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Hindawi Publishing CorporationScience and Technology of Nuclear InstallationsVolume 2013 Article ID 932546 9 pageshttpdxdoiorg1011552013932546

Research ArticleThe Fission-Based 99Mo Production Process ROMOL-99 andIts Application to PINSTECH Islamabad

Rudolf Muenze1 Gerd Juergen Beyer1 Richard Ross2 Gerhard Wagner1 Dieter Novotny1

Erik Franke1 Mustansar Jehangir3 Shahid Pervez4 and Ahmad Mushtaq4

1 GSG International GmbH Eichenstraszlige 12 8808 Pfaffikon Switzerland2 IAF Radiookologie GmbH Karpatenstraszlige 20 01326 Dresden Germany3 Foundation University Islamabad 44000 Islamabad Pakistan4 Isotope Production Division Pakistan Institute of Nuclear Science and Technology (PINSTECH) PO Nilore Islamabad45650 Nilore Pakistan

Correspondence should be addressed to Gerd Juergen Beyer gerdbeyergsg-intcom

Received 27 June 2013 Accepted 15 August 2013

Academic Editor Pablo Cristini

Copyright copy 2013 Rudolf Muenze et alThis is an open access article distributed under the Creative Commons Attribution Licensewhich permits unrestricted use distribution and reproduction in any medium provided the original work is properly cited

An innovative process for fission based 99Mo production has been developed under Isotope Technologies Dresden (ITD) GmbH(former Hans Walischmiller GmbH (HWM) Branch Office Dresden) and its functionality has been tested and proved at thePakistan Institute of Nuclear Science and Technology (PINSTECH) Islamabad Targets made from uranium aluminum alloy cladwith aluminum were irradiated in the core of Pakistan Research Reactor-1 (PARR-1) In the mean time more than 50 batchesof fission molybdenum-99 (99Mo) have been produced meeting the international puritypharmacopoeia specifications using thisROMOL-99 processThe process is based on alkaline dissolution of the neutron irradiated targets in presence of NaNO

3 chemically

extracting the 99Mo from various fission products and purifying the product by column chromatographyThis ROMOL-99 processwill be described in some detail

1 Introduction

The present sources of molybdenum-99 (99Mo 11987912= 66 h)

are research reactors by neutron-induced fission of 235Uwhich results in high-specific activity 99Mo or using the (119899 120574)nuclear reaction with 98Mo (natural Mo or enriched 98Mo =24) resulting in low-specific activity 99Mo Generally thespecific activity of molybdenum produced by fission is morethan 1000 times higher than that obtained by (119899 120574) pro-cess The almost universal means by which technetium-99m(99mTc 119879

12= 6 h) is made available for clinical applications

is from the elution of generators containing high-specificactivity fission-based 99Mo

The first chemical process for separation of fission 99Mowas described by the Brookhaven group USA [1] In this pro-cess the target (93 enriched U-235 alloyed with Al) was dis-solved in 6M nitric acid catalyzed by mercuric nitrate In theformer Zentralinstitut fur Kernforschung (ZfK) Rossendorf

a fission-based 99Mo separation technology became opera-tionally ready in 1963 which was actually the basis of thefirst fission-based 99Mo99mTc generator in Europe Metallicnatural uranium pellets were used as target material andthe dissolution of the irradiated U-pellets was done withconcentrated HCl Quartz and glass apparatus was used inchemical processing and yield of 99Mowassim70 [2] In 1980this process was replaced by the AMOR process (AMORAnlage zur Mo Production Rossendorf) developed in thesame institute [3] The AMOR process made use of originalfuel elements of the RF-reactor as qualified target whichwas dissolved in HNO

3Hg Batch-wise adsorption at Al

2O3

and sublimation technique were used for separation andpurification of the 99Mo This process was in operation untilthe shut-down of the Rossendorf Research Reactor in 1991

Another small-scale production process for fission 99Mowas proposed by the Rossendorf group in which naturaluranium as uranium oxide was used as target material [4]This procedure was particularly interesting for those which

2 Science and Technology of Nuclear Installations

do not dispose of enriched nuclear fuel material Approxi-mately 400 g of uranium oxide enclosed in irradiation cansare dissolved in nitric acid after irradiation for 100 hrs at aneutron flux of 5 times 1013 cm2sminus1 in a research reactor Theseparation of 99Mo from the fuel-fission product solutionis performed by ion exchange with alumina in a chro-matography column Final purification includes the repeatedchromatography separation and subsequently a sublimationstage

Based on their own long-term experiences and consider-ing international achievements in 99Moproduction scientistsof the Radio-Isotope department of the former Rossendorfinstitute ZfK designed a new process for fission-based 99Moproduction named ROMOL-99 [5ndash7]The basic principles ofthis process are as follows (see also the flow scheme Figure 1)

(i) The dissolution of the UAlxAl-clad targets shall beperformed in amixture of NaOHNaNO

3without H

2

generation under reduced pressure conditions(ii) The Xe shall be trapped cryogenically after passing a

gas treatment line(iii) The NH

3generated in the dissolving process shall be

separated prior to Mo separation(iv) The radioiodine shall be separated prior to 99Mo-

separation as well(v) During dissolving process nitrite is generated which

shall be eliminated prior to the 99Mo separation

The basic parameters of this process has been developedwith modern nonradioactive analytical techniques by theIAF-Radiookologie GmbH Dresden while the active testingand optimization of the process has been carried out atPINSTECH Islamabad under supervision of the Germanscientists In this paper the chemical process of the ROMOL-99 technology will be described in some detail

2 Materials and Methods

All chemicals were purchased from E Merck (Germany) andwere of guaranteed reagent grade (GR) or analytical reagent(AR) grade Al

2O3(90 active acidic for column chromatog-

raphy 70ndash230 mesh ASTM) was used Silver-coated aluminawas freshly prepared at institute Organic anion-exchangeresin was purchased from BioRad USA

The non-radioactive development work was performedusing uranium-free Al-plates (purchased from PINSTECH)having the same composition as the material used for theoriginal targets

Tracer experiments were performed using 131I traceractivities which were taken from the PINSTECH routine131Iodine production and the 99Mo tracer was taken fromthe routine PAKGEN 99mTc generator production (99Moimported from South Africa)

21 Irradiation of Target Qualified HEUAl alloy clad withhigh purity aluminum target plates [8] were irradiated for12ndash18 h at a neutron flux of sim15 times 1014 cmminus2sminus1 inside the

Irradiated Xe-133decay

Basic dissolution NH3 H2OXeKrH-3

Filtration NH3-trappingin H2SO4

HL solidwaste

U-235Iodine removing

Xe (residues)

(residues)IL solid wastespent

Agaluminacolumns

AcidificationHNO3

Iodine(residues) Iodine gas trap

Al2O3 column ILL acid wasteHNO3

Purification 1DOWEX

IL solid wastespent column

Purification 2Evaporation

LLL basicwaste

Purification 3Sublimation

LL solid wastespent materials

dispensing

(final product)

Gastraps

UAl targets

3 M NaOH4 M NaNO3

U + FP + TU

Mo + FP

99Mo

99Mo

99Mo separation

filter cake

Figure 1 Process flow scheme of the ROMOL-99 process

core of the Pakistan Research Reactor-1 (PARR-1) After 24 hcooling the irradiated target plates were transferred to the99Molybdenum Production Facility (MPF) for separation of99Mo from the uranium actinides and fission products Forthe warm test runs targets were irradiated for short times atlower flux density but the target composition was identicalwith those for production runs The irradiation conditionswere chosen in a way that the total activity inventory for thedevelopment work was of the order of 4GBq

22 Process Control and Quality Control Gamma ray spec-troscopy high-purity Ge detector (Canberra Series 85 multi-channel analyzer) was used to determine the activity balanceduring all process steps and for the determination of radionu-clide impurities in the final 99Mo product This concernsmainly 131I and 103Ru 132Te Beta counting of 89Sr and 90Srwas done by a liquid scintillation analyzer (Tri-Carb 1900TR Packard Canberra Company) after separation by ion-exchange and precipitation with the aid of carrier Con-tamination of alpha emitters was done with the 120572-counter(UMF-200) Radiochemical purity of [99Mo] molybdatewas determined by means of paper chromatography with a

Science and Technology of Nuclear Installations 3

mixture of hydrochloric acid water ether and methanol (5 15 50 30) as mobile phase The chemical purity was occa-sionally determined after decay by optical emission spec-trometry (Optima 3300XL Perkin Elmer) It was used for thedetermination of toxic elements such as Cr Co As Sn CdPb and U the detection limits in ppm were 2 5 5 5 1 5 and2 respectively

The final 99Mo product was dispensed and assayed bymeans of a calibrated ionization chamber Radioactivity con-centration (MBqcm3) was calculated by dividing the totalproduct activity by the final volume of the product solutionAll required nuclear data were taken from NuDat 25 [9]

3 Results and Discussion

31 The Dissolving Process When dissolving the target platesin the solvent 3M NaOH4M NaNO

3 3 reactions must be

considered leading to different reaction products as follows

8Al + 3NaNO3+ 5NaOH + 2H

2O 997888rarr

8NaAlO2+ 3NH

3

(1)

Al + 15NaNO3+NaOH 997888rarr

NaAlO2+ 15NaNO

2+ 05H

2O

(2)

Al +NaOH +H2O 997888rarr NaAlO

2+ 15H

2 (3)

The most important is reaction (1) where the Al reduces thenitrate ion down to NH

3 Close to the end of the dissolving

process the nitrate is reduced only to nitrite (2) This fractionis of the order of 10 to 15 The theoretically possiblereduction (3) generating hydrogen is nearly suppressed Gaschromatographic determination of hydrogen in the off-gasfrom the dissolving process did not show any signal for H

2

meaning the upper limit for H2generation is lt2 and is

therefore without any dangerUnder the conditions that 119909 represents the mass unit of

the target matrix that undergoes to nitrite formation andconsequently (1 minus 119909) represents the mass units of the targetmatrix that undergoes under NH

3formation we obtain the

ldquomaster equationrdquo for dissolving the targets following

Al + 00085U + (03814 + 1125119909)NaNO3

+ (06271 + 0375119909)NaOH

+ (02585 minus 075119909)H2O 997888rarr

NaAlO2+ 000425Na

2U2O7

+ (1 minus 119909) 03814NH3 + 15 timesNaNO2

(4)

The value 119909 representing the fraction of the aluminum that isdissolved under nitrite formation ranges between 01 lt 119909 lt016

The solvent volume needed for the process is determinedby the solubility of the sodium aluminate (NaAlO

2) which

is 21ML corresponding to 57 gL Al Furthermore the Naconcentration should be kept as high as possible in order toreach safely the saturation concentration for the precipitate

Na2U2O7 A high nitrate concentration is needed for avoiding

the formation of hydrogen while the viscosity of the solutionshould be suitable for easy filtrationWe found a compositionof 3M NaOH4MNaNO

3as most suitable for the dissolving

processThe dissolving process is strong exothermic (close to

600 kcal are generated for dissolving 100 g Al) and in addi-tion the dissolving speed increases with the second powerof the temperature Thus the reaction is self-acceleratingFollowing the experiences collected in Dresden (IAF) andPINSTECH the control of the dissolving process is easy andsafely possible by short heating and cooling pulsesWith thesetechniques one can easily adjust the dissolving temperature ataround 70ndash80∘C Furthermore the process can be performedat slightly reduced pressure conditions (see Figure 2) Thedissolving process is performed in a special dissolving vesselequipped with heater and cooling jacket

32 NH3Distillation Since the iodine shall be removed from

the process solution using a silver-coated column materialthe NH

3is recommended to be eliminated because it has

potential to influence the efficiency of the iodine removalat the Ag-coated column The simplest way to separate theNH3is the distillation from strong basic solution Preliminary

experiments have shown that 150ndash200mL distilled volumeis sufficient This volume can be distilled off from the targetsolution within about 20minutes In the production runs thedistilled NH

3is trapped in 5N H

2SO4solution

33 Filtration The precipitate that is formed during the dis-solving process is composed ofmainly 2 components theNa-diuranate and in addition the nonsoluble hydroxides oxidesor carbonates of several alloying metals of the Al-matrixthat are coprecipitated together with the Na

2U2O7 Based

on analytical data of the Al-matrix material used for thetarget preparation the following quantities for the precipitateshould be expected (Table 1)

Assuming a density of the precipitate of 44 gcm3 (basedonsim30porosity) and the uranium in the formofNa

2U2O7times

6H2O one would obtain a precipitate volume of sim237 cm3

which corresponds to a filter bed thickness of 119889 le 15mmThe target element uranium after dissolution must be

present exclusively in the chemical form of Na2U2O7because

it is well known that uranium species of lower oxidation stageabsorb 99Mo and consequently lower the production yieldDissolving the same targets alone in NaOH or KOH (withoutNaNO

3) [10] an additional oxidation process (usually H

2O2)

is required to reach the oxidation stage of +6 for both of theU and the Mo

As shown from the crystallographic analysis the targetelement uranium was found after our ROMOL-99 dissolvingprocess straight as sodium diuranate (Na

2U2O7) in the

precipitate (Figure 3) without any further treatmentThe time needed for filtration is mainly determined by

the surface area and the porosity of the used filter plate andthe filter cake the viscosity of the solution and the filtrationpressure The filter plate consists of a 3mm thick metallic(INOX) sinter plate with a porosity of sim30 120583m The cold


0

20

40

60

80

100

0 10 20 30 40 50 60 70 80 90Time (min)

Temperature during dissolving process

Hea

ting

on

Coo

ling

on

Coo

ling

jack

et em

pty

Coo

ling

jack

et em

pty

End of dissolving

Tem

pera

ture

(∘C)

(a)

minus05

minus04

minus03

minus02

minus01

0

0 10 20 30 40 50 60 70 80 90

Pressure in the vessel during dissolving process

Time (min)

Pres

sure

(b)

(b)

Figure 2 Temperature gain during controlled dissolving process (a) and the pressure situation during the dissolving process (b)

Table 1 Composition of the target material and the related compo-sition of the precipitate after the dissolving process

Alloyingelement

Content (of Al-weight)

Content in(mg) for 3targets

Precipitatedspecies

Precipitatein (mg) for3 targets

Fe 014 1288 Fe(OH)2 20714Mn 0002 184 Mn(OH)2 303Si 001 920 SiO2 1933Ca 016 1472 CaCO3 95043C 01 92 C 9200U 516 5100 Na2U2O7 681485

and hot runs showed that first of all the precipitate can befiltrated from the target solutionwith the above given alloyingcomponents and in addition sufficient filtration speed (200ndash300mLmin) is achieved in 10ndash20min at a temperature ofaround 50∘C

34 Iodine Removal In order to minimize the risk of iodinerelease in later production steps and waste the adsorptionon silver is the most promising approach for trapping theradioiodine before the 99Mo is separated During the produc-tion process we have to deal with 132I (23 h half-life daughterof 132Te) 133I (208 h half-life) and 131I (802 d half-life)Freshly prepared silver-coated Al

2O3material has shown to

be the most appropriate material this material has beenprepared according to the Wilkinson et al method [11] Theiodine removal process is performed by controlled filtrationof the filtrated target solution over a column filled withthis material The flow rate needs to be controlled Sincethe optimal flow rate for high iodine trapping efficiencyis identical with the speed for introducing the basic targetsolution into the strong acid reaction vessel (next processstep) there is no technological separation of both steps thuswhile transferring the basic solution into the nitric acid foracidification the radioiodine is removed simultaneously Thetransfer process lasts for about 60ndash90 minutesThe efficiency

for iodine trapping has been determined to be gt98TheAg-column also traps a good fraction of the Ru (see Figure 4)99Mo could not be detected within a detection limit of 3

35 Acidification and Nitrite Destruction For the main sep-aration stepmdashthe separation of the 99Mo from the processsolution after iodine removalmdashAl

2O3column chromatog-

raphy has been selected Molybdate is adsorbed from weakHNO

3-acid media at Al

2O3(this principle is used in the

99Mo99mTc-generator technology) Thus the strong basicprocess solution needs to be acidified This is not an easystep since the Al-concentration is high An anion-exchangeprocess as it is used in cases were only NaOH or KOH isinvolved for dissolving the targets under H

2generation is

not possible due to the high NO3

minus concentration Many testexperiments have been performed in order to determine theoptimal conditions for this step When introducing strongbasic aluminate solution into strong acid HNO

3solution

in the first step Al(OH)3is precipitated This hydroxide

needs to dissolve immediately otherwise it may transmuteinto nonsoluble configurations which may create problemsin the further production steps When the basic solutionis introduced with moderate speed (50ndash70mLmin) understrongmixing one observes first a thick white precipitate thatis redissolved relatively fast Due to neutralization heat thesolution is warming up In order to bring the solution to boiladditional heating is required

As said before we also have nitrite in the system whichis recommended to be destroyed Simultaneously with theacidification process the nitrite is reduced with urea undernitrogen formation according to

(NH2)2CO + 2HNO

2997888rarr 2N

2+ CO2+ 3H2O (5)

In test experiments this gas generation looked like very finesilk This gas generation is mixing the solution only a littlebecause of the microscopic fine bubbles this effect is by farinsufficient additional strong stirring is required The com-plete nitrite destruction and the re-dissolving of the primaryprecipitated hydroxides require refluxing under stirring forone additional hour after complete solvent transfer


0

1000

2000

3000

4000

5000

6000

5 10 20 30 40 50 60 70 802120579

Lin

(cou

nts)

26-0973 (D)-Sodium Uranium Oxide-Na2U2O7-Y 5625-d x by 1-WL 178897

09-0174 (D)-Uranium Oxide-UO2-Y 5000-d x by 1-WL 178897

05-550 (D)-Uraninite syn-UO2-Y 5000-d x by 1-WL 178897

Operations Smooth 0150 | Background 0676 1000 | Import

-Company TU Dresden Geologie-Creation 031406 041223File 4781 IAF WDHRAW-Start5000∘-End 80000∘-Step 0030∘-Step time 20 s-WL1 178897

Figure 3 X-ray diffraction patterns of the uranium precipitate thatshow only the reflections of Na

2U2O7and excluded other uranium

species to be present This X-ray diffractogram was performed byTU DresdenGeologie

1E + 01

1E + 02

1E + 03

1E + 04

1E + 05

200 300 400 500 600 700 800 900 1000

Cou

nts 103Ru

131I133I

132I

Energy (keV)

Figure 4 Gamma spectrum of the Ag-coated Al2O3column after

passing the filtrated target solution The measurement was donefrom large distance Only gamma signals from iodine radionuclidesand Ru could be identified

The reaction gases of this acidification process and inaddition a slight carrier gas flow release also remain volatileiodine species (from iodine residue and decay of Te-parentnuclides) and radio Xe (mainly from 133I-decay) The radioiodine is retained in a gas adsorption trap filled with Ag-IONEX This is a Zeolite exchange material that adsorbs at119879 gt 100

∘C volatile inorganic and organic iodine species thatis widely used in fuel reprocessing process for decontamina-tion of acid off-gases After passing the IONEX filter off-gasfrom the acidification process that still may contain some Xeis introduced into the gas process line for further treatment

When the nitrogen formation and iodine release is fin-ished the solution is cooled down to room temperature andis ready for the Al

2O3column process

36 Alumina Column Process The separation of the 99Mofrom the acidified target solution is achieved via anion

0

1

2

3

4

5

6

7

8

9

10

5 10 15 20 25Volume (mL)

pH an

dd

(pH

)

Figure 5 Potentiometric titration of 1mL of the acidified targetsolution after nitrite destruction diluted to 100mL with 0100NNaOH

exchange chromatography using week acid Al2O3as column

materialThe adsorption efficiency forModependsmainly onthe salt concentration and the acidity of the solution and notso much on the absorber material itself For the optimizationof the column parameters the control of the free acidityin the FEED solution played an important role Due to thehigh salt concentration (especially that of Al3+) a direct pH-measurement is not possible A potentiometric titration didnot show the required precision (see Figure 5)

The safe and better is to dilute a sample of the solution by afactor 1 100 with distilled waterThis solution could perfectlyundergo a pHmeasurement with an ordinary glass electrodeThe pH determined in this way was always in the region of22 lt pH lt 26 which means that the free acid concentrationin the original FEED solution under practical conditions wasin the range of about 015 lt [H+] lt 07M

Under practical conditions the volume of the loadingsolution (FEED) is around 6 L (for sim100 g target material)After the loading process the column shall be washed with05ndash10 L of 05MHNO

3500mLwater and thenwith 1500mL

001M NH4OHThe 99Mo is then eluted with up to 2000mL

of 1M NH4OH solution One obtains a raw 99Mo product of

already≫99 radionuclide purityIn order to define the optimal Al

2O3column parameters

one needs to consider

(i) the adsorption capacity of the exchange materialAl2O3

(ii) the selectivity related to the separation from radioac-tive contaminations

(iii) the possible and needed loading- and elution speedwhich is relevant for the duration of the process


Table 2 Optimal parameters for the alumina column process

Al2O3 column About 50mm times 145mm bottom G 3 fritAl2O3 weak acidmaterial

250 g size sim60120583m density 125mLgporosity 0875

Loading process FEED volume sim58 L 015 lt [H+] lt 07Msim120min

(1) Wash process 1000mL 05M HNO3 time about 15min(2) Wash process 500mL water time about 7min(3) Wash process 1000mL 001M NH3 time about 15minLiquid waste volume 8300mLElution 1000mL 1-2M NH3 time about 30minAlumina columnprocess Total time about 3 h

The capacity of Al2O3for Mo adsorption is known to be

sim30mg Mog Al2O3column material In test experiments

using 50mL of model-target solutions containing a Mo-concentration of 20ndash33mgMoL and columnswith 2 g Al

2O3

column material (07 times 56 cm column dimension) using aflow rate of 7 cmmin corresponding to 27mLmin the Mocould be adsorbed with an average yield of gt90 Thus inthese experiments only a small fraction (15ndash25) of thecapacity of the exchanger has been utilizedThis correspondsto 05ndash08mgMogAl

2O3 Based on this data onewould need

for processing of 3 target plates theoretically 140 g of Al2O3

corresponding to 152mL Al2O3for the separation process

For defining the column dimensions one needs to finda compromise between the needed amount of the Al

2O3

material and reasonable high applicable elution speed Fur-thermore one has to consider losses due to irreversible boundMowith increasingAl

2O3quantities Assuming the following

practical conditions

(i) the total volume of liquids that has to pass the columnis sim11 L composed from 58 L acidified target solution33 L wash solutions and 20 L elution volume

(ii) the linear filtration speed is 7 cmmin (50mLmin forloading and eluting and 80mLmin washing)

(iii) the diameter of the column shall be 5 cm

one obtains a volume flow speed of 137mLmin under prac-tical conditions

Considering the previous determined 140 g or 152mLAl2O3absorber material one would obtain an absorber bed

height of 78 cm If one increases the dimensions by at least afactor 2 for compensating not optimal conditions the lengthof the Al

2O3column becomes 156 cm filled with 304mL

Al2O3absorber material

During the commissioning it has been demonstrated thata 250 g alumina column bed is acceptable which correspondsto a column bed volume of about 275mL Table 2 summarizesthe Al

2O3column process parameters

Using the parameters shown in Table 2 the profile foreluting the 99Mo from theAl

2O3columnhas been performed

As seen in Figure 6 the 99Mo is eluted in a relativelysharp peak and 1000mL of 10M NH

3solution is sufficient

020000400006000080000

100000120000140000160000

0 500 1000 1500 2000 2500mL of eluate

CPM

on

MCA

Figure 6 Elution profile for 99Mo elution from the Al2O3column

with 1M NH3using the parameters shown in Table 2

The 99Mo retention at the column using model solutions waspractically 100 and the 99Mo recovery was measured to be912

The Al used in the target material contains some quan-tities of Si It is well known that Si forms very unpleasantnonsolubleMo Si-species whichmay cause dramatic losses inthe 99Mo yield Certain limited quantities of Mo-carrier canhelp solving this problemThe other way around would be toelute the Al

2O3column with higher-concentrated NH

3(2M

instead of 1M) or with NaOH

37 DOWEX-1 Column Process Molybdenum in its anionicform MoO

4

2minus is adsorbed directly from the ammonia solu-tion eluted from the Al

2O3column at strong basic anion

exchange resins as DOWEX-1 (configuration OHminus) Thedistribution coefficients has been determined to be119870

119863= 270

for adsorption from 1M NH4OH and 119870

119863= 08 for the

desorption with 1M (NH4)2CO3solution

The dimensions of a suitable DOWEX-1 column andits operation parameters are determined in a similar wayas demonstrated for the Al

2O3column For a column of

about 26 times 120mm a linear flow speed of 13 cmmin is themaximum If the volume of the Mo solution is 2000mLone would need theoretically 546 g of the ion exchangeresin DOWEX-1 in the dry form Considering the density of065 gmL resin this would give an 84mL volume of the resinFor rinsing the column 4 bed volumes are required whichcorrespond to 340mL Table 3 summarizes the parametersfor the DOWEX column process The corresponding elutionprofile is shown in Figure 7

38 Evaporation Step The purification step at the DOWEXcolumn delivers 200mL of the 99Mo molybdate in 1M(NH4)2CO3solution In the following step this eluted solu-

tion is evaporated to the dryness in a special evaporatorwith condenser During evaporation the (NH

4)2CO3is being

decomposed thus no additional salts are introduced into thefinal configured [99Mo] molybdate solution

The residue is redissolved in the desired volume ofdiluted NaOH solution forming the final product solution


Table 3 Optimal parameters for the DOWEX-1 column process

DOWEX-1 column About 26mm times 120mm bottom G 3 frit

Loading process99Mo-solution in 1M NH3 volume sim10 Lsim15min

(1) Wash process 170mL water time about 3min(2) Wash process 170mL water time about 3minLiquid wastevolume

sim14 L (depending on FEED and washvolume)

Elution 200mL of 1M (NH4)2CO3 solution timeabout 10min

DOWEX columnprocess Total time about 35ndash40min

020000400006000080000

100000120000140000160000180000

0 50 100 150 200 250 300Eluted volumn (mL)

Cou

nts o

n M

CA

Figure 7 99Mo elution profile from theDOWEX-1 columnwith 1M(NH4)2CO3-solution using the parameters shown in Table 3

[99Mo]Na2MoO4 This final product solution is then trans-

ferred into a corresponding plastic vial and transferred intothe hot cell 3 for further processing precisemeasurement anddistribution

A sublimation step (at 1000∘C) is foreseen as an additionalreserve for improving purity if required In this case theresidue after evaporation shall be redissolved in dilutedHNO

3or NH

4OH

39 Radioactivity Balance during the Process Careful studieshave been performed to obtain a full picture on the behaviorof the 99Mo of the most important impurities in 99Mopreparations for other fission products and for the targetelement itself On one hand tracer activities of 99Mo and 131Ihave been used and after having optimized the separationconditions the same full protocol has been applied to studythe separations technology with weak irradiated originaltarget material (activity level sim4 GBq) Figure 8 summa-rizes gamma-spectroscopicmeasurements that illustrate howpowerful the individual separation steps are Segments oforiginal measured gamma spectra are shown in one graphSignals of the most critical radionuclides are clearly identi-fied In order to have a good overview the original data of thedifferent spectra have been expanded using a factor shown inthe graph

The upper spectrum has been taken from a small fractionof the filter cake (precipitate) followed by the spectrum froma sample from the filtrate It is clearly seen that only fewgamma lines are left in the filtrate which correspond to 99Mo

1E + 01

1E + 02

1E + 03

1E + 04

1E + 05

1E + 06

1E + 07

1E + 08

1E + 09

100 200 300 400 500 600

Cou

nts p

er ch

anne

l

99Mo239Np 140La

103Ru133I

131I

Filtrate

Energy (keV)

99Mo

99m Tc

X 1000

X 100

X 10

X 01 Final product

Precipitate

+ 01

+ 02

+ 03

+ 04

+ 05

+ 06

+ 07

+ 08

+ 09

99Mo239Np 140La

103Ru133I

131I

Filtrate

99Mo

99m Tc

X 1000

X 100

X 10

X 01 Final product

Precipitate

Feed to AL2O3

Figure 8 Gamma spectra of samples from the precipitate filtrateFEED solution (filtrate after iodine removal) from the final productillustrating the different separation and purification steps (for moredetails see text)

its daughter 99mTc the radioiodinersquos and some fractions ofRuThe strongest signals in the precipitate (239Np and 140La)are not seen in the filtrate solution As said before the filtrateis passed through a silver-coated Al

2O3column prior to

the acidification process Thus comparing the spectra 2 and3 one clearly sees that iodine is missing in the FEED solution(see also Figure 4) When interpreting spectrum 3 one needsto consider that the strongest gamma signal from 99Mo is739 keV with the branching of 1213 (not shown in thisgraph)The two gamma lines here at 181 keV and 366 keVhavea branching of only 599 and 119 respectively Finally thelast spectrum below is taken from a sample of the final 99Mopreparation All measurements have been performed using aPb absorber to suppress the strong gamma signal from 99mTc(and other low-energetic radiation)

310 Radioactivity Distribution between Precipitate and Fil-trate In total the precipitate collects more than 60 of theradioactivity formed in the nuclear process in the chemicalform of hydroxides oxides or carbonates of the fissionproducts This corresponds to the fission products of Ba andSr the rear earth elements and actinides ZrNb Te andSb are nearly quantitatively collected in the precipitate Theresults of a corresponding tracer experiment are summarized


Table 4 Radioactivity distribution between precipitate and filtrateafter dissolving irradiated natU-targets of original composition

Nuclide Precipitate () Solution ()239Np 100 ≪1132Te 100 lt3143Ce 100 ≪1141Ce 100 ≪1140Ba 100 ≪1140La 100 ≪1131I 060 9939103Ru 20ndash40 60ndash8099Mo 057 9943Note Ru behaves in different experiments differently thus these data providejust an estimate

Table 5 Radioactivity distribution of 99Mo and themost importantimpurities during the process

99Mo 103Ru 132Te 131IFilter cake lt05 1920 9630 ndFiltrate gt995 8070 370 100Ag-column nd 2270 100 gt98FEED gt99 6690 160 lt2Al2O3 column 106 010 110 ndAl-waste nd 7540 nd ndDOWEX column 0003 006 nd ndFinal 865 lt0001 lt0001 lt0001The values relates to the individual content of the specified nuclide and notto 99Mo(nd not detected)

in Table 4 In this experiments target plates of the originalcomposition were used

The most important impurities have been followed upquantitatively throughout the process as good as gamma-spectroscopy could do under practical conditions with lim-ited measuring time The results are summarized in Table 5The FEED solution (filtrate after passing the silver column)contains already relatively clean 99Mo however in presenceof high salt concentration (Al Na including 24Na and fission-Cs) Up to 80 of the Ru is found in the filtrate at thesilver column already about 22 are retainedThe remainingRu is passing the Alumina column during the loadingprocedure Careful washing avoids the transfer of Ru to thenext purification steps Ru shows a nonstandard behaviorsometimeswe observed significant higher Ru-retention in thefilter cake

The 132Te is nearly quantitatively coprecipitated Thehighest 132Te-content in the filtrate was 37 of the originalquantity About half of this fraction is retained at the silvercolumn the other half fraction at the Alumina column Inthe filtrate and wash solutions from the Alumina columnthe 132Te could not be detected any more (with the appliedspectrometric parameters)

The iodine is nearly quantitatively retained at the silvercolumn The small fraction that is passing the silver column

Table 6 Quality parameters of fission 99Mo produced at PIN-STECH meeting international standard

Gamma131I le5 times 10minus2 MBqGBq 99Mo

103Ru le5 times 10minus2 MBqGBq 99Mo

Beta89Sr le6 times 10minus4 MBqGBq 99Mo90Sr le6 times 10minus5 MBqGBq 99Mo

Alpha le1 times 10minus6 MBqGBq 99MoOther gamma le1 times 10minus1 MBqGBq 99Mo

is then distributed throughout the systemmainly in thewastesolutions through the washing procedures of the columnsSummarizing the separation and purification process isefficient and easy

311 99Mo Production Facility at PINSTECH The 99Mo Pro-duction Facility (MPF) is installed at PINSTECH Phase-1building near reactor hall of PARR-1The technical realizationof the ROMOL-99 process in a semiautomated separationfacility has been carried out by ITD Dresden GmbH (formerHans Walischmiller (HWM) GmbH Branch office Dres-den) The main working areas of this facility are the HotCell complex (3 Hot Cells) interim liquid storage tankscharcoal filter beds for iodine retention xenon delay tanksand the operator and service areas interconnected with itAdditionally there are the so-called lock rooms throughwhich the activated targets the final product and solid andliquid wastes are moved Still there are areas for personnelpreparation of reagents storage dosimetry measurementand decontamination Further equipment in other rooms orbuildings which participate in the 99Mo production is theexisting equipment of the main exhaust system with filterchamber Secomak blowers and themain exhaust blowerThespent target material (loaded filter plates enclosed in screwshut cans) is stored in Spent Fuel bay of PARR-1 The solidlow-radioactive wastes (spent ion-exchange columns tubesinterconnections and other one-way materials) are storedwhile decayed radioactive liquid waste is cementized in theradioactive waste management Group building

More than 50 commercial batches of fission based 99Mousing ROMOL-99 process have been successfully completedAfter the evaporation step the residue is dissolved in thedesired volume of diluted NaOH solution forming the finalproduct solution [99Mo]Na

2MoO4 This final product solu-

tion is then transferred to the PAKGEN 99mTc generatorproduction site at PINSTECH These generators are thendistributed to the 35 nuclear medical centers in PakistanThe performance of these generators is comparable tothat of generators produced from imported fission 99MoThe quality of the 99Mopreparations produced at PINSTECHcorresponds to the required international standard (Table 6)Details about the preparation of PAKGEN 99mTc generatorsand their quality control have already been reported [12]The next steps at PINSTECH related to the routine 99Mo-production are upscaling the production capacity and trans-mutation to LEU (low enriched uranium) as target fuel


4 Conclusion

The ROMOL-99 process allows dissolving UAlxAl claddispersion targets under reduced pressure conditionswithoutgeneration of hydrogen at temperatures between 70 and 80∘CThe technology implements the separation ofNH

3and radio-

iodine prior to the 99Mo separation Generated nitrite issafely destroyed during the acidification process by urea toN2 The technical realization of the ROMOL-99 process in

a semiautomated separation facility has been carried out byITD Dresden GmbH (former Hans Walischmiller (HWM)GmbH Branch Office Dresden) More than 50 commer-cial batches of fission-based 99Mo using the ROMOL-99process have been successfully completed at PINSTECHPAKGEN 99mTc generators were prepared by using thislocally produced high purity fission 99Mo and distributed to35 nuclear medical centers in Pakistan The performance ofthese generators is comparable to that of generators producedfrom imported fission 99Mo

Conflict of Interests

The authors declare that they have no conflict of interests

References

[1] L G Stang BNL 864 (T-347) 1964[2] D Novotny and G Wagner ldquoProcedure of small scale pro-

duction of Mo-99 on the basis of irradiated natural uraniumtargetsrdquo in Proceedings of the IAEA Consultancy Meeting onSmall Scale Production of Fission Mo-99 for Use in Tc-99mGenerators Vienna Austria July 2003

[3] R Muenze O Hladik G Bernhard W Boessert and RSchwarzbach ldquoLarge scale production of fission 99Mo by usingfuel elements of a research reactor as starting materialrdquo Inter-national Journal of Applied Radiation and Isotopes vol 35 no 8pp 749ndash754 1984

[4] O Hladik G Bernhardt W Boessert and R Muenze ldquoPro-duction of fission 99Mo by processing irradiated natural ura-nium targetsrdquo Fission Molybdenum for Medical Use IAEA-TECDOC-515 IAEA Vienna Austria 1989

[5] G J Beyer R Muenze D Novotny A Mushtaq and MJehangir ldquoROMOL-99mdasha new innovative small-scale LEU-based Mo-99 production processrdquo in Proceedings of the 6thInternational Conference on Isotopes Seoul Republic of KoreaMay 2008

[6] G Beyer R Muenze D Novotny M Ahmad and M JehangirldquoS8-4 ROMOL-99 a new innovative small-scale LEU-basedMo-99 production processrdquo in Proceedings of the InternationalMeeting on Reduced Enrichment for Research and Test Reactors(RERTR rsquo08) Washington DC USA October 2008

[7] G Beyer R Muenze D Novotny M Ahmad and M JehangirldquoS13-P6 ROMOL-99 a new innovative small-scale LEU-basedMo-99 production processrdquo in Proceedings of the 31th Interna-tional Meeting on Reduced Enrichment for Research and TestReactors (RERTR rsquo09) Beijing China November 2009

[8] A Mushtaq ldquoSpecifications and qualification of uraniumaluminum alloy plate target for the production of fissionmolybdenum-99rdquo Nuclear Engineering and Design vol 241 no1 pp 163ndash167 2011

[9] NuDat 25 wwwnndcbnlgovnudat2[10] A A Sameh and H J Ache ldquoProduction techniques for fission

molybdenum -99rdquo Radiochimika Acta vol 41 pp 65ndash72 1987[11] M V Wilkinson A V Mondino and A C Manzini ldquoSep-

aration of iodine produced from fission using silver-coatedaluminardquo Journal of Radioanalytical andNuclear Chemistry vol256 no 3 pp 413ndash415 2003

[12] A Mushtaq S Pervez S Hussain et al ldquoEvaluation of Pakgen99mTc generators loaded with indigenous fission 99Mordquo Radio-chim Acta vol 100 pp 793ndash800 2012

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Power ElectronicsHindawi Publishing Corporationhttpwwwhindawicom Volume 2014

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Renewable Energy

Submit your manuscripts athttpwwwhindawicom


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Hindawi Publishing Corporation httpwwwhindawicom

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Nuclear EnergyInternational Journal of


High Energy PhysicsAdvances in

The Scientific World JournalHindawi Publishing Corporation httpwwwhindawicom Volume 2014


do not dispose of enriched nuclear fuel material Approxi-mately 400 g of uranium oxide enclosed in irradiation cansare dissolved in nitric acid after irradiation for 100 hrs at aneutron flux of 5 times 1013 cm2sminus1 in a research reactor Theseparation of 99Mo from the fuel-fission product solutionis performed by ion exchange with alumina in a chro-matography column Final purification includes the repeatedchromatography separation and subsequently a sublimationstage

Based on their own long-term experiences and consider-ing international achievements in 99Moproduction scientistsof the Radio-Isotope department of the former Rossendorfinstitute ZfK designed a new process for fission-based 99Moproduction named ROMOL-99 [5ndash7]The basic principles ofthis process are as follows (see also the flow scheme Figure 1)

(i) The dissolution of the UAlxAl-clad targets shall beperformed in amixture of NaOHNaNO

3without H

2

generation under reduced pressure conditions(ii) The Xe shall be trapped cryogenically after passing a

gas treatment line(iii) The NH

3generated in the dissolving process shall be

separated prior to Mo separation(iv) The radioiodine shall be separated prior to 99Mo-

separation as well(v) During dissolving process nitrite is generated which

shall be eliminated prior to the 99Mo separation

The basic parameters of this process has been developedwith modern nonradioactive analytical techniques by theIAF-Radiookologie GmbH Dresden while the active testingand optimization of the process has been carried out atPINSTECH Islamabad under supervision of the Germanscientists In this paper the chemical process of the ROMOL-99 technology will be described in some detail

2 Materials and Methods

All chemicals were purchased from E Merck (Germany) andwere of guaranteed reagent grade (GR) or analytical reagent(AR) grade Al

2O3(90 active acidic for column chromatog-

raphy 70ndash230 mesh ASTM) was used Silver-coated aluminawas freshly prepared at institute Organic anion-exchangeresin was purchased from BioRad USA

The non-radioactive development work was performedusing uranium-free Al-plates (purchased from PINSTECH)having the same composition as the material used for theoriginal targets

Tracer experiments were performed using 131I traceractivities which were taken from the PINSTECH routine131Iodine production and the 99Mo tracer was taken fromthe routine PAKGEN 99mTc generator production (99Moimported from South Africa)

21 Irradiation of Target Qualified HEUAl alloy clad withhigh purity aluminum target plates [8] were irradiated for12ndash18 h at a neutron flux of sim15 times 1014 cmminus2sminus1 inside the

Irradiated Xe-133decay

Basic dissolution NH3 H2OXeKrH-3

Filtration NH3-trappingin H2SO4

HL solidwaste

U-235Iodine removing

Xe (residues)

(residues)IL solid wastespent

Agaluminacolumns

AcidificationHNO3

Iodine(residues) Iodine gas trap

Al2O3 column ILL acid wasteHNO3

Purification 1DOWEX

IL solid wastespent column

Purification 2Evaporation

LLL basicwaste

Purification 3Sublimation

LL solid wastespent materials

dispensing

(final product)

Gastraps

UAl targets

3 M NaOH4 M NaNO3

U + FP + TU

Mo + FP

99Mo

99Mo

99Mo separation

filter cake

Figure 1 Process flow scheme of the ROMOL-99 process

core of the Pakistan Research Reactor-1 (PARR-1) After 24 hcooling the irradiated target plates were transferred to the99Molybdenum Production Facility (MPF) for separation of99Mo from the uranium actinides and fission products Forthe warm test runs targets were irradiated for short times atlower flux density but the target composition was identicalwith those for production runs The irradiation conditionswere chosen in a way that the total activity inventory for thedevelopment work was of the order of 4GBq

22 Process Control and Quality Control Gamma ray spec-troscopy high-purity Ge detector (Canberra Series 85 multi-channel analyzer) was used to determine the activity balanceduring all process steps and for the determination of radionu-clide impurities in the final 99Mo product This concernsmainly 131I and 103Ru 132Te Beta counting of 89Sr and 90Srwas done by a liquid scintillation analyzer (Tri-Carb 1900TR Packard Canberra Company) after separation by ion-exchange and precipitation with the aid of carrier Con-tamination of alpha emitters was done with the 120572-counter(UMF-200) Radiochemical purity of [99Mo] molybdatewas determined by means of paper chromatography with a









2O 997888rarr

8NaAlO2+ 3NH

3

(1)


NaAlO2+ 15NaNO

2+ 05H

2O

(2)


2+ 15H

2 (3)




2






Al + 00085U + (03814 + 1125119909)NaNO3

+ (06271 + 0375119909)NaOH

+ (02585 minus 075119909)H2O 997888rarr

NaAlO2+ 000425Na

2U2O7


(4)



2) which












3is trapped in 5N H

2SO4solution


2U2O7 Based



2U2O7times






2O2)



2U2O7) in the




0

20

40

60

80

100

0 10 20 30 40 50 60 70 80 90Time (min)


Hea

ting

on

Coo

ling

on

Coo

ling

jack

et em

pty

Coo

ling

jack

et em

pty

End of dissolving

Tem

pera

ture

(∘C)

(a)

minus05

minus04

minus03

minus02

minus01

0

0 10 20 30 40 50 60 70 80 90


Time (min)

Pres

sure

(b)

(b)



Alloyingelement



Precipitatedspecies











3-acid media at Al



2generation is



3solution




(NH2)2CO + 2HNO

2997888rarr 2N

2+ CO2+ 3H2O (5)



0

1000

2000

3000

4000

5000

6000

5 10 20 30 40 50 60 70 802120579

Lin

(cou

nts)









1E + 01

1E + 02

1E + 03

1E + 04

1E + 05

200 300 400 500 600 700 800 900 1000

Cou

nts 103Ru

131I133I

132I

Energy (keV)






2O3column process


0

1

2

3

4

5

6

7

8

9

10

5 10 15 20 25Volume (mL)

pH an

dd

(pH

)
























2O3






2O3


















020000400006000080000

100000120000140000160000

0 500 1000 1500 2000 2500mL of eluate

CPM

on

MCA






3(2M



4




119863= 270


119863= 08 for the







4)2CO3is being











020000400006000080000

100000120000140000160000180000

0 50 100 150 200 250 300Eluted volumn (mL)

Cou

nts o

n M

CA





3or NH

4OH



1E + 01

1E + 02

1E + 03

1E + 04

1E + 05

1E + 06

1E + 07

1E + 08

1E + 09

100 200 300 400 500 600

Cou

nts p

er ch

anne

l

99Mo239Np 140La

103Ru133I

131I

Filtrate

Energy (keV)

99Mo

99m Tc

X 1000

X 100

X 10

X 01 Final product

Precipitate

+ 01

+ 02

+ 03

+ 04

+ 05

+ 06

+ 07

+ 08

+ 09

99Mo239Np 140La

103Ru133I

131I

Filtrate

99Mo

99m Tc

X 1000

X 100

X 10

X 01 Final product

Precipitate

Feed to AL2O3



2O3column prior to























4 Conclusion


3and radio-





References

















FuelsJournal of







Advances in



Journal of


Renewable Energy





RotatingMachinery


EnergyJournal of

























2O 997888rarr

8NaAlO2+ 3NH

3

(1)


NaAlO2+ 15NaNO

2+ 05H

2O

(2)


2+ 15H

2 (3)




2






Al + 00085U + (03814 + 1125119909)NaNO3

+ (06271 + 0375119909)NaOH

+ (02585 minus 075119909)H2O 997888rarr

NaAlO2+ 000425Na

2U2O7


(4)



2) which












3is trapped in 5N H

2SO4solution


2U2O7 Based



2U2O7times






2O2)



2U2O7) in the




0

20

40

60

80

100

0 10 20 30 40 50 60 70 80 90Time (min)


Hea

ting

on

Coo

ling

on

Coo

ling

jack

et em

pty

Coo

ling

jack

et em

pty

End of dissolving

Tem

pera

ture

(∘C)

(a)

minus05

minus04

minus03

minus02

minus01

0

0 10 20 30 40 50 60 70 80 90


Time (min)

Pres

sure

(b)

(b)



Alloyingelement



Precipitatedspecies











3-acid media at Al



2generation is



3solution




(NH2)2CO + 2HNO

2997888rarr 2N

2+ CO2+ 3H2O (5)



0

1000

2000

3000

4000

5000

6000

5 10 20 30 40 50 60 70 802120579

Lin

(cou

nts)









1E + 01

1E + 02

1E + 03

1E + 04

1E + 05

200 300 400 500 600 700 800 900 1000

Cou

nts 103Ru

131I133I

132I

Energy (keV)






2O3column process


0

1

2

3

4

5

6

7

8

9

10

5 10 15 20 25Volume (mL)

pH an

dd

(pH

)
























2O3






2O3


















020000400006000080000

100000120000140000160000

0 500 1000 1500 2000 2500mL of eluate

CPM

on

MCA






3(2M



4




119863= 270


119863= 08 for the







4)2CO3is being











020000400006000080000

100000120000140000160000180000

0 50 100 150 200 250 300Eluted volumn (mL)

Cou

nts o

n M

CA





3or NH

4OH



1E + 01

1E + 02

1E + 03

1E + 04

1E + 05

1E + 06

1E + 07

1E + 08

1E + 09

100 200 300 400 500 600

Cou

nts p

er ch

anne

l

99Mo239Np 140La

103Ru133I

131I

Filtrate

Energy (keV)

99Mo

99m Tc

X 1000

X 100

X 10

X 01 Final product

Precipitate

+ 01

+ 02

+ 03

+ 04

+ 05

+ 06

+ 07

+ 08

+ 09

99Mo239Np 140La

103Ru133I

131I

Filtrate

99Mo

99m Tc

X 1000

X 100

X 10

X 01 Final product

Precipitate

Feed to AL2O3



2O3column prior to























4 Conclusion


3and radio-





References

















FuelsJournal of







Advances in



Journal of


Renewable Energy





RotatingMachinery


EnergyJournal of


















0

20

40

60

80

100

0 10 20 30 40 50 60 70 80 90Time (min)


Hea

ting

on

Coo

ling

on

Coo

ling

jack

et em

pty

Coo

ling

jack

et em

pty

End of dissolving

Tem

pera

ture

(∘C)

(a)

minus05

minus04

minus03

minus02

minus01

0

0 10 20 30 40 50 60 70 80 90


Time (min)

Pres

sure

(b)

(b)



Alloyingelement



Precipitatedspecies











3-acid media at Al



2generation is



3solution




(NH2)2CO + 2HNO

2997888rarr 2N

2+ CO2+ 3H2O (5)



0

1000

2000

3000

4000

5000

6000

5 10 20 30 40 50 60 70 802120579

Lin

(cou

nts)









1E + 01

1E + 02

1E + 03

1E + 04

1E + 05

200 300 400 500 600 700 800 900 1000

Cou

nts 103Ru

131I133I

132I

Energy (keV)






2O3column process


0

1

2

3

4

5

6

7

8

9

10

5 10 15 20 25Volume (mL)

pH an

dd

(pH

)
























2O3






2O3


















020000400006000080000

100000120000140000160000

0 500 1000 1500 2000 2500mL of eluate

CPM

on

MCA






3(2M



4




119863= 270


119863= 08 for the







4)2CO3is being











020000400006000080000

100000120000140000160000180000

0 50 100 150 200 250 300Eluted volumn (mL)

Cou

nts o

n M

CA





3or NH

4OH



1E + 01

1E + 02

1E + 03

1E + 04

1E + 05

1E + 06

1E + 07

1E + 08

1E + 09

100 200 300 400 500 600

Cou

nts p

er ch

anne

l

99Mo239Np 140La

103Ru133I

131I

Filtrate

Energy (keV)

99Mo

99m Tc

X 1000

X 100

X 10

X 01 Final product

Precipitate

+ 01

+ 02

+ 03

+ 04

+ 05

+ 06

+ 07

+ 08

+ 09

99Mo239Np 140La

103Ru133I

131I

Filtrate

99Mo

99m Tc

X 1000

X 100

X 10

X 01 Final product

Precipitate

Feed to AL2O3



2O3column prior to























4 Conclusion


3and radio-





References

















FuelsJournal of







Advances in



Journal of


Renewable Energy





RotatingMachinery


EnergyJournal of


















0

1000

2000

3000

4000

5000

6000

5 10 20 30 40 50 60 70 802120579

Lin

(cou

nts)









1E + 01

1E + 02

1E + 03

1E + 04

1E + 05

200 300 400 500 600 700 800 900 1000

Cou

nts 103Ru

131I133I

132I

Energy (keV)






2O3column process


0

1

2

3

4

5

6

7

8

9

10

5 10 15 20 25Volume (mL)

pH an

dd

(pH

)
























2O3






2O3


















020000400006000080000

100000120000140000160000

0 500 1000 1500 2000 2500mL of eluate

CPM

on

MCA






3(2M



4




119863= 270


119863= 08 for the







4)2CO3is being











020000400006000080000

100000120000140000160000180000

0 50 100 150 200 250 300Eluted volumn (mL)

Cou

nts o

n M

CA





3or NH

4OH



1E + 01

1E + 02

1E + 03

1E + 04

1E + 05

1E + 06

1E + 07

1E + 08

1E + 09

100 200 300 400 500 600

Cou

nts p

er ch

anne

l

99Mo239Np 140La

103Ru133I

131I

Filtrate

Energy (keV)

99Mo

99m Tc

X 1000

X 100

X 10

X 01 Final product

Precipitate

+ 01

+ 02

+ 03

+ 04

+ 05

+ 06

+ 07

+ 08

+ 09

99Mo239Np 140La

103Ru133I

131I

Filtrate

99Mo

99m Tc

X 1000

X 100

X 10

X 01 Final product

Precipitate

Feed to AL2O3



2O3column prior to























4 Conclusion


3and radio-





References

















FuelsJournal of







Advances in



Journal of


Renewable Energy





RotatingMachinery


EnergyJournal of


























2O3






2O3


















020000400006000080000

100000120000140000160000

0 500 1000 1500 2000 2500mL of eluate

CPM

on

MCA






3(2M



4




119863= 270


119863= 08 for the







4)2CO3is being











020000400006000080000

100000120000140000160000180000

0 50 100 150 200 250 300Eluted volumn (mL)

Cou

nts o

n M

CA





3or NH

4OH



1E + 01

1E + 02

1E + 03

1E + 04

1E + 05

1E + 06

1E + 07

1E + 08

1E + 09

100 200 300 400 500 600

Cou

nts p

er ch

anne

l

99Mo239Np 140La

103Ru133I

131I

Filtrate

Energy (keV)

99Mo

99m Tc

X 1000

X 100

X 10

X 01 Final product

Precipitate

+ 01

+ 02

+ 03

+ 04

+ 05

+ 06

+ 07

+ 08

+ 09

99Mo239Np 140La

103Ru133I

131I

Filtrate

99Mo

99m Tc

X 1000

X 100

X 10

X 01 Final product

Precipitate

Feed to AL2O3



2O3column prior to























4 Conclusion


3and radio-





References

















FuelsJournal of







Advances in



Journal of


Renewable Energy





RotatingMachinery


EnergyJournal of

























020000400006000080000

100000120000140000160000180000

0 50 100 150 200 250 300Eluted volumn (mL)

Cou

nts o

n M

CA





3or NH

4OH



1E + 01

1E + 02

1E + 03

1E + 04

1E + 05

1E + 06

1E + 07

1E + 08

1E + 09

100 200 300 400 500 600

Cou

nts p

er ch

anne

l

99Mo239Np 140La

103Ru133I

131I

Filtrate

Energy (keV)

99Mo

99m Tc

X 1000

X 100

X 10

X 01 Final product

Precipitate

+ 01

+ 02

+ 03

+ 04

+ 05

+ 06

+ 07

+ 08

+ 09

99Mo239Np 140La

103Ru133I

131I

Filtrate

99Mo

99m Tc

X 1000

X 100

X 10

X 01 Final product

Precipitate

Feed to AL2O3



2O3column prior to























4 Conclusion


3and radio-





References

















FuelsJournal of







Advances in



Journal of


Renewable Energy





RotatingMachinery


EnergyJournal of





































4 Conclusion


3and radio-





References

















FuelsJournal of







Advances in



Journal of


Renewable Energy





RotatingMachinery


EnergyJournal of





















FuelsJournal of







Advances in



Journal of


Renewable Energy





RotatingMachinery


EnergyJournal of

















the fission-based 99 mo production process …downloads.hindawi.com/journals/stni/2013/932546.pdfare...

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