

Organic

(mL^g)

1693

2.7845x10 **

S.D.

1646

2.6024x104

n

3

4

KJ Range(mL/g)

280 to 3500

180 to 6.3x10h3

3

LognorraalDistribution

.035 0.5527

.954 1.150


log^0K, for lead, with a corresponding standard deviation of 0.7 (see Table

I). Lead should behave similarly to polonium and K values for polonium can

be found in Section 3.6.

Lead References

Abd-Elfattah, A. and K. Wada. 1981. Adsorption of lead, copper, zinc,cobalt and cadmium by soils that differ in cation-exchange materials.J. Soil Sci. 32_, 271-283.

Baes III, CF. and R.D. Sharp. 1981. Predicting radionuclide leaching fromroot zone soil for assessment applications. Oak. Ridge National Labora-tory Report, CONF-810606-44.

Gerritse, R.G., R. Vriesema, J.W. Dalenberg and H.P. De Roos. 1982. Effectof sewage sludge on trace element mobility in soils. J. Environ. Qual.1^, 359-364.

Soldatini, G.F., R. Riccardo and R. Levi-Minzi. 1976. Lead adsorption bysoils. I. Adsorption as measured by the Langmuir and Freundlich iso-therms. Water, Air Soil Pollut. 6 111-118.

Wolf, A., K. Bunzl, F. Dietl and W.F. Schmidt. 1977. Effect of calciumions on the absorption of lead (2+), copper (2-.), cadmium (2+), andzinc (2+) by humic substances. Chemosphere 6, 207-213.

3.5 NEPTUNIUM

The summary on neptunium geochemistry presented by Johnston and

Gillham (1980) indicates that

- 11 -

(1) neptunium should exist as Np in the form of NpO 2+ in an oxidi-

zing soil environment; however, it is not evident whether NpO J" is

also the dominant species under reducing conditions;

(2) neptunium colloids have been reported in some soil-solution exper-

iments (Sheppard et al., 1976) and absent in others (Routson et

al., 1977).

The recommended K value means, standard deviations, ranges and

distribution parameters for neptunium by soil type, based on Table 6, are

given in Table 7.

TABLE 7

FOR NEPTUNIUM

SoilType

S.D.d(mL/g)

^ Range

(mL/g)Lognormal

Distribution

Sand

Silt

Clay

Organic

37

471327

857

.6

.41

.

.5

9435

1529

101

.57

.88

.

.1

1764

2

0.16

1.27

41786

to

to

to

to

390

953200

929

0.6782

1.426

2.619

2.932

0.9728

0.6925

0.9222

0.0513


logi0K, for neptunium, with a corresponding standard deviation of 1.0 (see

Table 1). Allard et al. (1977) reported K ranges of 10 to 16 mL/g for

clay/mud and 25 to 50 mL/g for granites. Vandergraaf (1982) recommended a

K of 40 to 100 mL/g for granites,d

Neptunium References

Allard, B., H. Kipatsi and J. Rydberg. 1977. Sorption of long-lived radio-nuclides in clay and rock. Part 1. Determinations of DistributionCofficients. KBS Technical Report 55.

SoU X X XType Sand Sil t CLay

Sand fine sandy loamfine sandy loanfine sandy loanfine sandy loan

l l# i t loanlight loam

sandsandsandsand

sandy claysandy claysandy claysandy clay

76.0 21.2 2.894.6 1.6 3.8

sandSl i t s l l t y clay loan

s l l ty clay loanloanloan

12.6 65.8 21.632-0 56.0 12.0

Clay clayc Layclayclay


7.Organic

2.42.45.75.78.48.4--------

0.430.210.392.82.82.52.53.610.840.60.60.860.29

40.840.8

X pH*CaXlj Saturated Paste

5.3 (4.08)5.3 (5.57)5.0 (4.42)5.0 (6.06)6.0 (5.56)6.0 (b.57)2 . 5 - 3.12 . 5 - 3.12 . 5 - 3.12.5 - 3.12 . 5 - 3.12 . 5 - 3.12.5 - 3.12 . 5 - 3.1

8.15.28.1

5.9 (5.83)5.9 (6.85)6.7 (6.13)6.7 (6.83)

5.36.5

7.8 (7.29)7.8 (8.28)

8.18.1

7.2 (6.24)7.2 C7.25)

Kj VALUES FOR NEPIUNIUM :

E^ CEC(V) (meq/100 g)

151515151515

--

------

5.940.69

0 sat.20202525

16.8810.76

3030

0 sat.0 sat .

6060

X FreeIron Oxides

1.651.651.521.525.295.29-----------

1.291.292.412.41--

1.201.20

-1.571.57 >

LTIERA1UKE SURVEY

CompetingCation

-

-----

0.002 m l / L Ca

0.2 O D I / L Ca

0.015 m l / L Na3 .0 mol/L Na0.002 mol/L Ca0 .2 mol/L Ca0.015 n c l / L Na3 .0 no l /L Na

---------------

sumuo

W g )

3183322610B2.370.363.93.20.250.160.70.415.432.4390 t 16359552811.2720.2411171950 ± 3103200 ±890786929

Soil Locationor Description

Milbis (Louisiana)Malbls (Louisiana)Lytmn (mine)Lyrnan (Msine)Aiken (California)Alken (California)Burtenk (Vhshlngton)Burbank (Washington)Burbank (Vhshlngton)Burbank (Vhshlngton)Scuth CarolinaSouth CarolinaSouth CarolinaSouth CaroLtnaBurtank (Rlchland, Vtahington)Fuquay (5-50 cm)K.E. Irish Sea SedinentSharpsburg (loua)Siarpsburg (lots)Yolo (California)Yolo (California)MiscatineRltzvrUleHoltsvllleIbltsvllleW Mediterranean sea sedimentNE Atlantic sea sedimentEgbertEgbert

Reference

Nlahlta et a l . ,Nlshlta et a l . ,Nlshlta et a l . ,Nlshlu et a l . .NLshlca et a l . .Nlshlta ec a l . ,Routson et a l . .Routson et a l . ,Routson et a l . ,Routson ec a l . ,Routson et a l . .Rcutson et a l . ,Rcutson ec a l . ,Routaon et a l . ,

19791979197919791979197919771977197719771977197719771977

tues I Ra?, 1976Ames & Rat, 1978Fowler & Aston,Nlshlu ec a l . ,Nlshlta et a l . ,Nlshlta et a l . ,NLshlta ec a l . ,

19821979197919791979

toes & Rat, 1978tos i Rat, 1978Nlshlu et a l . ,Nlshlta et a l . .Fowler 4 Aston,Fowler & Aston,Nlshlu et a l . ,NLshlU et a l . ,

197919791962198219791979

to

I

value Is bracketed It Is extract nH.

- 13 -

Ames, L.L. and D. Rai. 1978. Radionuclide Interactions with soil and rockmedia, Volume 1. U.S. Environmental Portection Agency Report, EPA52O/6-78-OO7 .

Baes III, C.F. and R.D. Sharp. 1981. Predicting radionuclide leaching fromroot zone soil for assessment applications. Oak Ridge National Labora-tory Report, CONF-810606-44.

Fowler, S-W. and S.R. Aston. 1982. Application of 23iftp in experimentalaquatic radioecology: Preliminary observations on neptunium behaviorin sea water, sediments and zooplankton. Health Phys. 4_2_, 515- 520.


Nishita, H., A. Wallace, E.M. Romney and R.K. Schulz. 1979. Effect of soiltype on the extractability of 23^Jp, 2 3%u, 241Am and 21<Ltm as a func-tion of pH. NUREG/CR-0997 UCLA 12-1192. 32 pp.

Routson, R.C., G. Jansen and A.V. Robinson. 1977. 241Ara, 23^Ip and 99Tcsorption on two United States subsoils from differing weathering inten-sity areas. Health Phys. 33_, 311-317.

Sheppard, J.D., J.A. Kittrick and T.L. Hart. 1976. Determination of dis-tribution ratios and diffusion coefficients of neptunium, americium andcurium in soil-aquatic environments. Richland Operations Office Con-tract Report, RL0-2221-T-12-2.


3.6 POLONIUM

Polonium information in the literature is extremely scarce.

Bismuth should behave similarly to polonium, and also lead and polonium

should behave similarly. All of the K, information on polonium reported

here (see Table 8) comes from one research program (Hansen, 1970; Hansen and

Watters, 1971). The chemical form of natural polonium in soils, resulting

from the decay of radium, may be similar to that of selenium (Hansen, 1970).

Tellurium is also a member of Group VIA of the Periodic Table and may behave

similarly to polonium. Polonium compounds with +2 and +4 oxidation states

have been reported, with the preferred oxidation state being +4 (Hansen,

1970). Polonium in air is generally found as polonium dioxide (PoO j)

* Unrestricted unpublished report, available from SDDO, Atomic Energy ofCanada Limited Research Company, Chalk River, Ontario KOJ 1J0.

TABLES

K, VALUES FTH FOLOKIW : UTHfflURE SURVEY SHUBX

Sail T. X Z Z Z fHTyj*s Sirei S t i c Q a y Organic CaCO3 Sa turated P a s t e

E CEC 1 Fcee Carpetingg ) I r o n CWdes Cfctian (mlig)

Soil Locationor Description Reference

42.0 3J.0 26.0 6.1 22.8

455459627295849597

%57

74

80

74

49

57

47

42222015180621

230

17

16

22

39

30

29

13242123105

1032

213

8

4

4

12

13

24

6.56.75.55.77.85.95.45.55.5

5.65.5

5.7

6.0

6.0

6.6

5.5

6.8

5.4----

3.02.61.81.5

4.6-

-

-

-

16.8

-

_ _

120

203

310

766

± 5*

±22

±41

I K S

1213 ± 186

643

723

192206508814275263525171555771713

30

66

75

254

371

137

±85

±83

±26± 11±34±42± 9

± 2± 3± 2± 1±0.6±17± 29± 1± 2

± 7

± 9

± 8

±22

±36

± 5

Him si l ty clay loam(All) (Colorado)

H n sl lty clay loam(A12) (Colorado)

rtftn s l l ty clay I o n(B,) (Colorado)

[ism sl l ty clay loam(S2t) (Colorado)

Hsm sl lty clay loan(BjCa) (Colorado)

Mxm allty clay loan(CCa) (Colorado)

DinflttOc alley city loss(C) (IOUB)

Lapeer loaa (Ap) (viaconsln)Lapeer loan (B2|) (Wisconsin)Lapeer loan (B29) (Ulaconsln)Lapeer loam (B3) (Utscoreln)lapser loan (C,) (Wisconsin)Adansville (A^ (Florida)BUnton (Ap (Florida)Lakeland (A[) (Horlda)Leon (Aj) (Florldz)Leon (A2> (Florida)Leon (Bn) (norlda)Leon (C) (Florida)RjsUn (A,) (Fkirliia)Darling gravelly sandy loan(B2) (Colorado)

Darling gravelly sandy l w(B,, r ) (Colorado)

Itorling gravelly sandy loan(C[) (Colorado)

Darling gravelly sandy loan(C2) (Colorado)

Gogebic sandy loam (ty(MLsconsiji)

Gogebic sandy loan (Bir)( « scons in)

Gogebic aandy loai (Birh)(Wlsccraln)

ftnsen & Vbtters, 1971

ttansen i Vbtters, 1971

Ifensen & Vfetcers, 1971

Hmsen t Wtcers, 1971

tensen t Vbtters, 1971

Fhnsen & Vbtters, 1971

Ihnsen I Vfctters, 1971

{fansen & Witters, 1971Hrasen 4 * t t « - » , 1971tenser & Vbcters, 1971Ifamen & o t t e r s , 1971Ansen 4 Vbtters, 1971•Ansen i Vhtters, 1971ibnsen & Vbtters, 1971Hansen & Witters, 1971tfensen & Witters, 1971Hansen i Vbtters, 1971Ifensen f. Vbtters, 1971Hansan i Vbrters, 1971Hmsen & Vbtters, 1971Hamen I Vbttzrs, 1971

Ifanscn t vktten, 1971

Hmaen I Vbtten, 1971

Hmsen 4 Vbttera, 1971

Vhnsen I Vbtters, 1971

Hmsen 4 Vbtters, 1971

Iknssi i Vhtters, 1971

(contlimKl...)

TABLE 8 (Condir ied)

S o i l X X X X XType Snrxl Silt day Organic CaO03 Saturated P&slte (V)

CEC X Free Carpeting K,(raeqAOO g) Iron Ojddes Cation (ni./g)

Soil Location

or Description

68

46

46

67

67

82916311

17

3

10

U

10

8

5

2

5

5

33

27

27

44

43

20

20

50

2768

55

73

61

65

80

71

66

66

65

66

52

55

5

10

11

13

13

139

1021

28

24

29

24

10

21

29

32

30

29

15

18

3.8

5.9

6.8

6.9

8.2

8.4

6.35.05.65.8

5.6

5.5

5.9

7.8

5.9

6.2

6.1

5.6

5.3

5.5

5.1

5.5

5.1

-

-

-

2.71.93.4

25.2

-

2o.4

-

-

11.2

-

-

-

-

-

28.9

16.4

242 ± 25

227 ± 20

412 ± 150

2248 ± 1200

7020 ± 3600

76 ± 11188 ± 1549 t 31030 ± 49

976 ± 127

1136 ± 118

968 ±32

1830 ± 210

970 ± 160

122+3

92 ± 3

597 ± 55

80 ± 2

772 ±29

24 ± 1

405 ±28

Gogebic sandy loan (B3)(Wisconsin)

Onaway fine sandy loan (Ap)(Wisconsin)

Onaway fine sandy loan (BLrh)(Wisconsin)

Onauay fine sandy loam (Cj)(Wisconsin)

Onauay fine sandy loan (Cj)(Wisconsin)

Anite (A;) AlabaoBIndependence (AL) (Alabana)Wlckhan (A,) (Alabama)Dinsdale s l l ty clay loam(A) (lew)

Dinsdale s l l ty clay loan(B) (loua)

Miscatine s l l ty clay loan(A) (low)

Hiscatlne s l l ty clay loan(B) (loua)

Miscatine s i l ty clay loao(C) (Ioua)

Fayette s i l t loan (Ap)(Wisconsin)

Fayette l i l t loan (Bj)(Wisconsin)

Fayette s i l t loan (BJJ)(Wisconsin)

Fayette s i l t loan (B22)(Wisconsin)

Fayette s i l t loan (B23)(Wisconsin)

Fayette s i l t loan (C,)(Wisconsin)

Darling gravelly sandy loam(Aj) (Cblorado)

Cbngaree (A.) (Alabana)

Hansen & Witters, 1971

Hansen & Vbtters, 1971

Hmsen & Ifetters, 1971

ftmsen «. Wattera, 1971

Hmsen 5 l i t t e r s . 1971

Hmsen i Hatters, 1971Hansen i Witters, 1971Hmsen & Hitters, 1971Hansen & Matters, 1971

Hansen & Hatters, 1971

Hareen I Hitters, 1971

Hansen 6 Hitters, 1971

Hansen & Hitters, 1971

Uansen £ Hitters, 1971


Hansen 6. Hatters, 1971

Hmsen I Hatters, 1971

Hansen i Matters, 1971

Hansen i Hitters, 1971


thnsen & Hitters, 1971

All error terns in this table are standard error of the mean (S.E.)

- 16 -

(Hansen, 1970). Hansen also reported that, for pH values of 1 to 5, 7 to 8

and 12 to 14, polonium exists mainly in dissolved forms, while for pH values

of 6 to 7 and 10 to 11, most of the polonium exists as a colloid. Thus, in

the acidic organic and acidic sandy soils of the Precambrian Shield,

polonium may exist only in the dissolved form*

The recommended K., value means, standard deviations, ranges and

distribution parameters for polonium by soil type, based on Table 8, are

given in Table 9.

TABLE 9

SoilType

Sand

Silt

(mL/g)

504.2

692.5

S.D.

1215

535.7

FOR POLONIUM

n

35

13

K. Range(mL/g)

13 to 7020

24 to 1830

2

2

LognormalDistribution\i a

.188 0.6574

.607 0.5789


log10K for polonium, with a corresponding standard deviation of 0.3 (see

Table 1). The value for [i is higher, but the range of K., values is

narrower, than recommended for lead.

Polonium References


Hansen, W.R. 1970. Polonium-210 in soils and plants. Special Report onU.S. Atomic Energy Commission Contract No. AT(11-1)-1733, COO-1733-11.

Hansen, W.R. and R.L. Watters. 1971. Unsupported 210PoO2 in soil: Soiladsorption and characterization of soil solution species. Soil Sci.112, 145-155.

- 17 -

3.7 PLUTONIUM

Plutonium, like americium, has been studied extensively because of

weapons testing in the 1950s. The summary on plutonium geochemistry pre-

sented by Johnston and Gillham (1980) indicates that

(1) Pu4* is considered the most probable oxidation state in the envi-

ronment because of reduction of Pu "*• to pu^* by organic materials;

reduction of Pu4* to P u ^ could occur at pH <6 under anaerobic

conditions;

(2) plutonium adsorption is a function of oxidation state (Pu6*" is

adsorbed less than Pu 1^), organic matter content and solution pH;

(3) K, values for plutonium reported in the literature were often

obtained without knowledge of the oxidation state, and caution

must be used in interpreting results that use these K, values.

Most K, values in the literature apply to aerobic conditions. The recom-

mended K value means, standard deviations, ranges and distribution para-

meters for plutonium by soil type, based on Table 10, are given in Table 11.

TABLE 11

SoilType *4

(mL/g)

S.D.

FOR

n

PLUTONIUM

K^ Range(mL/g)

LognormalDistribution|j 0

Sand 1.041x103 1.568x103 19 33 to 6.865x103 2.663 0.5964

Si l t 1.3871x104 3.0836x104 8 230 to 9.0x104 3.474 0.7906

Clay 4.2842x104 6.8934x104 13 316 to 1.9x10b 3.706 1.047Organic 2.2902xl04 2.8181xl04 4 1.655xlO3 to 6.2X101* 3.970 0.7469


log10K, for plutonium, with a corresponding standard deviation of 1.0 (see

Type Sind 5Ut Clay

Sand fine sanily loanfine sandy Iranfine sandy loaafine sandy loan

light l alight loan

coarse sand

44.0 20.0 36.064.0 14.0 22.044.0 24.0 32.066.0 11.0? 23.038.0 32.0 30.074.0 12.0 t .074.0 12.0 14.078.0 2.0 20.048.0 34.0? 18.082.0 9.0 9.0

subsoil sandsubsoil sand

Silt sl l ty clay loansl l ty clay loan

loam

loan16.0 50.0 34.09.0 54.9 37.0

31.0 53.0 16.0s i l t suspended In se

Clay clayclayclay

5.0 31.0 64.032.0 32.0 36.032.0 32.0 36.010.0 34.0 56.0

treated day

XOrganic

: , 4

5.75.78.48.4

-

2.43.4

0.20.30.10.30.10 . 7

0.7

0 .6--

2.82.82.52.50.82.33.6

awter0.60.6

-

0.71.02 .7

3.2-

Ct-sat. soil clay fraction

Ca-sat. soil clay fraction

Ca-sat. soil clay fraction

abysaal red clay

abyssal red clay


bone charcoalcoconut charcoal

-

-

40.840.8

--

c*r>3

_------

0.40.37.95.2

0 .0

0 .60.00.2

0.20.7

2 .0

2 .0----

17.20 . 60.7

---

-

2.4

0 .0

0 . 00.9-

-

-

-

-

----

pH«Saturated Taste

5.3 (4.08)5.3 (5.57)5.0 (4.42)5.0 (6.06)6.0 (5.56)6.0 (6.57)

7-S

5.75.68.38 . )7.5

8 .0

8.25.46.4

4.88.6 (6.5)8.6 (9.3)5.9 (5.83)5.9 (6.85)6.7 (6.13)6.7 (6.83)

7.82.33.6-

7.8 (7.29)7.8 (8.28)

7-8

7.94 .85.46.24 . 0

6.5

6.5

6.5

2.7

6.9

7.2 (6.24)7.2 (7.25)

7.07.0

K

F

fV)

-------

0.410.520.430.470.450.430.440.540.490.57------

0.440.570.56----

0.420.490.450.57

-

-

-

_

-

-

---

-

VALUES TOR

(T.Cn»q,100 g)

15151515

1515

-

20.017.513.8

8.217.5

6.45.82.97.0

3.85.05.0

2020

2525

15.516.217.4

-3030-

29.620.516.034.4

-

-

-

_

-

60

60-

-

TABLE 10

FLL1OK1LW :

Z Free

Iron Oxides

1.651.651.521.525.29

5.29-

_

-----------

1.291.292.412.41

--

--

1.201.20-

-----

-

-

_

-

1.571.57--

LTERAIWE SURVEY SuMIAiQ'

CarpetingCation

-

-----

Na (907. sa t .solution)

----------------_----

Na (9Ot sa t .solution)

----

5 azaol/L Ca^"(Ca N0,)2

5 nmol/L C a *

(Ca N0q)25 nmol/L Ca^*"

(Ca N0,)2

5 umol/L Ca*(Cracetate)0.68 mnol/LNaCl0.691 NoCl

solution---

-

(mJg)

8.5xlO2

1.515x10*9 . J 8 X 1 0 '3.3x10'6.85xlO3**1.352xlO3

2xlO2

2.2xl03 ± 460+2.OxlO2 ± 24+3.2xlO2 1 26+6.9xlO2 ± 110+2.1xlO3 ± 640+l.OxlO2 ± 7+4.3xl02 i 27+2.8xlO2 ± 5+l.OxlO2 ± 5+8.0x10' t 3+Ul4xlO3

2.OxlO2

6.3O2xlO3

3.024xl03

4.938xl03

4.341xl03

1.7xlO3 t 70+4.3xlO2 ± 23+2.3X1O2 1 10+9x10"7.44xlO2

3.61X1O2

lxlO"

1.9xlO3 ± 110+2.6xl03 t 640+8.lxlO2 t 130+7.1xl02 ± 36+1.9xlO5

1.04xlOs

1.63xl05

7.5x10"

3.16xl02

2.5X1O3

2.951xlO3

1.655xl03

6.2x10"2.5x10"

Soil Locationor [description

Milbla (Louisiana)felbls (Louisiana)Lyaun (ttilne)Lyman (telne)Alken (California)Alken (California)(Netherlands)

Colorado A (Rocky flats)Colorado B (Sugar Loaf)Idaho BIdaho CIdaho DWashington A (Hanford)Vbshlngton B (Ifenford)S. Carolina (&n*«n)New *-xlco (Los Alms)Arkansas BhanfordHanfordSiarpsburg (Iowa)Sharrsburg (Ioua)Yolo (California)Yolo (California)Idaho AArkansas CIllinois

tbltsvlllett>ltsville(Netherlands)

Colorado C (Rocky Plats)Ifennessee (Oak Ridge)Neu York (West Valley)Arkansas A2MJ"u(VI)

237Pu(IV)

23sPu(W)

235pu(VI)

—

EgbertEgbert—

—

Reference

Nlshita et a l . ,Nlshita et a l . ,Nlshita et a l . .Nlshlta et a l . .NisMta et a l . .Nlshlta et a l . ,

197919791979197919791979

Hamtra & Verkerk, 197 7

Glover et a l . ,Glover et a l - ,Glover et a l . ,Glnver et a l . .Glover et a l . ,Glover et a l . ,Glover et a l . ,Glover et a l . ,Glover et a l . ,Glover et a l . ,Bcdes, 1957modes, 1957Mshlr* et al.Nlshiu et al.NisMu et al.,NLshita et a l .Glover et a l . ,Glover et a l . ,Glover et a l . ,PUlal & HithnvKlshlta et al.Wshlta et a l .

1976197619761976197619761976197619761976

1979197919791979

197619761976, 19/5

19791979

ihimtni t Verkerk, 1977

Glover et &1.,Glover et a l . ,Glover e t a l . ,Glover et a l . ,

1976197619761976

Bondietti & Reynolds,1976

Boodlettl et a l . , 1975

Bondietti et a l . , 1975

Bondietti et a l . , 1975

Eridtsor.. 1980

Erlckson, 1980

KLshiU et a l .Nlshlta et a l .Taura, 1972Tamira, 1972

, 1979, 1979

Wien the value is bracketed, It Is pH of the extract.

Nlshlta et a l . , 1978 report Plutonian KJ values w.r.t. pH for this soil.d

K, value determined with Initial plutonlun concentration of 10~s mol/L (data foa

Sind, s i l t aivi clay percentages exceeded 1002 in original report.

OO

I

10~7 and 10~6 mol/L can he found In the reference).

- 19 -

Table 1). Allard et al. (1977) reported that the plutonium K, range for

both granite and clay/mud Is 6.3 x 10 1 to 1.6 x 10 2 mL/g. Vandergraaf

(1982) recommended a K, valia

2.0 x 103 mL/g for granite.

(1982) recommended a K, value range for plutonium of 2.8 x 10 2 to

Plutonium References

Allard, B., H. Klpatsi and J. Rydberg. 1977. Sorption of long-lived radio-nuclides in clay and rock. Part 1. Determination of distributioncoefficients. KBS Technical Report 55.

Baes III, C.F. and R.D. Sharp. 1981. Predicting radionuclide leaching fromroot zone soil for assessment applications. Oak Ridge National Labora-tory Rep' ft, CONF-810606-44.

Bondietti, E.A. and S.A. Reynolds. 1976. Field and laboratory observationson plutonium oxidation states. In: Proceedings of the Actinide-Sedi-raent Reactions Working meeting at Seattle, Washington, 1976 February10-11, 1976, Battelle Pacific Northwest Laboratories Report, BNWL-2117,pp. 505-537.

Bondietti, E.A. S.A. Reynolds and M.H. Shanks. 1975. Interaction of pluto-nium with complexing substances in soils and natur.il waters. In;Transuranium Nuclides in the Environment. International Atomic EnergyAgency Report, IAEA-SM-199/51, pp. 273-287.


Glover, P.A., F.J. Miner and W.0. Polzer. 1976. Plutonium and araericiumbehaviour in the soil/water environment. I. Sorption of plutonium andamericium by soils. _Iti: Proceedings of the Actinide-Sediment Reac-tions Working Meeting at Seattle, Washington on 1976 Feb. 10-11. Bat-telle Pacific Northwest Laboratories Report, BNWL-2117, pp. 225-254.

Hamstra, J. and B. Verkerk. 1977. Review of Netherlands program for geo-logic disposal of radioactive waste, ^n: Nuclear Power and its FuelCycle. International Atomic Energy Agency Report, IAEA-CN-36/289.


Nishita, H., A. Wallace, E.M. Romney and R.K. Schulz. 1979. Effect of soiltype on the extractability of 237Np, 239Pu, 241Am and 244Cm as a func-tion of pH. NUREG/CR-0997 UCLA 12-1192. 32 pp.

- 20 -

Pillai, K.C. and E. Mathew. 1975. Plutonium in the aquatic environment -its behaviour, distribution and significance, la: Transuranium Nucli-des in the Environment. International Atomic Energy Agency Report,IAEA-SM-199/27.

Rhodes, D.W. 1957. The effect of pH on the uptake of radioactive isotopesfrom solution by a soil. Soil Sci. Amer. Proc. 1_, 389-392.

Taraura, T. 1972. Sorption phenomena significant in radioactive waste dis-posal. J n: Underground Waste Management and Environmental Implica-tions. Amer. Assoc. Pet. Geol. Mem. l&j 318-330.


3.8 PROTACTINIUM

Nothing on K, values or soil chemistry for protactinium was found

in the literature. We suggest that K values for thorium or uranium bed

used, or even some combination of the values for these elements, such as

|(Th+U).

3.9 RADIUM

The interaction of radium with geological materials and soils, and

the environmental behaviour of radium have been documented by Gillham et al.

(1981b); Nathwanl and Phillips (1979), and Sheppard (1980), respectively.

The K values for radium vary from 50 to 1000 tnL/g (Gillham et al., 1981).d

Johnston and Gillham (1980) summarized the information relevant to K asd

follows:

(1) Radium is present as Ra in the pH range 4 to 8, and does not

readily form complex species.

(2) Radium can be expected to coprecipitate with BaSO4, carbonates and

ferric hydroxides.

(3) Cation exchange is an important adsorption mechanism, since K,

values have been correlated to cation exchange capacity (CEC).

Unrestricted, unpublished report, available from SDDO, Atomic Energy ofCanada Limited Research Company, Chalk River, Ontario K0J 1J0.

- 21 -

The recommended K value means, standard deviations, ranges andd

distribution parameters for radium by soil type, based on Table 12, are

given in Table 13.

TABLE 13

FOR RADIUM

SoilType 4

(mL/g)

S.D. ^ Range(mL/g)

LognormalDistributionu a

Sand

Silt

Clay

1

3

1

.0435x104

.0x105

.5637x104

2

41

.0845x10

.3566x10

.7216x10

4

5

4

3

48

106 to 3.8x104

2.0x104 to 9.5x105

696 to 5.6x104

3.402 1.289

5.10 0.6362

3.961 0.5522

The K, values for strontium may be used as a guide because of the

chemical similarity of radium and strontium. Baes and Sharp (1981)

suggested a mean value of 1.4 for the log1QK for strontium, with a corre-

sponding standard deviation of 0.9 (see Table 1). Allard et al. (1977)

reported a K, range for radium of 40 to 79 mL/g for clay/mud and 63 to

100 mL/g for granite. Vandergraaf (1982) recommended a K range of 5 tod

5000 mL/g for granite. Since no data were found for organic soils, theradium K.value for clay, or the strontium K. value for organic soil, is

d arecommended.

Radium References

Allard, B., H. Kipatsi and J. Rydberg. 1977. Adsorption of long-livedradionuclides in clay and bedrock. Part 1. Determination of distribu-tion coefficients. KBS Technical Report 55.


Cochran, J.K. and S. Krishnaswami. 1980. Radium, thorium, uranium and21°Pb in deep-sea sediments and sediment pore waters from the northequatorial Pacific. Amer. J. Sci. 280, 849-889.

S a i l X % X 7. %Type Sire] Silt Clay Orgsnlc CaJD3 Saturai

pH E. CECted Pas t e (V) (roeqAOO g)

Z free CbopetingI ron Oxides Cation

Soil locationor Description Btference

SanJ 93.0 5.0 2.0 0.05 40.8 7.8 (Cad2)

Silt

Oay.

91.1

91.1

35.0

6.7

6.7

43.7

43.7

31.0

6.8

6.8

36.0

47.9

47.9

48.9

4S.9

34.0

I . I

1.3

29.0

45.4

45.4

7.4

7.4

35.0

3.1

3.1

0.41

16.2

16.2

1.0

1.0

0.81

5.2

5.2

33.8 8.5 (Caa2)

5.4

5.4

4.3

4.3

5.2 7.8 (Can,)

clay

clay sedliiEnt

day sedtnent

clay sedL-mt

clay sedtnEnt

clay sediitent

clay sedbicnt

7.55?

10.9

10.9

8.32

34.7

34.7

10,4

10.4

31.48

Initial Racone, beforesoil contact1.6xlCT5 mg/La24" 0.05 mlA

no Ca

Initial Racone, beforesoil contact4xlCT5 og/LCaM 0.05 HDIA

no Ca

Ca2*" 0.05 nol/L

no Ca

Initial Racone, beforesoil contact3.7xlO-5 mg/LNi+288 mg/LCa21" 75 mg/L

-

-

-

-

-

106 ±16

4x10 3

3.8X1011

1262 ± 370

l . lxlO 5

9.5xl05

l.OtlO"

1.2xl05

696 ± 185

S.fodO1*

13.3X103*

lO.SxlO3*

8.OslO3*

4.3X1O3*

14.9X103*

17.4X1O5*

Learalngton (6)nedlun sand

St. Trams

St. Ihanns

WRBf(2) d a y loam

Uendover

Vfendover

GrlJDBby

Grtasby

Alberta clay losa

d a y , nud

d a y sediment (Pacific)

clay sediment (Radf lc)

clay sedloent (Pacific)

clay sediment (Pacific)

clay sedliEnt (Pacific)

c lay sediment (Pacific)

Clllhan e t a l . , 1981b

Nathvanl 4 Ph i l l i p s ,1979

Nathwni & n j l l l p s ,1979

Clllhamet a l . , 1981b

Nath«nl 6 P h i l l i p s ,

1979fethumi & R i i l l l p e ,

1979N3thuml 5 Ph i l l i p s ,

1979fethuml 5 Phil l ips ,

1979Gt l lhmet a l . , 1981b

Allard et a l . , 1977

Cochrai & Krlshnaswmn.1980

Cbchran & KrlshnasuamlI960

Cbchran & KrLshnaswaBl1980

Cbchran & Krlshnaswnl1990

Cbchran & Krlshnasvonl1980

Cbchrsn & KrlAhnastHsl1980

1WE - Ihlteshell Mclear tewarch &£abllsta-nt, Plnaw, Mmltota

Minimni values reported and data based on desorptlon of deep sea clays.

IsJ

- 23 -

Gillham, R.W., H.D. Sharma, M.R. Reddy, E.L. Cooper and J.A. Cherry. 1981b.Barium and radium migration in unconsolidated Canadian geological mate-rials. Atomic Energy Control Board Report, INFO-0048.

Johnston, H.M. and R.W. Gillham. 1980. A review of selected radionuclidedistribution coefficients of geologic materials. Atomic Energy ofCanada Limited Technical Record, TR--90*.

Nathwani, J.S. and C.R. Phillips. 1979. Adsorption of 226Ra by soils inthe presence of calcium (2+) ions. Specific adsorption (II). Chem-osphere 8 293-299.

Sheppard, M.I. 1980. The environmental behaviour of radium. Atomic Energyof Canada Limited Report, AECL-6796.


3.10 THORIUM

Little information is available in the literature on thorium in-

teractions in the environment; however, two brief reviews of thorium chemis-

try are available (Rancon, 1973; Sheppard, 1980). Johnston and Gillham

(1980) summarized the information relevant to K as follows:

(1) The primary thorium adsorption mechanism is ion exchange.

(2) In non-calcareous soils, thorium adsorption is extremely sensitive

to initial thorium solution concentrations. In organic materials,

increased pH causes increased humic acid solubility and thorium

complexation, resulting in lower K values. In calcareous soils,d

K values are high (> 10 mL/g), regardless of pH or thorium con-

centration, because of the buffering capacity of the soil and the

precipitation of Th(0H)4<

(3) K., values are generally high, (> 103 mL/g), in dilute solutions,

indicating limited thorium migration.

The recommended K value means, standard deviations, ranges and distribu-d

tion parameters for thorium by soil type, based on Table 14, are given in

Table 15.


TABLE 14

, VALUES FOR THORIUM : LITERATURE SURVEY SUtHARY

Soil 7, % Z 7, 7, pH E. CECType Sand Silt Clay Organic C3CO3 Saturated Paste (V) (meq/100 g) I

7. Free Competingran Oxides Cation

Soil Locationor Description Reference

Sand 45 <XS1O,)40 (7-

40 (Z

Organic 5 (X

5 a

30

60

60

12

12

0

0

60

60

25 C. car-bonate)

0 (Z car-bonate)

0 (% car-bonate)

23 (7, car-bonate)

23 (2 car-bonate)

7.0

3.2

4.8

6.7

7.4

Th Cone. 1.5xl05 Cadarache sediment tencon, 1973(1 g/L)Th Cone. 8 clay schist Bancon, 1973(1 g/L)Th Cone. lx lO 5 c l ay sch i s t Rancon, 1973(0 .1 g/L)Th Cone. 8x10'* rt\<er peat tencon, 1973

(lgA.)Th Cone. 1.5x10* river peat(0.1 g/L)

Rancon, 1973

- 25 -

SoilType

Clay

Organic

(mL/g)

5.0x10 **

4.75xlO474

S.D.

.0710x104

.5962x104

TABLE

FOR

n

CSI

CM

15

THORIUM

K^ Range(mL/g)

8.0 to 1.0x105

l.SxlO'' to 8.0x10 h2

4

LognormalDistribution

.95 2.90

.54 0.5141


log^QK, for thorium, with a corresponding standard deviation of 0.6 (see

Table 1). Allard et ai. (1977) reported K ranges from 40 to 316 mL/g andd

500 to 1260 mL/g for clay/mud and granite, respectively. Vandergraaf (1982)

recommended a K value for thorium of 850 mL/g for granite.

Thorium References

Allard, B., H. Kipatsi and J. Rydberg. 1977. Sorption of long-lived radio-nuclides in clay and rock. Part 1. Determination of DistributionCoefficients. KBS Technical Report 55.


Johnston, H.M. and R.W. Glllham. 1980. A review of selected radlonuclldedistribution coefficients of geologic materials. Atomic Energy ofCanada Limited Technical Record, TR-90*.

Ran^on, D. 1973. The behaviour in underground environments of uranium andthorium discharged by the nuclear industry. In: Environmental Behav-iour of Radionuclides Released in the Nuclear Industry. InternationalAtomic Energy Agency Report, IAEA-SM-172/55.

Sheppard, M.I. 1980. The environmental behaviour of uranium and thorium.Atomic Energy of Canada Limited Report, AECL-6795.



- 26 -

3.11 URANIUM

Several reviews of uranium chemistry exist (Harmsen and de Haan,

1980; Borovec, 1981; Sheppard, 1980), but few K values have been reported

in the literature. The summary on uranium geochemistry presented by John-

ston and Gillham (1980) indicates that

(1) in oxidizing environments, U ***" compounds are stable and can pre-

cipitate, whereas U4* is stable in a reducing environment and

would precipitate as U02; thus the oxidation-reduction status is

important;

(2) soluble uranium (U6*) can be adsorbed or reduced by organic mat-

ter; if U6"1" is reduced to U4"1", precipitation can occur;

(3) UC^2* can be adsorbed by clay minerals by cation exchange, but may

also form complexes with anions such as carbonate or phosphate.

Borovec (1981) indicated that K, values for uranium for clay minerals range

from 50 to 1000 mL/g and for peat from 10 4 to 106 mL/g. The recommended

K, value means, standard deviations, ranges and distribution parameters for

uranium by soil type, based on Table 16, are given in Table 17.

SoilType

Sand

Clay

8

2

(mL?g)

.065

.6349x10511

4.

*d

S.D.

.22

5597x10

TABLE

FOR

n

25 3

17

URANIUM

KJ Range(mL/g)

0.13 to 16.0

200 to 7.9x105

LognormalDistribution

u a

0

3

.159 1.478

.543 2.040


log1QK for uranium, with a corresponding standard deviation of 0.6 (see

TABLE 16

K. VALUES FOR URANIUM : LITERATURE SURVEY SUrMAKY

SoU I * Z X * pM« E^ <SC * FreeType Sand Silt Clay Organic CaCX)3 Saturated Paste (meq/lQO g) Iron Oxides Catlcn (Jg)

Soil locationor Description

Sand

SiltOjy.

Organic

45 -; sioj)

30

sandy soilalluvial i

40; SID2)

abyssal redabyssal red

5

: sin,)

soil60

cLsvclay

12

< 1

--0

-60

25 OS car-bonate)

--

0 (Z car-bonate)

--

23 (7. car-bonate)

<

i

2.7,

7

7

.8

.17

Cadarache seduisnt I^ncon» 1973

4.3 ug CD^/wL 0.134.3 ug tT3

2-/nL 0.25270 altered schist

0.68 rolA NaCI 2000.68 m l A Nad 7.9J1O5 - -

33 organic pest

Yataicto et a l . , 1973Yanancto et a l - . 1973Rancon, 1973

Erickson, 1980Erlckson, 1980Rancon, 1973

Iro

- 28 -

Table 1). Allard et al. (1977) reported K, ranges from 2.5 to 20 mL/g ford

clay/mud and 4 to 13 mL/g for granites. Vandergraaf (1982) recommended a Kd

range of 0.4 to 10 mL/g for granites.

Uranium References

Allard, B., H. Kipatsi and J. Rydberg. 1977. Sorption of long-lived radio-nuclides in clay and rock. Part 1. Determination of DistributionCoefficients. KBS Technical Report 55.

Baes H I , C.F. and R.D. Sharp. 1981. Predicting radionuclide leaching fromroot zone soil for assessment applications. Oak Ridge National Labora-tory Report, CONF-810606-44.

Borovec, Z. 1981. The adsorption of uranyl species by fine clay. Chem.Geol. 32_, 45-48.


Harmsen, K. and F.A.M. de Haan. 1980. Occurrence and behaviour of uraniumand thorium in soil and water. Neth. J. Agric. Sci. 8_, 40-62.


Ran$on, D. 1973. The behaviour in underground environments of uranium andthorium discharged by the nuclear industry. _In: Environmental Behav-iour of Radlonuclides Released in the Nuclear Industry. InternationalAtomic Energy Agency Report, IAEA-SM-172/55.



Yamaraoto, T., E. Yunoki, M. Yamakawa and M. Shimizu. 1973. Studies onenvironmental contamination by uranium. 3: The effects of carbonateIon on uranium adsorption to and desorption from soils. J. Radiat.Res. 14_, 219.


- 29 -

4. DISTRIBUTION COEFFICIENTS FOR FISSION PRODUCTS

4.1 CALCIUM

K, values for calcium reported by Graham (1973) and Graham and

Silva (1979) vary from 1 x 10-3 to 9.8 mL/g; however, there is some

confusion about the units. Wong et al. (1983) reported K values of 1117

and 1900 mL/g for a sand and a muck soil, respectively. It is recommended

that the K values for strontium be used for calcium (see Section 4.11).

Calcium References

Graham, E.R. 1973. Selective distribution and labile pools of micronutri-ent elements as factors affecting plant uptake. Soil Sci. Soc. A'Jier.Proc. 37_, 70-74.

Graham, E.R. and C.G. Silva. 1979. Labile pools and distribution coeffi-cients for soil calcium, magnesium, and potassium determined with ox-change equilibria and radioisotopes. Soil Science 128, 17-22.

Wong, K.V., S. Sengupta, D. Dasgupta, E.L. Daly, Jr., N. Nemerow and H.P.Gerrish. 1983. Heavy metal migration in soil-leachate systems. Bio-cycle 24, 30-33.

4.2 CARBON

Allard et al. (1981) studied the sorption of Hi£*C0 ~ on some

solids using the batch technique. The sorption of 14C was generally low,

but appeared to increase with increasing calcium content of the solid.

Retardation factors of up to 3 (i.e., three times slower transport of i4C

than of water) were measured for calcite. Concrete will probably retain

most of the 14C, and a retardation factor >10 might be expected for a

bentonite-quartz mixture (K, = 2.2 x 10"6 mL/g). Owing to the paucity of

information, a conservative retardation factor of 1, or a K of 0 mL/g, is

recommended.

- 30 -

Carbon Reference

Allard, B., B. Torstenfelt and K. Andersson. 1981. Sorption behaviour of1L|C in groundwater/rock and in groundwater/concrete environments.Report Prav 4.27.

4.3 CESIUM

The work of Gillham et al. (1981a) is the most extensive on K.

values for cesium for Canadian soils. Their study showed that for 15 Cana-

dian soils, K values for cesium ranged from 1 x 10 2 to 2 x 10 4 mL/g, but

there was no significant correlation between the K value and measured soild

properties such as CEC, major cation concentration, clay mineral composi-

tion, organic matter content and pH. In more than half of the samples, how-

ever, the K values were related significantly to the natural exchangeable

cesium content of the soil, and this must be accounted for in sorption

studies.

The recommended K value means, standard deviations, ranges and

distribution parameters for cesium, based on Table 18, are given in Table

19.

SoilType

SandSiltClay

21631.1395xlO4

8379

K

S.D.

322678991.3613X101*

TABLE

_, FOR

n

24205

19

CESIU1

1065065

•1

K, Range(mL/g)

tototo

l.OxlO4

3.0x10h

3.15x10 *•

232

LognormalDistributionM- ^

.668 0.9332

.912 0.4227

.945 1.216


log1QK for cesium, with a corresponding standard deviation of 0.8 (see

Table 1). Allard et al. (1977) reported K ranges from 6 to 32 mL/g and 32

TABLE 18

SoUType

Sand

Silt

Clay

7.

Sari)

100

93%5259

6252

%6087-

94

Z

Silt

-

54

4524

3139

2229-

I

Clay '

-203

17792

184-

6 (<O.O74 ma)river sand

subsoil randclinoptilollte

84

63

363428123445

BurbankBurhankBurtn*ftn-nanV

13

32

sardsandsand353541553444

soilsoilsoilsoil

3

5

293111333211

alluvial silt loam• i

313818403445

7183

tedlun lnam69626645

5247927196

sUtv clay.sil ty clay44

315034

00

16151481

111

, f>*-3, PC-2

635

10&T < 0.02 mn

-lay

Savannah River serf.Savannah River sed.

-

0.05O.i".O.'«0~0o.y0.330.302.050.10

---

-

-----

0.16

0.21

---

0.430.401 .270.350.850.14(Ap)---

-----

----

0.230J31-

JOC03 Saturated Paste (V)

41.340.8000

18.343.411.17.10.07---

2-----

2.8

1.36

---

33.634.1

21.105.11.4-------------

3.85.2-

-

(<100 urn) -(<100 urn) -

8.3 (C«C12)7.8 (CaCl2)6.3 (Cad2)5.0 (CaCl,)6.5 (CaT.l2)7.6 (C*C12>8.0 (Cad2)8.0 (CaCl2)7.8 (Cad2)8.23 (CaCl2)

--

7-8

8.6------

-

7.07.07.0

8.1 (Cad2)8.1 (CaCl2)

6.7 (CaCl2)7.7 (Cad2)B.83 (CaCl2)

--------------

7.8 (Cad2)-

7-8

-7.0

K VALUES FOR CESIUM : LTBKAWRE SURVEY S

C£C 1 Free Coveting(meq/100 g) Iron Oxides Cation

1.41.21.11.61.92.20.70.4

21.25.0---

5-----

5.1

5.3

---

8.48.65.9

10.232.712.0

--2.62.76.31.84.91.54.23.55.2--

11.031.535

-

--

R«? ref.see ref.see ref.see ref.see ref.see ref.see ref.see ref-see ref.see ref.

so;

90S NaClsolution4 TOI/L NaCl

-grouncHoter3 HDI/L NaNO3

0.5 raol/L NJCI0.25 ITOI/L Ci£l2

0.63 0.2 nol/L Nadsee ref.

1.02 0.2 nclA Nadsee ref.

---- see ref*

see ref-

see ref.sec ref.

-0.1 nul/L W0,

-_--_-__--

1.21 0.2 tml/L NaClsee n-f.

- -

9CK NaClsolution

Nad_

V

(ot/8)

1.19x10^1.37x103

7.4X101

1.0x10"l.OxlO3

1.0x10"1.5xl02

5.OxlO2

l.OxlO2

1.5xlO3 ±189.5xlO?

10

16.44.2xlO3

9.OxlO3

4.66X102

1.09xl03

5.21xlO3

2.4OX1O3

3.51xlO3

98*84*40*1.78x10"1.84x10"

2.0x10"

l.OxlO1'1.35x10"3x10"6.5xlO2

5J2xlO 3

9.55xlO3

1.04x10"1.14x10"

7.3xlO3

6.2xlO3

2.07x10"1.52X1O11

2.0x10"3.OxlO3

2.7xlO3

3.96x103

1.0x10"3.15x10"

2x102

65 (n-8)130*

Soil Location

or Description

Soil *4 (IKRE)Soil ' 6 (Leamington)Soil HI (C1M.)+

Soil «8 (North Bay)Soil »10 (VNRF.)

Soi l #11 (WRE)SoU #12 ( a m ) *

Soil « 3 (C.F.B. Borden)SoU « 6 (Alberta)

320 Sediiuent B (Solution 1)

Iron & s i l t y sandsConposite s o i l

River sand

Hanford BubsoU

CUnopt i loUte (Idaho)Burbark soUBurbank so i lBurba* so i lBurhank so i l

Burhank sand (average profi le)

Ephrata sard (average profUe)

Four ndle creekPen BranchPar Pond

SoU »1 (1«RE)Soil n (KIRE)

SoU #5 (Leamington)Soil M (North Bay)SoU »14 (Alberta)

± 4741 Sediioent A (Solution 1)Captlna s i l t loan (Ap)SodpodzoUc s o i l

a l l uv ia l soU (Cadarache)a l i n r i a l soU (Cadarache)Vlndobonian sed. (Cadarache)

Vlndobonlan sed. (Cadarache)Vlndobonian sed. (Cadarache)Vindobooian sed. (Cadarache)

sandy-day sed. (Durance R.)sandy-clay sed. (Durance R.)

sandy-day sed. (Durance R.)s l l ty clay (Idaho)s l l ty clay (Idaho)Ritzvllle s i l t (avg. profile)SoU '15 (Alberta)very fine suspended sediments

(Durance River)clay

Savannah River sedLaentsSavannah River clay

Reference

Glllham et a l . , 1981aGlUham et a l . , 1981aCUlhan et a l . , 1981aGUlham et a l . , 1981aGlllham et a l . , 1981aGlllham et a'.., 1981aClllhan et a l . , 1981aGUlham et a l . , 1981aGlllham et a l . , 1981aSeme et a l . , 1978Tyrochowlcz, 1981SchmLt, 1972Harotra S Verkerk, 1977

BrxJes, 1957Wlldung 4 Rhodes, 1963Hajek 4 Aoes, 1968Hajek 4 ABES, 1968Hajek 4 Aces, 1968Hajek S, Area, 1968RoutBon, 1973

Rcutaon, 1973

Zelazny et a l . , 1978Zelazny et a l . , 1978Zelazny et a l . , 1978GUlham et a l . , 1981aClllhaa et a l . , 198UClllham et a l . , 1981aGlllham et a l . , 1981aGUlhas et a l . , 1981aSeme et a l . , 1978Rogowkl 4 Taoura, 1965Aleksakhln, 1965Rancon, 1972Rancon, 1972Rancpn, 1972Rancon, 1972Rancon, 1972Rancon, 1972Rancrm, 1972Rancon, 1972Rancon, 1972Ulldung I Rhodes, 1963Wlldffi££ & FnoQCSf I763Rutson, 1973Glllhao et a l . , 1981aRancon, 1972

Hanstra 4 Verkerk, 1977

Elprince « a l . , 1977Zelazny et a l . , 1978

CW1L - Chalk River Nuclear Laboratories, Chalk River, Ontario

HFP - Rnre Nuclear Pc*«r Development

AL«w dat^ for sorption versus p?I, see reference.

- 32 -

to 794 mL/g for clay/mud and granite, respectively. Vandergraaf (1982)

recommended a K,range of 40 to 1000 mL/g for granite.

Cesium References

Aleksakhln, R.M. 1965. Radioactive contamination of soils and plants.USAEC Report AEC-tr-6631.

Allard, B., H. Kipatsi and J. Rydberg. 1977. Sorptlon of long-lived radio-nuclides in clay and rock. Part 1. Determination of DistributionCoefficients. K.BS Technical Report 55.


Elprince, A.M., C.I. Rich and D.C. Martens. 1977. Effect of temperatureand hydroxy aluminum interlayers on the adsorption of trace radioactivecesium by sediments near water-cooled nuclear reactors. Water Resour.Res. 13_, 375-380.

Gillham, R.W., L.E. Lindsay, W.D. Reynolds, T.J. Kewen, J.A. Cherry and M.R.Reddy. 1981a. Studies of cesium and strontium migration in unconsoli-dated Canadian geological materials. Atomic Energy Control Board Re-port, INFO-0049.

Hajek, B.F. and L.L. Ames, Jr. 1968. Strontium and cesium equilibriumdistribution coefficients: Batch and column determinations.BNWL-481-3.

Hamstra, J. and Verkerk, B. 1977. Review of Netherlands program for geo-logic disposal of radioactive waste. JLn_: Nuclear Power and its FuelCycle. International Atomic Energy Agency Report, IAEA-CN-36/289.

Rancon, D. 1972. Practical utilization of the distribution coefficient forthe measurement of the radioactive contamination of minerals in rocks,soil and subterranean water. Cadarache Nuclear CEA Research Center,ANL-trans-931, Report-R-4274.

Rhodes, II.W. 1957. The effect of pH on the uptake of radioactive isotopesfrom solution by a soil, boil Sci. Amer. Proc. n_, 389-392.

Rogowski, A.S. and T. Tamura. 1965. Movement of 137Cs by runoff, erosionand infiltration on the alluvial Captina silt loam. Health Phys-11_, 1333-1340.

Routson, R..C. 1973. A review of studies on soil-waste relationships on theHanford Reservation from 1944 to 1967. BNWL-1464, UC-70.

- 33 -

Serne, R.J., D. Rat and S.J. Phillipso 1978. Monitoring and physical char-acterization of unsaturated zone transport: Laboratory analysis. In:Nuclear Waste Management Quarterly Progress Report Oct.-Dec. 1977,Pacific Northwest Laboratory Report, PNL-2377-4, UC-70.

Schmalz, B.L. 1972. Radionuclide distribution in soil mantle of the litho-sphere as a consequence of waste disposal at the National Reactor Test-ing Station, USAEC Report, IDO-10049.

Tymochowicz, S. 1981. Sorptive properties of mineral deposits occurring inPoland. Nukleonika, 26, 595-599.

Wildung, M.W. and D.W. Rhodes. 1963. Removal of radioisotopes from solu-tion by earth materials from eastern Idaho. IDC-14624.


Zelazny, L.W., D.C. Martens, A.M. El-Prince and C.I. Rich. 1978. Effect oftemperature and hydroxy-aluminum interlayers on cesium selectivity andfixation in river suspensions and soils. ORO-4851-2.

4.4 IODINE

The most extensive study of iodine adsorption on soil was that of

Wildung et al. (1974). Johnston and Gillham (1980) have summarized the

known soil chemistry of iodine as follows:

(1) the most stable form of iodine in both oxidizing and reducing

environments is iodide, I~. Because the predominant iodine spe-

cies is an anion, ion exchange would not be important in soil

adsorption, particularly at neutral or high pH values.

(2) organic matter appears to be a significant factor in iodine ad-

sorption.

(3) K, values for iodine range from 0.1 to 50 mL/g, depending on the

form of the iodine and the pH of the solution. The maximum Kd

value would be obtained for I~ at a pH of 4 to 6.


- 34 -

Since no K, values for specific soils were found in the literature, thed

multiple-regression equations (based on iodide (I~) and methyl iodide (CH3I)

interactions with 22 soils) reported by Wildung et al. (1974) were applied

to soils already described in this report. The K, values were calculatedd

only for soils whose properties were within the range of the soils used togenerate the multiple-regression equations. The equations for iodide K, and

dmethyl iodide K, differ, and are

d

K. = 0.33 X, + 0.09 X, (5)diodide l 3

K, ,_ , = 0.027 X,, + 0.10 Xo (6)d methyl 2 3

iodide

where X, is the silt content (range for equation development is 17.6 to

58.0%),

X 2 is the clay content (range for equation development is 3.8 to

46.6%), and

X3 is the organic carbon content (range for equation development

is 0.23 to 28.8%).

The recommended K. value means, standard deviations, ranges and distribu-d

tion parameters by soil type (using Equation (6) since it will predict the

lowest K, values because methyl i

Table 20, are given in Table 21.

lowest K, values because methyl iodide is more highly mobile), based on

TABLE 21

K, FOR IODINE—q

Soil KJ S.D. n KJ Range LognormalType (nL/g) OnL/g) Distribution

\i a

Sand 0.5514 0.3595 7 0.2 to 1.210 -0.3404 0.2929Silt 0.9145 0.3201 11 0.18 to 1.50 -7.99xlO~2 0.2351Clay 1.293 0.3697 4 1.03 to 1.83 9.952x10"2 0.1140

- 35 -

TABLE 2 0

K VALUES FOR l O D D E : LITERATURE SURVEY SUMMARY-d •

CalculatedS o i l X X X K .Type Silt Clay Organic (mL/g)


Reference

Sand

Silt

Clay

31392229392820505453353635415534

5034323234

79185

.4 18

.4 22

.0 3634371625293131333229

635363656

.8

.0

.4

.0

.1

0.38

0.332.050.450.600.982.40.82.33.60.430.410.401.270.350.857.1

0.230.81

1.02.73.2

0.0.0.0.0.0.1.1.1.0.0.0.0.0.0.0.1.

0.1.1.1.1.

2328692055702100237983828896939450

1803072483

Soil lll\ (WNRE)

Soil 012 (BNPD)Soil #16 (Alberta)Hanford AIdaho AIdaho DColorado A

Idaho A

Arkansas CIllinoisSoil Itl (WNRE)Soil 112 (WNRE)Soil 113 (WNRE)Soil 115 (Lemlngton)Soil 119 (North Bay)Soil 014 (Alberta)Brookston stlt(average profile)Ritzvllle siltSoil #15 (Alberta)Tennessee (Oak Ridge)New York (West Valley)Arkansas A

Cillham et al., 1981aClllham et al., 1981aCillham et al., 1981aAmes & Ral, 1978Ames & Ral, 1978Glover et al., 1976Glover et al., 1976Glover et al., 1976Glover et al., 1976Glover et al., 1976Gillhara et al., 1981aGillham et al., 1981aGlllhara et al., 1981aGill ham et al., 1981aGillham et al., 1981aGillham et al., 1981aJuo & Barber, 1970

Routson, 1973Gillham et al., 1981aGlover et al., 1976Glover et al., 1976Glover et al., 1976

The K, range reported for methyl iodide in soil was 0.1 to 3.1

(Wildung et al., 1974). The multiple-regression equations were developed

for mineral soils. A single value of > 30 mL/g for charcoal is pertinent to

organic soil (Novak, 1981). Vandergraaf (1982) recommended a K, value for

iodine of 0 mL/g, until a cationlc species of iodine is identified.

Iodine References

Ames, L-L. and D. Rai. 1978. Radionuclide interactions with soil and rockmedia, Volume 1. U.S. Environmental Protection Agency Report, EPA520/6-78-007.


Juo, A.S.R. and S.A. Barker. 1970. The retention of strontium by soils asinfluenced by pH, organic matter and saturation cations. Soil Sci.109, 143-U8.

- 36 -

Gillham, R.W., L.E. Lindsay, W.D. Reynolds, T.J. Kewen, J.A. Cherry andM.R. Reddy. 1981a. Studies of cesium and strontium migration in un-consolidated Canadian geological materials. Atomic Energy ControlBoard Report, INFO-0049.

Glover, P.A., F.J. Miner and W.O. Polzer. 1976. Plutonium and aaiericiumbehaviour in the soil/water environment. I. Sorption of plutonium andamericium by soils. In: Proceedings of the Actinide-Sediment Reac-tions Working Meeting at Seattle, Washington on 1976 Feb. 10-11. Bat-telle Pacific Northwest Laboratories Report, BNWL-2117, pp. 225-254.

Nowak, E.J. 1981. Composite backfill materials for radioactive waste iso-lation by deep burial in salt. Scientific Basis of Nuclear Waste Man-agement 2. 545-552.

Routson, R.C. 1973. A review of studies on soil-waste relationships on theHanford Reservation from 1944 to 1967. Battelle Pacific NorthwestLaboratories Report, BNWL-1464, UC-70.


Wildung, R.E., R.C. Routson, R.J. Serne and T.R. Garland. 1974. Pertech-netate, iodide, and methyl iodide retention by surface soils. BNWL-SA-5195.

4.5 MOLYBDENUM

No data were found in the literature for molybdenum; however,

E its position in t

can be used for molybdenum.

because of its position in the Periodic Table, the K. values for technetiumd

4.6 NICKEL

Little information exists for soil adsorption of nickel. Swanson

(1981) reported a range of K, values for nickel of 5.2 x 10 1 tod

1.2 x 104 mL/g for a selected size fraction of Hanford soil (75 to 150 JJU)

with a soil-to-solution ratio of 0.010 g/mL. Contradictory results and the

use of organic complexants in the Swanson experiments indicate that values

for specific samples should not be used.


- 37 -

Gerritse et al. (1982) suggested that the K, value range ford

nickel is 1 x 10 2 to 1 x 103 inL/g. They reported two sandy mineral soil

values of 6 x 10 * and 3.4 x 10 2 mL/g and four peat soil values of 3.6 x 10 2,

6 x 102, 9.9 x 10 2 and 4.7 x 10 3 mL/g. Wong et al. (1983) reported K

values of 604 and 1437 tnL/g for a saftd and a muck soil, respectively. The

recommended values of \i and a for the K, distribution for nickel, based ond

this information and distribution information for the other nuclides, are

given in Table 22.TABLE 22

RECOMMENDED VALUES OF n AND o FOR NICKEL

Soil Lognorraal DistributionType (i a

SandSiltClay

Organic

1.52.03.03.0

1.0• 1 . 0

1.01.0

Nickel References

Gerritse, R.G., R. Vriesema, J.W. Dalenberg and H.P. De Roos. 1982. Effectof sewage sludge on trace element mobility in soils. J. Environ. Qual.11_, 359-364.

Swanson, J.L. 1981. Effect of organic complexants on the mobility of low-level waste radionuclides in soils: Status report. Pacific NorthwestLaboratory Report, PNL-3927, UC-70.

Wong, K.V., S. Sengupta, D. Dasgupta, E.L. Daly, Jr., N. Nemerow and H.P.Gerrish. 1983. Heavy metal migration in soil-leachate systems. Bio-cycle 24_, 30-33.

4.7 PALLADIUM

No specific information was found on soil adsorption of palladium.

We suggest that the K, values for nickel be used for palladium. Vandergraaf

- 38 -

(1982) reported a range of 0 to 28 mL/g for the K of palladium for granite.d

He recommended that a K value of 11 mL/g be used.d

Palladium Reference


4.8 RARE EARTHS - TERBIUM, SAMARIUM AND CERIUM

Terbium, samarium and cerium are fission products, and it is con-

venient to discuss these three rare-earth elements together because of their

chemical similarity. Cerium was the only one of these elements for which

data were found. Vandergraaf (1982) reported that the K, value for ceriuma

ranges from 250 to 5000 mL/g, and recommended a value of 1000 mL/g. Allard

et al. (1977) reported a K range for cerium of 100 to 10 000 mL/g for

clay/ mud and 1000 to 1.6 x 104 mL/g for granite. Baes and Sharp (1981)

suggested a mean value of 3.0 for the logigK, for cerium, with a correspon-

ding standard deviation of 0.6, and a K range of 58 to 6000 mL/g (see

Table 1) for all soils. We recommend using the values of Baes and Sharp for

all soil types.

Rare Earths References

Allard, B., H. Kipatsi and J. Rydberg. 1977. Sorption of long-lived radio-nuclides in clay and rock. Part 1. Determination of DistributionCoefficients. KBS Technical R.eport 55.



Unrestricted, unpublished report, available from SDDO, Atomic Energy ofCanada Limited Research Company, Chalk River, Ontario K0J 1JO.

- 39 -

4.9 SELENIUM

Elsokkary (1980) reported selenium adsorption for three soils,

which allowed the computation of K. values of 1.6, 2.2 and 2.5 mL/g on a

clay soil and two silty soils, respectively. Frost and Griffin (1977)

reported a K, value of ~ 50 mL/g for HSeO3~ adsorption on calcium-montmoril-

lonite at a pH of 7. Singh et al. (1981) reported K, values ranging from 3d

to 73 mL/g for selenate adsorption on sandy soils. Since insufficient data

are available, we suggest that the values for polonium be used for assess-

ment purposes.

Selenium References

Elsokkary, I.H. 1980. Selenium distribution chemical fractionation andadsorption in some Egyptian alluvial and lacustrine soils. Z. Pflan-zenernaehr. Bodenkd., 143, 74-83.

Frost, R.R. and R.A. Griffin. 1977. Effect of pH on adsorption of arsenicand selenium from landfill leachate by clay minerals. Soil Sci. Soc.Amer. J. 4^, 53-57.

Singh, M., N. Singh and P.S. Relan. 1981. Adsorption and desorption ofselenite and selenate selenium on different soils. Soil Sci. 132,134-141.

4.10 SILVER

Little information exists for soil adsorption of silver and no

specific soil K, values were found. Consequently, it is suggested that in-d

formation for copper be used for silver because of their proximity In the

Periodic Table. Gerritse et al. (1982) suggested that the K. value rangea

for silver is 1 x 103 to 1 x 105 mL/g. They reported K values of 1.6 x 10 2

and 5.6 x 102 mL/g for copper on sandy mineral soil, and K values ofd

4.4 x 103, 1.7 x 104, 2.2 x 10h and 3.3 x 104 mL/g for copper on peaty soil.

Values for copper also ranged from 5.5 x 104 to 1.2 x 105 mL/g for 0 to

0.9 meq Ca^/g dry peat. Wong et al. (1983) reported K, values for copper

of 206 and 197 mL/g for a sand and a muck soil, respectively. The recom-

mended K, distribution parameter values for silver, based on this informa-

d

tion, on the distribution information for the other nuclides and on Table23. are given in Table 24.

, VALUES FOR SILVER : IJTERAUJRE SURVEY SHHAKI

Type Sirai Silt Clay CdX, Saturated Pasted C X Free Competing

(neqAOO g) Iron Oxides Cation Wg)Sol i Locationor Description ftefer-ence

0

20---

----_

3.5

2,5__

__

90>90>9Q

>90

4.5-5.07.5-8.0

£.86.25.07.46.64.5

4 to 56

6.2

22

16-_-

----—

1.6riO2 Soil C5.6xlO2 Soil D

0.1 nDl/L Cad2 2.7 Florida 1 - sand0.1 rol/l &C12 33.00.1 UDIA. CaCt2 28.0

0.1 ml/L CaCl2 2000.1 iml/L CaQ2 333

Gerrttse et a l . , 1982Gerrltse et a l . , 1982Ctahaa, 1973

Florida 2 - Band + organic oatt£r Grahan, 1973Mssourl 23 Grahan, 1973Missouri 24 Grahai, 1973Mssouri 38 Grahan, 1973

4.4xl03 Soil A Gerritse et a l . , 19822.2xlOJ< Peat A Gerritse et a l . , 19821.7x10" Peat B Gerrltse et a l . , 19823.3idO^ Soil B GHirltce et a l . , 1982

O

I

- 41 -

TABLE 24

RECOMMENDED VALUES OF u AND a FOR SILVER

Lognormal DistributionSoil Type |i a n

Sand 1.726 0.9988 4

Silt 2.090 0.5678 3Clay 4.0Organic 4.184 0.3792 4

Silver References

Gerritse, R.G., R. Vriesema, J.W. Dalenberg and H.P. De Roos. 1982. Effectof sewage sludge on trace element mobility in soils. J. Environ. Qual.ll_, 359-364.

Graham, E.R. 1973. Selective distribution and labile pools of raicronutri-ent elements as factors affecting plant uptake. Soil Sci. Soc. Amer.Proc. 3]_, 70-74.

Wong, K.V., S. Sengupta, D. Dasgupta, E-L. Daly, Jr., N. Nemerow and H.P.Gerrish. 1983. Heavy metal migration in soil-leachate systems. Bio-cycle 24, 30-33.

4.11 STRONTIUM

The most extensive report on strontium K, values for Canadian

soils is the work of Gillham et al. (1981a). For 15 Canadian soils, the Kd

values ranged from 2.5 to 1 x 10 2 mL/g. The study also showed that stron-

tium "in some or possibly many circumstances would migrate at velocities

smaller than the groundwater velocity but at velocities which nevertheless

could be significant."

The recommended K, value means, standard deviations, ranges and

distribution parameters for strontium by soil type, based on Table 25, are

given in Table 26.

TABLE 25

SoliType

zSand

ZSilt

7.day Organic

XOCO,J Satura ted Paste

K, VALUES PCR SntCNITLtl :

CEC Z Free(meq/100 g) Iron Oxide

LITERATURE

Competings Cation

SURVEY S*MARY

<"L?g)Soil Locationor Description Inference

1009396525962966087

4524312

229

203

1772

18A

9.030.050.51

o.oe0.40J.380.302.050.10

94 6 (<0.0/« ran) -

subsoil sandsand 20

Burlnnk soilEurha* m i lBurbar* soliBurhenk soil

84 13 3

63 32 5

p i l f e r sandaquifer sandaquifer sandaquifer sandaquifer sandaquifer sand

2.9

41.340.8000

18.311.17.10.07

8.3 (CadJ7.8 (CaCl.,)6.3 (CaCX,)5.0 (CaCl,)6.5 (CaClj)7.6 (CaCl,)8.0 CCad.)7.8 (CaCl,)8.23 ( d

aC l ,Cad ,) -

1.41.2l. l1.61.92.20.4

21.25.0

519.2

-

5.55.55.55.55.55.5

-

-

DM0.420.420.420.420.42

5.1

5.3

0.25-0.90.25-0.90.25-0.90.25-0.90.25-0.90.25-0.9

see ref.see ref.see ref.see ref.see ref.see ref.see ref.see ref.see ref.

-902 Nadsolution4 rol/L Na+,0.01 mol/L PO,,-

3xlCT3 raol/LSra 2

graundwater3 rol/L NaTO3

0.5 ml/L feel3ncl/LNa0A:0.2 m l A NaClsee ref.0.2 ml/L teasee ref.see ref.*see ref.*see ref.*see ref.*see ref.*see ref.»see ref*

2.0x10'2.52.0xi0'l.OxlO2

2.5x10'5.0x10'1.0x10'5.0x10'l.HxlO2 • 92.4x10'2

1.2x10'

8.0x10'10

4.8x10'2.17.32.231.62x10'

1.6x10'

1.42xl0'9.27.81.67x10'1.13x10'6.0

Soil S4 (WIRE)Soil lib (Leanlngton)Soil IP (CR.NL)Soil 118 (North Bay)Soil »IO (VtJRE)Soil #11 (UffiE)Soil W3 (C.F.B. Borden)Soil »16 (Alberta)Sediment B (Solution 1)Cbnposlte soilRiver sand

ftaford subsoil

Hmford subsoUSldell sand

Burbank soilBurbank soUBurbank soilBurbank soilBurbsnk sand (average profile)

fyhrata sand (average profile)

Chalk River (CR) aquifer sandChalk River (RA) aquifer sandChalk River (Q) aquifer sandChalk River (SB) aquifer sandChalk River 00 aquifer sandChalk River (HA) araiifer sand

Gillhamet a l . , 1981aGillham et a l . , 1981aGillham et a l . , 1981aGlllhan et a l . , 1981aGlllhsm et a l . , 1981aGillham et a l . , 1981aGillham et a l . , 1981aGillham et a l . , 198LaSeme et a l . , 1978Sctaal*. 1972Hratra S Vertetk, 1977

Rhodes, 1957

Rx>des, 1957Juo b Barber, 1970

llajek S. ta, 1968fejek i J tes, 1968H3jek 4 tees, 1963Hajek I tes, 1968Houcson, 1973

Rojtson, 1973

Patterson & SpDel, 1981Patterson i Spoel, 1981Patterson & Spoel, 1981Patterson & Spoel. 1981Patterson & Spoel, 1981Patterson 5 Spoel, 1981

ro

I

TABLE 25 (Collided)

SoU 7. :

Type Sand Sil t

Silt 363534281234

45

35363541553444

7. 7.

Clay Organic

29

2131313332

11medlun lonn 31.6

medlun 1c

31381840

34457

183

696266455247927196

s U t

44Clay 31

heavy

heavy

heavy

5034lcs

0.430.410.401.270.350.850.142.94

(0.01 am)m 41.6

(0.01 mn]00

1615148

1111

29.1

635

c 53.41(0.01 am)

losm 46.67.(0.01 on)

loan 67 .Wrn m ™.\

clayey 60.7Z(0.01 am)

100Z (<0.02 nn)

Organic muck '

1.28

----

-----

7 .1

0.230.812.04

-

4.87

6.86

-

(9.8

7.

CaCO,

33.633.834.121.10

5.11.4-

-

----

-----

-

3.85.2-

-

-

_

-

Saturated Pasts (V)

8.1 (OC12)8.1 (CaCl2)8.1 (CaCl2)7.7 (CaCl2)6.7 (CaCl2)7.7 (CaCl2)8.83 (CaCl,)

6 .6

8.4

----

--

- ---

6

„

7.8 (CaCl-,)6.6

6.7

8 .0

6.8

-

7 . 0

CEC 7. Free(meq/100 g) Iron Oxide

8.48 .38.65.9

10.232.712.010.6

12.2

2.62.76.31.84 . 91.54 .2

3.55.2

39.4

11.0 1.2131.526.1

30.4

32.9

32.2

35

70.0

Competings Cation

see ref .see ref.see ref.see ref.see re f .Bee ref.see ref .

-

-

----

-----

3xlO"3 rol/L

StClo*0.2 rol/L Nadsee ref.

-

-

-

_

-

3x10-3 ml/ISrCl2

(°i./g)

2.0x10'2 .0x10 '2.0x10'1.0x10'l.OxlO2

8.01.12xlO2± 13.OxlO2 ±

1.7X102 ±

1.4x10'2.3x10'1.8x10'1.6x10'1.6x10'1.4x10'2.2x10'1.6x10'1.6x10'5.0x10'

2.47x10'85.7xlO2 +

l . tSx lO 3 :

A.3X102 ±

A.9X102 t

4 .7x10 '

l .SxlO 2

60

30

80

SoU Locationor Description

Soi l #1 (WRE)SoU #2 (WTO)SoU »3 (VKRE)SoU K (Leanlngton)SoU m (North Bay)SoU #14 (Albert*)Sediment A (Solution I)low ash podzollc

Serozafl

alluvial soil (Cadarache)alluvial soil (Cadarache)Vlndobonian sed. (Cadarache)Vlndobonlan sed. (Cadarache)Vlndobonian sed. (Cadarache)Vlidobonlan sed. (Cadarache)sandy-day Bed. (Durance R.)sandy-clay sed. (Durance R.)sandy-day sed. (Durance R.)Brookston s U t

RitzvUle sUt (avg. profile)Soil #15 (Alberta)Chestnut

t 140 Leached Chernozem

X

50

Southern Chernozem

Thick Chernozem

very fine suspaded oedinent(Durance River)Muck

Reference

Glllhai et a l . , 1981aGUlham et a l . , 1981aGOJhai et a l . , 1981aGlllham et a l . , 1981aGUlham e t a l . , 1981aGil lhao e t a l . , 1981aSeme e t a l . , 1978A l e k s a k h K 1965

Aleksakhin, 1965

Rancon, 1972Rsncon, 1972Rancon, 1972Rsncon, 1972fancon, 1972Rjncon, 1972Rancon, 1972Rancon, 1972Rancon, 1972Juo 5 Barber, 1970

Routson, 1973Gillham e t a l . , 1981oAleksakhin, 1965

Aleksakhlit, 1965

Aleksakhln, 1965

Aleksakhin, 1965

Rancon, 1972

J<x> 4 Barber, 1970

Data available for competing cations sodlun, potasslun, magneslun, calclun, barlun and hydrogen.

- 44 -

SoilType

Sand

Silt

Clay

(mL/g)

26.02

49.49

449.2

S.

30.

72.

415

D.

21

44

.7

TABLE 26

Kj FOR STRONTIUM

n

26

20

6

Kd Range(mL/g)-

2.0 to 114

8.0 to 300

8.0 to 1150

1

1

2

LognormalDistributionH 0

.162 0.4964

.436 0.4254

.286 0.8239


log1QK, for strontium, with a corresponding standard deviation of 0.9 (see

Table 1). K values for strontium determined for various pure clay minerals

ranged from 0.2 to 9.0 mL/g (Wahlberg et al., 1965). K , values determinedd

for various minerals (including clay minerals) ranged from 0 mL/g for quartz

to 2.1 x 103 mL/g for alumina (both at pH = 7.5) in a natural water solution

and from 1 mL/g for quartz to 1.44 x 103 mL/g for alumina (both at pH = 7.0)

in a 0.1 mol/L sodium nitrate solution (Tamura, 1972). Palmer et al. (1981)

also reported extensive results for strontium sorption on pure clay, clay/

silica and alumina/clay for various solution compositions and pH. Allard et

al.(1977) reported a K, range of 20 to 63 mL/g for clay/mud and a range of 3

to 16 mL/g for granite. Vandergraaf (1982) recommended a K range ford

strontium of 0.6 to 600 mL/g for granite.

Strontium ReferencesAllard, B., H. Kipatsi and J. Rydberg. 1977. Sorption of long-lived radio-nuclides in clay and rock. Part 1. Determination of DistributionCoefficients. KBS Technical Report 55.

Aleksakhln, R.M. 1965. Radioactive contamination of soils and plants.USAEC Report AEC-tr-6631.


- 45 -

Gillham, R.W., L.E. Lindsay, W.D. Reynolds, T.J. Kewen, J.A. Cherry and M.R.Reddy. 1981a. Studies of cesium and strontium migration in unconsoli-dated Canadian geological materials. Atomic Energy Control Board Re-port, INFO-0049.

Hajek, B.F. and L-L. Ames, Jr. 1968. Strontium and cesium equilibriumdistribution coefficients: Batch and column determinations. BattellePacific Northwest Laboratories Report, BNWL-481-3.

Hamstra, J. and B. Verkerk. 1977. Review of Netherlands program for geo-logic disposal of radioactive waste. In: Nuclear Power and its FuelCycle. International Atomic Energy Agency Report, IAEA-CN-36/289.

Juo, A.S.R. and S-A- Barber. 1970. The retention of strontium by soilsinfluenced by pH, organic matter and saturation cations. Soil Sci.109, 143-148.

Palmer, D.A., S.Y.Shiao and R.E. Meyer. 1981. Adsorption of nuclides onmixtures of minerals. J. Inorg. Nucl. Chem. 3_, 3317-3322.

Patterson, R.J. and T. Spoel. 1981. Laboratory measurements of the stron-tium distribution coefficient K,Sr for seaquifer. Water Resour. Res. j7_, 513-520.tiura distribution coefficient K,Sr for sediments from a shallow sand

Ranc.on, D. 1972. Practical utilization of the distribution coefficient forthe measurement of the radioactive contamination of minerals in rocks,soil and subterranean water. Cardarache Nuclear CEA Research Center,ANL-trans-931, Report-R-4274.

Rhodes, D.W. 1957. The effect of pH on the uptake of radioactive isotopesfrom solution by a soil. Soil Sc. Am. Proc. 1_, 389-392.

Routsons R.C. 1973. A review of studies on soil-waste relationships on theHanford Reservation from 1944 to 1967. Battelle Pacific NorthwestLaboratories Report, BNWL-1464, UC-70.


Serne, R.J., D. Rai and S.J. Phillips. 1978. Monitoring and physical char-acterization of unsaturated zone transport: Laboratory analysis. In:Nuclear Waste Management Quarterly Progress Report 1977 Oct.-Dec.Pacific Northwest Laboratory Report, PNL-2377-4, UC-70.

Tamura, T. 1972. Sorption phenomena significant in radioactive waste dis-posal. Jji: Underground Waste Management and Environtaental Implica-tions. Araer. Assoc. Pet. Geol. Mem. 18^, 318-330.

- 46 -

Vandergraaf, T.T. 1982. A compilation of sorptlon coefficients for radio-nuclldes on granites and granitic rocks. Atomic Energy of Canada Lim-ited Technical Record, TR-120*.

Wahlberg, J.S., J.H. Baker, R.W. Vernon and R.S. Dewar. 1965. Exchangeadsorption of strontium on clay minerals. U.S. Geol. Surv. Bull.,1140-C, U.S. Government Printing Office, Washington.

4.12 TECHNETIUM

The environmental behaviour of technetium has recently been re-

viewed (Turcotte, 1982), as has the chemistry of technetium (Paquette et

al., 1980). Technetium migration is generally retarded under reducing con-

ditions (i.e., in geological formations), where it is less soluble. Techne-

tium, however, moves with the groundwater in aerated soils of low organic

carbon content. Johnston and Gillham (1980) indicated that

(1) because the pertechnetate ion, TcO^, is the most stable species

of technetiuni in aqueous solutions, TcO4" will not be subject to

ion exchange; hence, technetium will show little adsorption to

soil;

(2) in soils with appreciable organic matter, Tc "• may be reduced to

and adsorbed.

The recommended K value means, standard deviations, ranges and distribu-

tion parameters for technetium by aoil type, based on Table 27, are given in

Table 28.

TABLE 28

SoilType

Sand

Silt

Organic

(mLy

29.39

1.426

118.4

S.D.

100.1

3.869

192.0

FOR

n

15

8

3

TECHNETIUM

1

1

K d Range(mL/g)

.0x10-3 to

.0x10-3 to

0.24 to

388

11

340

LognorraalDistribution

\i a

-1

-1

1

.148 1.565

.332 1.290

.029 1.581


TABLE 27

S i l l %Type Snnrt

S.ini 6787

87

87

53954077

'.9

59

59

59

4587

I

Silt

9

9

9

9

353

38114

4

4

4

44

9

day

4

4

4

4

122

221237

37

37

37

114

coarse <wndSilt 45

16

399

3727

8

Organic

44

52806457334360

1132172734303032

charcoal

fen

zOrganic

0.100.10

0.10

1.10

3.01.22.81.8

-

-

-

0.140.10

-0.148.32.35.4

11.07.32.43.1-

3.0 23.3

3phagrui peat 92

•C-COj

0.070.07

0.07

0.07

----

<0.2

<0.2

<0.2

<0.2

_

-8.21.4--------

-

4.9

* * •

Sflt'irated Raste fV) (r

fl.238.2 ortdizeii

10.1 reduzed

10.1 reduced

5.45.76.08.15.1

5.1

5.1

5.1

8.88.2

8.4 (inter)

s.n7.65.57.77.77.85.96.6

6.3 - 6.6

4.5

3.8 < o t e r )

VALUES FOR THHNnTLM

CF.C

rqAOO

5.05.0

5.0

5.0

15.23.2

20.411.7

2.5

2.5

2.5

2.5

_

-1.2

12.027.011.316.936.443.519.326.8

-

46

64.7

I Freeg) Iron Orides

--

-

1.10.60.70.2-

-

-

-

_

-1382 (yg/g)

-0.41.40.10.50.30.91.2-

0.55

1050 (t^/g)

: LITERATURE SURVEY SU+Blft

CocpetlngCation

see ref.

Na3 CitrateCit/Tc tblarRatio - 0N*3 Citrate

Cit/Tc * l a r

Ritlo - 0Sa3 Citratea t / I t MjlarRatio- 1:1

----

0.0O2 iml/L

0.008 iml/t

0.020 IIDI/L

0.200 DDl/L

.JaHCOj

-

see ref .

see ref.-------

K>Cl brine

0.01 or 0.05m l A CaQjsee ref.

Kd(nt/g

0.07 i 0.320.32 (5xlCT9 mol/LTc)

52 (5x10-9 ml/L

Tc)

388 (5xlCT9 m>l/LTO

O.L550.0510.0780.00040.019 1 0.06

-O.052 i 0.01*

-0^)33 1 0.01«

4OJJ10 t 0M

0.040.030.O94-2.77 tO.23«0.0280.0680.1180.U80.0760.0110.000340

0.24

15.0


Sediment B (solution 1)Itenford soil

Hmford soil

Hanford soil

Aqulc Fragiochrept (AJ-AJ)Alf lc UdlpsaniHit (B)Aqutc * P : U ± J 1 1 (Ap)Aqulc Haploboroll (Ap)South Carolina subsoil

Scuth Carolina stfrcU

South Carolina sUnoll

Scuth Carolina sufceoU

ixlsaturated columuns?turated coLmnsandSediment A (solution 1)Cunulic HaplaqinllTyplc Eutroboralf (Aj)Aertc CaldaquoU (Aj)Omillc ifapLjqioll (Ap)Typlc ibplaquoU (Al)Aqulc Ibpluloll (Al)Udlc Ibplohoroll (Ap)activated "Mxhar"

fen soil, Enraen (Netherlands)

sphagnun peat

Reference

Seme et a l . , 1978Franz et a l . , 1982

Franz et a l . , 1982

Franz et a l . , 1982

Balogh i. Crigal, 1980Balogh S Grlgal, 1980Jfelogh S Origal, 1980Balogh I Crigal, 1980Rcutaon et s i . , 1977

ftxitson et a l . , 1977

Routson et a l . , 1977

Routson et al., 1977

Gee I Caopbell, 1980Gee S Campbell, 1980Sheppard et a l . , 1983Seme et a l . , 1978ialogh & Crtgal, 1980Balogh 4 Crigal, 1980Balogh 4 Crigal, 1980Balogh 4 Crtgal, 1980Balogh 4 Gr'gal, 1980Balogh 4 Grtgal, 1980Balogh 4 Crigal, I960Norak, 1981

rbusny 4 tyttenaere.1981Sheppard et a l . , 1983

.6-•vl

* ?iegatlvQ values will fae considered as a zero value.

- 48 -

Eaes and Sharp (1981) suggested a mean value of -1.5 for the

log10K for technetium, with a corresponding standard deviation of 0.5 (see

Table 1). Mousny and Myttenaere (1981) investigated the effect of tempera-

ture on the soil adsorption of technetium and reported that, for seven soils

investigated (including a podzol soil and a fen soil), K, ranged from 0.007

to 0.234 mL/g. Baes and Sharp (1981) suggested the K range is 0.003 to

0.28 mL/g (see Table 1). Wildung et al. (1974) selected 22 surface soils

with the following range of properties:

CEC(meq/100

5.5-90.0

g)

3

PH

.6-8.9

Carbonate

0-6.5

OrganicCarbon

0.23-28.8 14

Sand- %

.1-73.1 17

Silt

.6-58.0 3

Clay

.8-46.6

and suggested that the K, for technetium ranges from 0.007 to 2.8 mL/g.a

Thay also suggested a prediction equation of the form

Kd = 0.08 X3 - 0.09 X4 (7)

where X. is the organic carbon content,

X, is the pH.4

Vandergraaf (1982) recommended a K, range for technetium of 0 to 80 mL/g ford

granites.

Technetium References

Baes III, C.F. and R.D. Sharp, 1981. Predicting radionuclide leaching fromroot zone soil for asse. lent applications. Oak Ridge National Labora-tory Report, CONF-810606-44.

Balogh, J.C. and D.F. Grigal. 1980. Soil chromatographic movement of 93Tcthrough selected Minnesota soils. Soil Science 130, 278-282.

Franz, J.A., L.Y. Martin and D.J. Wiggins. 1982. Behavior of reduced 99Tcand y9Tc organic complexes on Hanford soil. Pacific Northwest Labora-tory Report, PNL-4178, UC-70.

- 49 -

Gee, G.W. and A.C. Campbell. 1980. Monitoring and physical characteriza-tion of unsaturated zone transport - Laboratory analysis. PacificNorthwest Laboratory Report, PNL-3304•


Mousny, J.M. and C. Myttenaere. 1981. Absorption of technetium by plantsin relation to soil type, contamination level and time. Plant and Soil6l_, 403-412.

Nowak, E.J- 1981. Composite backfill materials for radioactive waste iso-lation by deep burial in salt. Scientific Basis Nuclear Waste Manage-ment 3_, 545-552.

Paquette, J., J.A.K. Reid and E.L.J. Rosinger. 1980. Review of technetiumbehavior in relation to nuclear waste disposal. Atomic Energy ofCanada Limited Report, TR-25*.

Routson, R.C, G. Jansen and A.V. Robinson. 1977. 2l4lAm, 237Np, and 99Tcsorption on two United States subsoils from differing weathering inten-sity areas. Health Phys. 3_3_, 311-317.

Serne, R.J., D. Rai and S.J- Phillips. 1978. Monitoring and physical char-acterization of unsaturated zone transport: Laboratory analysis. In:Nuclear Waste Management Quarterly Progress Report 1977 Oct.-Dec,Pacific Northwest Laboratory Report, PNL-2377-4, UC-70.

Sheppard, M.I., T.T. Vandergraaf, D.H. Thibault and J.A.K. Reid. 1983.Technetium and uranium: Sorption by and plant uptake from peat andsand. Health Phys. 44_, 635-643.

Turcotte, M.S. 1982. Environmental behavior of technetium-99. E.I. duPont de Nemours & Co., Savannah River Plant and Laboratory Report,DP-1644, UC-11.


Wildung, R.E., R.C. Routson, R.J. Serne and T.R. Garland. 1974. Pertech-netate, iodide, and methyl iodide retention by surface soils. BattellePacific Northwest Laboratories Report, BNWL-SA-5195.

4.13 TIN

Gerritse et al. (1982) suggested that the K, value for tin ranges

from 1 x 102 to 1 x 106 mL/g. We recommend that the K. distribution infor-d

mation for lead be used for tin.


- 50 -

Tin Reference

Gerritse, R.G., R. Vriesema, J.W. Dalenberg and H.P. De Roos. 1982. Effectof sewage sludge on trace element mobility in soils. J. Environ. Qual.11, 359-364.

4.14 ZIRCONIUM AND NIOBIUM

Rhodes (1957) reported K, values ranging from 90 mL/g (pH = 6.0)

to > 1980 mL/g (pH = 2.7, 3.5, 4.4, 8.4 and 9.3) for zirconium-niobium ad-

sorption on Hanford subsoil. From this information, in the pH range of most

interest for surface soil (pH = 5 to 8, a sandy soil), zirconium has an

average K of 164 mL/g. This appears to agree well with the K, for niobiuma d

of 210 tnL/g recommended for granite (Vandergraaf, 1982). Vandergraaf also

recommended a K range for zirconium of 1000 to 6000 mL/g for granite.

Allard et al. (1977) reported a K range for zirconium of 50 to 1000 mL/g

for clay/mud and 1250 to 6300 mL/g for granite.

Based on this information, the recommended mean of the lognormal

distribution for zirconium and niobium is 2.5 with a standard deviation of

1.0. Because information is insufficient to break it down by soil type, one

value is recommended for all soil types.

Zirconium and Niobium References

Allard, B., H. Kipatsi and J. Rydberg. 1977. Sorptlon of long-li ed radio-nuclides in clay and rock. Part 1. Determination of DistributionCoefficients. KBS Technical Report 55.

Rhodes, D.W. 1957. The effect of pH on the uptake of radioactive isotopesfrom solution by a soil. Soil Sc. Am. Proc. 1_, 389.



- 51 -

5. DISTRIBUTION COEFFICIENTS FOR OTHER NUCLIDES

5.1 ANTIMONY

No specific soil K, information was found for antimony. The K

values for lead are recommended for antimony, because of its proximity to

lead in the Periodic Table.

5.2 BORON

Little information was found on boron adsorption on soils; how-

ever, there is some indication that adsorption is influenced by soil texture

and the presence of soluble salts and exchangeable cations (Gupta, 1980).

Boron adsorption information reported by Keren and O'Connor (1982) for mont-

morillonite and illite indicated that the K, value for boron for these pure

clays covld be as high as 20 mL/g. That work suggested that the K value

for soils may be in the range 0 to 10 mL/g. We recommend a value of 1 mL/g

for assessment purposes; the lognormal distribution parameter values cannot

be given.

Boron References

Gupta, I.C. 1980. Equilibrium adsorption of boron as affected by texturetsalinity and alkalinity of soil. Ann. Arid Zone _L9_, 243-248.

Keren, R. and G.A. O'Connor. 1982. Effect of exchangeable ions and ionicstrength on boron adsorption by aiontmorillonite and illite. Clays ClayMiner. 30, 341-346.

5.3 CADMIUM

Most of the work carried out with cadmium has been in response to

environmental concerns about the application of sewage sludge to agricultur-

al land. The sorption of cadmium on soils and sediments has been studied by

Poelstra et al. (1979), Rendell et al. (1980), Hendrickson and Corey (1981),

and Gerritse et al. (1982). The recommended K, value means, standard devia-

tions, ranges and distribution parameters for cadmium, based on Table 29,

are given In Table 30.

SoilType

Sand

SUt

ClayOrganic

I X XSand Silt day

sandy soil

sandy soil

sandy soil 0

sandy Mil 20

fine sand<74 m<74 m<74 yu

day soil 23organicpeat soU

sphagmiD peatsphagrun peat

plantation mjck

ZOrganic

-

-

3.5

2.5

1.40.721.81.56

16.39590

>90

>90

--

47

Z PH*CaX3 Saturated Paste

6.5

6.5

4.5 - 5.0

7.5 - 8.0

8.28.46.05.8

trace 7.45.2

5.1 (1U))4 . 5 ^

4 to5

6.2

4 to 54 to 5

7.2

K. VALUES FOR CADMIUM : LHHiAIURE SURVEY SUHARY .

Ev CEC I Free(V) (neq/100 g) Iron CWdea

31.6

31.6

- 22

- 16

- 1160 1.0725 1.0724 8.29

_33.8

_ -

- 34

CoipetlngCation

-

-

Ica«T0-0.015 train.

0-0.015 vein.-------

(a»i-0-0.015 mol/L[ C a » l -0-0.015 oo lA[ C a » l -0-0.015 nol/L

-0.025 HECaw/aL sol.

(nL7g)

66.7*

47.6*

2.62xlO2

5-OxlO2

72769.816625*23370*1.44xlO3

9.OilO3

5.7fctlO3

1.7riO>3x10'

341

SoU Locationor Description

Sandy soil (Braunschselg)0-20 cmSandy 8011 (Braunschuelg)30-40 cmSoU C

SoU D

n.11^4.1. f (jy. sandInpertal (California)Ollvcnhain (California)Bocoer (California)(Valburg) 0 - » csorganic(Schxnebeek)SoU A

Peat A

SoU B

PeatPeat

average of 3 layers

Reference

Poelstraet a l . , 1979

Poelstraet a l . , 1979


Gerrltaeet a l . , 1982

Vbnget a l . , 1983Carcla-Wragaya, 1980Garcla-Wragaya, 1960Gareia-ttlragaya, 19B0PDelstra et a l . , 1979Gsrda-MlragaTB, 1980Poelstraet a l . , 1979Gerritse et a l . , 1982

Gerrlue et a l . , 1982

Gerritse et a l . , 1982

tblf et a l . , 1977Ifclf et a l . , 1977

Ubnget a l . , 1983

rO

I

1 ueck equilibration

- 53 -

TABLE 30

K3 FOR CADMIUM—d -

Soil KJ S.D. n KJ Range LognormalType (mL/g) (mL/g) Distribution

\i a

SandSiltOrganic

189.733.934246

194.136.566110

538

47.69.8

23

tototo

50076

1.7x10 *•

21

2

.095

.359

.880

001

.4397

.4645

.090

Hendrickson and Corey (1981) reported K data from several

authors, and their plot indicated that the K, range is 0 to 6 mL/g and isd

significantly dependent on both the cadmium and calcium contents of thesoil. Navrot et al. (1978) reported K, values for cadmium for five Israeli

d

soils ranging from 1 x 103 to 1 x 10 ** mL/g, and the K value was correlated

to specific soil surface area.

Cadmium References

Garcia-Miragaya, J. 1980. Specific sorption of trace amounts of cadmium bysoils. Commun. Soil Sci. Plant Anal. _11 , 1157-1166.

Gerritse, R.G., R. Vrlesema, J.W. Dalenberg and H.P. De Roos. 1982. Effectof sewage sludge on trace element mobility in soils. J. Environ. Qual.11 , 359-364.

Hendrickson, L.L. and R.B. Corey. 1981. Effect of equilibrium metal con-centrations on apparent selectivity coefficients of soil complexes.Soil Science 1_31_, 163-171.

Navrot, J., A. Singer and A. Banin. 1978. Adsorption of cadmium and itsexchange characteristics in some Israeli soils. J. Soil Sci. 29,505-511.

Poelstra, P., M.J. Frissel and N. El-Bassam. 1979. Transport and accumula-tion of Cd ions In soils and plants. Z. Pflanzenernaehr. Bodenkd.142, 848-864.

Rendell, D.S., G.E. Batley and A.J. Cameron. 1980. Adsorption as a controlof metal concentrations in sediment extracts. Environ. Sci. Technol.14, 314-318.

- 54 -

Wolf, A., K. Bunzl, F. Dietl and W.F. Schmidt. 1977. Effect of calciumions on the absorption of lead (2+), copper (2+), cadmium (2+) and zinc(2+) by humic substances. Chemosphere 6_, 207-213.

Wong, K.V., S. Sengupta, D. Dasgupta, E.L. Daly, Jr., N. Nemerow and H.P.Gerrish. 1983. Heavy metal migration in soil-leachate systems. Bio-cycle 24, 30-33.

5.4 TELLURIUM

Allard et al. (1977) suggested that the K value for tellurium for

clay/mud and granite is 1 mL/g. This work suggests that the K range may be

0 to 1 mL/g. We recommend a K, value of 0 mL/g for assessment purposes; no

distribution parameter values can be given.

Tellurium Reference

Allard, B., H. Kipatsi and J. Rydberg. 1977. Adsorption of long-livedradionuclides in clay and bedrock. Part 1. Determination of distribu-tion coefficients. KBS Technical Report 55.

5.5 ZINC

Gerritse et al. (1982) suggested that the K, values for both zinca

and cadmium range from 1 x 103 to 1 x 10 "* mL/g, and their data for sandy and

organic soils show that the two elements exhibit very similar sorption be-

haviour. The recommended K, value means, standard deviations, ranges and

distribution parameters for zinc, based on Table 31, are given in Table 32.

SoilType

Sand

Silt

Organic

(mL/g)

622.0

51.8

4092

S.D.

911.6

68.17

4909

TABLE

K FOR

n

5

2

6

32ZINC

K^ Range(mL/g)

0.1 to 2120

3.6 to 100

70 to 1.3x104

1

1

3

LognormalDistribution\i a

.762 1.694

.278 1.021

.185 0.83

IABLE31

K. VALUES P3i ZDC ; UTEBAUJKE SURVEY SUMUg

Soi l % X S 7. Z pH* & (EC Z Free CountingType Sard Silt Clay Organic CaCD3 Saturated Paste (V) (raeq/100 g) Iron Oxides Cation (ni.7g)

Soil Uicatlonor Description

Sard

Silt

Organic

sandy soli

sandy soil

flrv sandsi l t lofnsi l t loanorganic

organic

orgpnlc

sphagrvQ peatsphagrun peat

3.5

2.5

1.4

90

m

>9O

:

4.5 - 5.0

7.5 - 8.0

4.86.28.25.07.44.5

4 - 5

6.2

4 - 54 - 5

22

16

11

7.2

7.0xl0l Soil C Gerrltse et a l . , 19820-0.015 ml/I .

[G>2+1-0-0.015 rol/L

0.1 nnlfl. CaClj0.1 rol/L CaCl2

-0.1 rol/L CaCl20.1 rol/L CaCLj(Ca2*] •0-0.015 aol/L

[Ca2*] -0-0.015 irol/L

fCa2*] •0-0.015 ml/L

-0.025 neqCa2+/nL sol.

2.12X1O3

0.1508703.61001.89idO3

6.3T1O3

2^8xl03

UulO"7.CW01

Soli D

Horlda 1Florida 2Kallandale fine sandMissouri 23Missouri 24Soil A

Peat A

SoU B

PeatPeat


Graham, 1973Graham, 1973Ubnget a l . , 1973GrahD, 1973Graham, 1973Cerrltae ec a l . , 1982


Gerrltse ec a l . , 1982

Hjlf et a l . , 1977Vblf et a l . , 1977

Plantation suck (averageof 3 layers)

Vot% et a l . , 1983

I

- 56 -

Zinc References

Gerritse, R.G., R. Vriesema, J.W. Dalenberg and H.P. De Roos. 1982. Effectof sewage sludge on trace element mobility in soils. J. Environ. Qual.U^, 359-364.

Graham, E.R. 1973. Selective distribution and labile pools of micronutri-ent elements as factors affecting plant uptake. Soil Sci. Soc. Amer.Proc. 21, 70-74.

Wolf, A., K. Bunzl, F. Dietl and W.F. Schmidt. 1977. Effect of calciumions on the absorption of lead (2+), copper (2+), cadmium (2+) and zinc(2+) by humic substances. Chemosphere 6_, 207-213.


5. CONCLUSIONS

The paucity of K, values for organic soil is the most striking

observation from our review of the literature. Plutonium, lead, technetium,

cadmium and zinc were the only nuclides for which more than two K, valuesd

have been determined for an organic soil (see Table 33). The next most

important observation is that very little work has been done with mineral

soils for some of the more mobile nuclides with K, values up to 100 mL/g,

such as uranium, technetium, molybdenum, iodine, selenium, carbon, boron,

and tellurium. There may be good reasons why more K, work is not warranted

for these nuclides in the Canadian waste management program, such as the

formation of precipitates or reduction to an immobile species in the vault

or geosphere. Our major recommendation is that effort be directed towards

the chemistry (including parameter determination, i.e., K, determinations)

of organic soils, and in particular the reactions of uranium, technetium,

iodine, selenium and carbon with organic soils. In spite of the limited

data base, it is possible to select reasonable K distribution parameter

values for most nuclides for long-term waste management assessment

purposes.

- 57 -

AVAILABILITY

Nuclide

ActiniumAmericiumAntimonyBismuthBoronCadmiumCalciumCarbonCesiumIodineLeadMolybdenumNeptuniumNickelPalladiumPlutoniumPoloniumProtactiniumRadiumRare EarthsSeleniumSilverStrontiumTechnetiumTelluriumThoriumTinUraniumZincZirconium & Niobium

X denotes 2 or fewer KJ

TABLE

OF Kd DATA FOR

Sand

X

X

X

XX

X

XX

X

XXX

XXXX

X

, values.

33

EACH NUCLIDE

Soil

Silt

X

X

X

XX

XX

XX

X

XXX

XXXXXX

BY SOIL TYPE

Type

Clay

X

XXXXXX

XX

XX

XX

XXX

XXXX

XX

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REFERENCES

Abd-Elfattah, A. and K. Wada. 1981. Adsorption of lead, copper, zinc,cobalt and cadmium by soils that differ in cation-exchange materials.J. Soil Sci. 32_, 271-283.

Allard, B., H. Kipatsi and J. Rydberg. 1977. Sorption of long-lived radio-nuelides in clay and rock. Part 1. Determination of DistributionCoefficients. KBS Technical Report 55.

Allard, B., B. Torstenfelt and K. Andersson. 1981. Sorption behaviour of1 xl in groundwater/rock and in groundwater/concrete environments.Report Prav 4.27.

Aleksakhin, R.M. 1965. Radioactive contamination of soils and plants.USAEC Report AEC-tr-6631-

Ames, L-L. and D. Rai. 1978. Radionuclide interactions with soil and rockmedia, Volume 1. U.S. Environmental Protection Agency Report, EPA520/6-78-007.

Arnold, E.M., G.W. Gee and R.W. Nelson. 1982. Proceedings of the Symposiumon Unsaturated Flow and Transport Modeling. Pacific Northwest Labora-tory Report, NUREG/CP-0030, PNL-SA-10325.

Baes III, C.F. and R.D. Sharp. 1981. Predicting radionuclide leaching fromroot zone soil for assessment applications. Trans. Am. Nucl. Soc. 38,111-112.

Balogh, J.C. and D.F. Grigal. 1980. Soil chromatographic movement of 9%cthrough selected Minnesota soils. Soil Sci. 130, 278-282.

Beals, D. 1984. Soil and climate parameters for post-closure biosphereassessment of nuclear fuel waste disposal. Atomic Energy of CanadaLimited Technical Record, TR-285*.

Bondietti, E.A. and S.A. Reynolds. 1976. Field and laboratory observationson plutonium oxidation states, _Tn: Proceedings of the Actinide-Sedi-ment Reactions Working meeting at Seattle, Washington, February 10-11,1976, Battelle Pacific Northwest Laboratories Report, BNWL-2117,pp. 505-537.

Bondietti, E.A. S.A. Reynolds and M.H. Shanks. 1975. Interaction of pluto-nium with complexing substances in soils and natural waters. In:Transuranium Nuclides in the Environment. International Atomic EnergyAgency Report, IAEA-SM-199/51, pp. 273-287.

Borovec, Z. 1981. The adsorption of uranyl species by fine clay. Chera.Geol. J32_, 45-48.

Boulton, J. 1978. Management of radioactive fuel wastes: The Canadiandisposal program. Atomic Energy of Canada Limited Report, AECL-6314.

- 59 -

Cochran, J.K. and S. Krishnaswami. 1980. Radium, thorium, uranium and210Pb in deep-sea sediments and sediment pore waters from the northequatorial Pacific. Amer. J. Sci. 280, 849-889.

Duguid, J.D. and M. Reeves. 1976. Material transport in porous media: afinite-element Galerkin model. Oak Ridge National Laboratory Report,ORNL-4928.

Elprince, A.M., C.I. Rich and D.C. Martens. 1977. Effect of temperatureand hydroxy aluminum interlayers on the adsorption of trace radioactivecesium by sediments near water-cooled nuclear reactors. Water Resour.Res. 3_, 375-380.

Elsokkary, I.H. 1980. Selenium distribution chemical fractionation andadsorption in some Egyptian alluvial and lacustrine soils. Z. Pflan-zenernaehr. Bodenkd., 143, 74-83.

Erickson, K.L. 1980. Radlonuclide sorption studies on abyssal red clays.In; Scientific Basis of Nuclear Waste Management Vol. 2. Plenum Press,ed. C.J.M. Northrup.

Franz, J.A., L.Y.. Martin and D.J. Wiggins. 1982. Behavior of reduced 99Tcand 99Tc organic complexes on Hanford soil. Pacific Northwest Labora-tory Report, PNL-4178, UC-70.

Fowler, S.W. and S.R. Aston. 1982. Application of 23iNp in experimentalaquatic radioecology: Preliminary observations on neptunium behaviorin sea water, sediments and zooplankton. Health Phys. 42_, 515- 520.

Friedman, A.M. 1976. Actinides in the Environment. ACS Symposium Series35, American Chemical Society, Washington, D.C.

Frost, R.R. and R.A. Griffin. 1977. Effect of pH on adsorption of arsenicand selenium from landfill leachate by clay minerals. Soil Sci. Soc.Amer. J. 4^, 53-57.

Garcia-Miragaya, J. 1980. Specific sorption of trace amounts of cadmium bysoils. Commun. Soil Sci. Plant Anal. _11_, 1157-1166.

Gee, G.W. and A.C. Campbell. 1980. Monitoring and physical characteriza-tion of unsaturated zone transport - Laboratory analysis. PacificNorthwest Laboratory Report, PNL-3304.

Gerritse, R.G., R. Vriesema, J.W. Dalenberg and H.P. De Roos. 1982. Effectof sewage sludge on trace element mobility in soils. J. Environ. Qual.1_1_, 359-364.

Gillham, R.W. and J.A. Cherry. 1979. Contaminant migration in noninduratedgeological deposits. _Iii_: Trends in Hydrogeology, Memoir Proceedings,Volume of the Geological Society of America.

- 60 -

Gillham, R.W., L.E. Lindsay, W.D. Reynolds, T.J. Kewen, J.A. Cherry andM.R. Reddy. 1981a. Studies of cesium and strontium migration in un-consolidated Canadian geological materials. Atomic Energy ControlBoard Report, INFO-0049.

Gillham, R.W., H.D. Sharma, M.R. Reddy, E.L. Cooper and J.A. Cherry. 1981b.Barium and radium migration in unconsolidated Canadian geological mate-rials. Atomic Energy Control Board Report, INFO-0048.

Glover, P.A., F.J. Miner and W.L. Polzer. 1976. Plutonium and americiumbehaviour in the soil/water environment. I. Sorption of plutonium andamericium by soils. Ln: Proceedings of the Actinide-Sediraent Reac-tions Working Meeting at Seattle, Washington on 1976 Feb. 10-11. Bat-telle Pacific Northwest Laboratories Report, BNWL-2117, pp. 225-254.

Graham, E.R. 1973. Selective distribution and labile pools of micronutri-ent elements as factors affecting plant uptake. Soil Sci. Soc. Amer.Proc. _3_7_» 70-74.

Graham, E.R. and C.G. Silva. 1979. Labile pools and distribution coeffi-cients for soil calcium, magnesium, and potassium determined with ex-change equilibria and radioisotopes. Soil Sci. 128, 17-22.

Gupta, I.C. 1980. Equilibrium adsorption of boron as affected by texture,salinity and alkalinity of soil. Ann. Arid Zone Jjj_, 243-248.

Hajek, B.F. and L.L. Ames, Jr. 1968. Strontium and cesium equilibriumdistribution coefficients: Batch and column determinations.BNWL-481-3.

Hamstra, J. and B. Verkerk. 1977. Review of Netherlands program for geo-logic disposal of radioactive waste. In; Nuclear Power and its FuelCycle. International Atomic Energy Agency Report, IAEA-CN-36/289.

Hansen, W.R. 1970. Polonium-210 in soils and plants. Special Report onU.S. Atomic Energy Commission Contract No. AT(11-1)-1733, COO-1733-11.

Hansen, W.R. and R.L. Watters. 1971. Unsupported 210pO02 in soil: Soiladsorption and characterization of soil solution species. Soil Sci.112, 145:155.

Harmsen, K. and F.A.M. de Haan. 1980. Occurrence and behaviour of uraniumand thorium in soil and water. Neth. J. Agric. Sci. 8_, 40-62.

Hendrickson, L.L. and R.B. Corey. 1981. Effect of equilibrium metal con-centrations on apparent selectivity coefficients of soil complexes.Soil Science l^i, 163-171.

Jenson, B.S. 1980. The geochemistry of radionuclides with long half-lives.Riso National Laboratory Report, RSO-R-430.


- 61 -

Juo, A.S.R. and S.A. Barber. 1970. The retention of strontium by soils asinfluenced by pH, organic matter and saturation cations. Soil Sci.109, 143-148.

Keren, R. and G.A. O'Connor. 1982. Effect of exchangeable ions and ionic

strength on boron adsorption by montmorillonite and illite. Clays ClayMiner. 30_» 341-346.

Mayer, S.W. and E.R. Tompkins. 1947. Ion exchange as a separation method:IV. A theoretical analysis of the column separation process. J. Amer.Chem. Soc. 69_, 2866-2874.

Mehta, K. 19<J . Nuclide inventory for nuclear fuel waste management:Post-closure phase. Atomic Energy of Canada Limited Report,AECL-6830.

Miller, C.W. 1983. Toward a comprehensive model of chemical transport inporous media. Lawrence Berkeley Laboratory Report, LBL-14604 Rev.

Mousny, J.M. and C. Myttenaere. 1981. Absorption of technetium by plantsin relation to soil type, contamination level and time. Plant and Soil61_, 403-412.

Murali, V. and L.A.G. Aylmore. 1981. A convective-dispersive-adsorptiveflow model for solute transport in soils. I Model description andsome simulations. Aust. J. Soil Res. 19_, 23-29.

Nathwani, J.S. and C.R. Phillips. 1979. Adsorption of 226Ra by soils inthe presence of calcium (2+) ions. Specific adsorption (II). Chemo-sphere 8_, 293-299.

Navrot, J., A. Singer and A. Banin. 1978. Adsorption of cadmium and itsexchange characteristics in some Israeli soils. J. Soil Sci. 29,505-511.

Nishita, H., A. Wallace, E.M. Romney and R.K. Schulz. 1979. Effect of soiltype on the extractability of 237Np, 239Pu, 241Am and 241*Cm as a func-tion of pH. NUREG/CR-0997 UCLA 12-1192. 32 pp.

Nowak, E.J. 1981. Composite backfill materials for radioactive waste iso-lation by deep burial in salt. Scientific Basis Nuclear WasteManagement 3_, 545- 552.

Onishi, Y., R.J. Serne, E.M. Arnold, C.E. Cowan and F.L. Thompson. 1981.Critical review: Radionuclide transport, sediment transport, and waterquality mathematical modeling; and radionuclide adsorption/desorptionmechanisms. U.S. Nuclear Regulatory Commission Report, NUREG/CR-1322,PNL-2901 RE.

Oster, C.A. 1982. Review of ground-water flow and transport models in theunsaturated zone. U.S. Nuclear Regulatory Commission Report,NUREG/CR-2917, PNL-4427.

- 62 -

Palmer, D.A., S.Y. Shiao and R.E. Meyer. 1981. Adsorption of nuclldes onmixtures of minerals. J. Inorg. Nucl. Chem. 43^ 3317-3322.

Paquette, J., J.A.K.. Reid and E.L.J. Rosinger. 1980. Review of technetiumbehavior in relation to nuclear waste disposal. Atomic Energy ofCanada Limited Report, TR-25*.

Patterson, R.J. and T. Spoel. 1981. Laboratory measurements of the stron-tium distribution coefficient K.Sr for seaquifer. Water Resour. Res. 17_, 513-520.tium distribution coefficient K,Sr for sediments from a shallow sand

Pillai, K.C. and E. Mathew. 1975. Plutonium in the aquatic environment -its behaviour, distribution and significance. In: Transuranium Nucll-des in the Environment. International Atomic Energy Agency Report,IAEA-SM-199/27.

Poelstra, P., M.J. Frissel and N. El-Bassam. 1979. Transport and accumula-tion of Cd ions in soils and plants. Z. Pflanzenernaehr. Bodenkd.142, 848-864.

Rancon, D. 1972. Practical utilization of the distribution coefficient forthe measurement of the radioactive contamination of minerals in rocks,soil and subterranean water. Cadarache Nuclear CEA Research Center,ANL-trans-931, Report-R-4274.

Rancjon, D. 1973. The behaviour in underground environments of uranium andthorium discharged by the nuclear industry. In: Environmental Behav-iour of Radionuclides Released in the Nuclear Industry. InternationalAtomic Energy Agency Report, IAEA-SM-172/55.

Rendell, D.S., G.E. Batley and A.J. Cameron. 1980. Adsorption as a controlof metal concentrations in sediment extracts. Environ. Sci. Technol.14_, 314-318.

Rhodes, D.W. 1957. The effect of pH on the uptake of radioactive isotopesfrom solution by a soil. Soil Sci. Amer. Proc. TL_, 389-392.

Rogowski, A.S. and T. Tamura. 1965. Movement of 137Cs by runoff, erosionand infiltration on the alluvial Captina silt loam. Health Phys. 11,1333-1340.

Routson, R.C. 1973. A review of studies on soil-waste relationships on theHanford Reservation from 1944 to 1S67. BNWL-1464, UC-70.

Routson, R.C., G. Jansen and A.V. Robinson. 1975. Sorption of 99Tc, 23^fpand 241Am on two subsoils from differing weathering intensity areas.Battelle Pacific Northwest Laboratories Report, BNWL-1889.

Routson, R.C., G. Jansen and A.U. Robinson. 1977. 2LtlAm, 23/Np and y9Tcsorption on two United States subsoils from differing weathering inten-sity areas. Health Phys. 3_3_, 311-317.

- 63 -


Serne, R.J., D. Rai and S.J. Phillips. 1978. Monitoring and physical char-acterization of unsaturated zone transport: Laboratory analysis. In:Nuclear Waste Management Quarterly Progress Report 1977 Oct.-Dec,Pacific Northwest Laboratory Report, PNL-2377-4, UC-70.

Sheppard, J.D., J.A. Kittrick and T.L. Hart. 1976. Determination of dis-tribution ratios and diffusion coefficients of neptunium, americium andcurium in soil-aquatic environments. Richland Operations Office Con-tract Report, RL0-2221-T-12-2.


Sheppard, M.I. 1981. SCEMR: A model for soil chemical exchange and migra-tion of radionuclides in unsaturated soil, Part 1: A user's manual.Atomic Energy of Canada Limited Technical Record, TX-175*.

Sheppard, M.I., T.T. Vandergraaf, D-H. Thibault and J.A.K. Reid. 1983.Technetiura and uranium: Sorption by and plant uptake from peat andsand. Health Phys. 4£, 635-643.

Singh, M., N. Singh and P.S. Relan. 1981. Adsorption and desorption ofselenite and selenate selenium on different soils. Soil Sci. 132,134-141.

Soldatini, G.F., R. Riccardo and R. Levi-Minzi. 1976. Lead adsorption bysoils. I. Adsorption as measured by the Langmuir and Freundlich iso-therms. Water, Air Soil Pollut. b_, 111-118.

Swanson, J.L. 1981. Effect of organic complexants on the mobility of low-level waste radionuclides In soils: Status report. Pacific NorthwestLaboratory Report, PNL-3927, UC-70.

Swedish Nuclear Fuel Supply Co. Ltd. 1983. Final storage of spent nuclearfuel. KBS-3, Volume III Barriers.

Tamura, T. 1972. Sorption phenomena significant In radioactive waste dis-posal. _Tn: Underground Waste Management and Environmental Implica-tions. Amer. Assoc. Pet. Geol. Mem. 18_, 318-330.

Turcotte, M.S. 1982. Environmental behavior of technetium-99. E.I. duPont de Nemours & Co., Savannah River Plant and Laboratory Report,DP-1644, UC-11.

Tyraochowicz, S. 1981. Sorptive properties of mineral deposits occurring inPoland. Nukleonika, 2b_, 595-599.


- 64 -

van Genuchten, M.T. 1978. Mass transport in saturated-unsaturated media:One-dimensional solutions. Water Resources Program, Dept. of CivilEngineering, Princeton University, Princeton, New Jersey, ResearchReport 78-WR-ll.

Wahlberg, J.S., J.H. Baker, R.W. Vernon and R.S. Dewar. 1965. Exchangeadsorption of strontium on clay minerals. U.S. Geol. Surv. Bull.,1140-C, U.S. Government Printing Office, Washington.

Wheeler, M.L. 1976. Moisture and solute transport in porous media. lit:Actinides in the Environnent, Friedman, A.M., ed. ACS Symposium Series35.

Wildung, M.W. and D.W. Rhodes. 1963. Removal of radioisotopes from solu-tion by earth materials from eastern Idaho. IDC-14624.

Wildung, R.E., R.C. Routson, R.J. Serne and T.R. Garland. 1974. Pertech-netate, iodide, and methyl iodide retention by surface soils. BattellePacific Northwest Laboratories Report, BNWL-SA-5195.

Wolf, A., K. Bunzl, F. Dietl and W.F. Schmidt. 1977. Effect of calciumions on the absorption of lead (2+), copper (2+), cadmium (2+), andzinc (2+) by huraic substances. Chemosphere b_, 207-213.


Wuschke, D.M., K.K. Mehta, K.W. Dormuth, T. Andres, G.R. Sherman, E.L.J.Rosinger, B.W. Goodwin, J.A.K. Reid and R.B. Lyon. 1981. Environmen-tal and safety assessment studies for nuclear fuel waste management:Post-closure assessment. Atomic Energy of Canada Limited TechnicalRecord, TR-127-3*.

Yamamoto, T., E. Yunoki, m. Yamakawa and M. Shimizu, 1973. Studies onenvironmental contamination by uranium. 3: The effects of carbonateion on uranium adsorption to and deeorption from soils. J. Radiat.Res. lk_, 219.

Yeh, G.T. and D.S. Ward. 1981. FEMWASTE: A finite-element model of wastetransport through saturated-unsaturated porous media. Oak Ridge Na-tional Laboratory Report, ORNL-5601.

Zelazny, L.W., D.C. Martens, A.M. El-Prince and C.I. Rich. 1978. Effect oftemperature and hydroxy-aluminura interlayers on cesium selectivity andfixation in river suspensions and soils. ORO-4851-2.


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