malmö, abm meeting may 2012 mineralogical investigations of the alternative buffer material test...
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![Page 1: Malmö, ABM meeting May 2012 Mineralogical investigations of the alternative buffer material test – II. Exchangeable cation population rearrangement Dohrmann,](https://reader035.vdocuments.mx/reader035/viewer/2022062221/56649ee45503460f94bf3333/html5/thumbnails/1.jpg)
Malmö, ABM meeting May 2012
Mineralogical investigations of the alternative buffer material test – II. Exchangeable cation population rearrangement
Dohrmann, R., Kaufhold, S., BGR/LBEGSiv Olsson, Clay TechnologyPatrik Sellin, SKB
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Malmö, ABM meeting May 2012
Motivation and questions• Large differences of initial and final exchangeable cation population of 10 blocks reported during 2010 meeting
• Open questions: - confirm this trend for more blocks - vertical profiles- Ca2+ dominating in the top region?- influence of cement at the top - combination of all data sets available
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BGR sampling
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Malmö, ABM meeting May 2012
Available blocks Block Material/abbreviation NH4Cl-ethanol Cu-trien Cu-trien5xcalcite horizontal vertical
30 MX80 29 MX80 28 Ikosorb (IKO)27 Dep. CAN 26 Ibeco Seal (IBE) 25 Friedland (FRI) 24 Asha 505 23 Calcigel (CAL) 22 Callovo-Oxfordian 21 Febex 20 MX80 granulate19 MX80 granulate +quartz18 MX8017 Kunigel V1 (JNB) 16 Rokle (Rawra) 15 Dep. CAN 14 Asha 505 13 Rokle (Rawra) 12 Callovo-Oxfordian11 MX80 10 Ikosorb (IKO) 9 Friedland (FRI) 8 Febex 7 MX80 granulate +quartz6 Ibeco Seal (IBE) 5 Calcigel (CAL) 4 Kunigel V1 (JNB)3 MX80 granulate2 MX80 1 MX80
samplingCEC method
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I. horizontal variation
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Malmö, ABM meeting May 2012
values of JNB-17 can be averagedMethod Bentonite Position Na+ K+ Mg2+ Ca2+ sum/CEC CEC
(cm) from contact (meq/100 g)
NH4Cl-ethanol JNB-Ref reference 86 2 1 9
NH4Cl-ethanol JNB-17 1 41 2 9 47
NH4Cl-ethanol JNB-17 5 42 2 9 48
NH4Cl-ethanol JNB-17 9 43 2 8 47
Cu-trien5xcalcite JNB-Ref reference 91 0 1 6 1.06 62Cu-trien5xcalcite JNB-Ref reference 92 0 1 6 1.00 64Cu-trien5xcalcite JNB-17 3 43 3 9 44 1.00 63Cu-trien5xcalcite JNB-17 3 44 2 9 44 1.02 61Cu-trien5xcalcite JNB-17 5 44 2 10 43 1.00 61Cu-trien5xcalcite JNB-17 5 45 3 10 42 1.02 61
Cu-trien JNB-Ref reference 102 1 3 36 1.41 59Cu-trien JNB-Ref reference 100 1 2 28 1.30 60Cu-trien JNB-17 0.1 41 0 9 86 1.37 49Cu-trien JNB-17 0.1 40 1 9 83 1.31 48Cu-trien JNB-17 1 45 1 9 74 1.29 58Cu-trien JNB-17 1 47 2 9 65 1.23 57Cu-trien JNB-17 3 43 1 10 74 1.29 58Cu-trien JNB-17 3 45 1 10 70 1.27 56Cu-trien JNB-17 5 43 1 10 74 1.29 58Cu-trien JNB-17 5 45 1 10 70 1.25 56Cu-trien JNB-17 7 46 2 10 68 1.25 59Cu-trien JNB-17 7 46 1 10 68 1.25 57
methods 1-3 JNB-Ref 94 1 2 17 1.19 61methods 1-3 JNB-17 1-7 44 2 10 58 1.18 59methods 1 and 3 JNB-Ref 7 1.03methods 1 and 3 JNB-17 1-7 45 1.01
average
(% / CEC)
(% / sum of cations)
contact
xx xx
possibly clinoptilolite dissolution?
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Typical lateral variation
0
20
40
60
80
100
0 1 2 3 4 5 6 7 8 9 10 11 12
cm
exch
ang
eab
le c
atio
ns
(%/C
EC
or
%/s
um
)
Na+ K+ Mg2+ Ca2+
typical lateral cation distribution after retrieval
refe
renc
e va
lues
c
on
tact
Ca2+
Na+
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Malmö, ABM meeting May 2012
No horizontal variation found for non-contact samples.
This trend was confirmed for the other blocks.
-> avarge values of reacted blocks were calculated and
compared with initial composition
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Malmö, ABM meeting May 2012
values of reference blocks• All values were measured, some were corrected:
• CEC%EC ‘MX80 granulate + quartz’ = MX80 x 0.7 according to a quartz content of 30 wt.%.
• Na+ (Ca2+) values of blocks 9 and 25 were corrected to give Na+=100‑K+‑Mg2+-Ca2+
• Ca2+ values of block 22 were corrected to give Ca2+=100‑Na+‑K+‑Mg2+.
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Malmö, ABM meeting May 2012
values of reacted blocks
• Ca2+ values of blocks 9, 22, and 25 were corrected to give Ca2+=100‑Na+‑K+‑Mg2+.
• Ethanolic NH4Cl-EC values of such samples were recalculated using the measured reference CEC to avoid largely inflated Ca2+ percentages and accordingly diminished percentages for Na+, K+, and Mg2+.
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Na+ K+ Mg2+ Ca2+ sum CEC Na+ K+ Mg2+ Ca2+ sum CECBlock Material/abbreviation (meq/100 g) (meq/100 g)
30 MX80 69 2 8 24 103 85 49 3 7 41 10029 MX80 69 2 8 24 103 85 41 2 13 44 10028 Ikosorb (IKO) 56 2 24 19 100 9027 Dep. CAN 27 2 27 46 102 84 25 2 10 63 10026 Ibeco Seal (IBE) 87 3 4 7 100 88 24 1 11 63 10025 Friedland (FRI) 69 8 22 2 101 23 37 6 11 46 100 2124 Asha 505 67 1 15 20 103 91 23 1 13 63 10023 Calcigel (CAL) 3 2 22 72 100 65 23 2 13 65 102 6422 Callovo-Oxfordian 24 11 29 35 100 12 44 8 26 22 100 1221 Febex 25 1 39 34 100 98 23 1 16 60 10020 MX80 granulate 69 2 8 24 103 8519 MX80 granulate +quartz 69 2 8 24 103 5918 MX80 69 2 8 24 103 8517 Kunigel V1 (JNB) 87 2 1 10 100 61 42 2 9 47 100 5716 Rokle (Rawra) 1 2 21 76 100 74 34 1 14 51 10015 Dep. CAN 27 2 27 46 102 84 36 2 17 50 104 7614 Asha 505 67 1 15 20 103 91 33 1 21 49 103 8313 Rokle (Rawra) 1 3 24 71 99 74 41 3 21 44 109 7112 Callovo-Oxfordian 24 11 29 35 100 1211 MX80 69 2 8 24 103 85 54 1 17 37 109 7610 Ikosorb (IKO) 56 2 24 19 100 90 45 2 18 36 100 879 Friedland (FRI) 69 8 22 2 101 23 59 9 19 13 100 218 Febex 27 3 37 33 100 101 42 3 23 34 102 957 MX80 granulate +quartz 69 2 8 24 103 596 Ibeco Seal (IBE) 90 4 6 8 109 88 40 4 12 50 106 805 Calcigel (CAL) 4 2 19 76 100 65 44 2 8 47 1004 Kunigel V1 (JNB) 87 2 1 10 100 613 MX80 granulate 69 2 8 24 103 852 MX80 69 2 8 24 103 85 60 2 10 28 1001 MX80 69 2 8 24 103 85
1-30
average (only of those blocks which were analysed after retrieval; exchangeable cations: n=21; CEC: n=12)
48 3 18 32 66 39 3 15 45 62
1-30 MIN 1 1 1 2 12 23 1 7 13 121-30 MAX 90 11 39 76 101 60 9 26 65 95
reference material
(%) (%)
retrieved samples 1-9 cm (averages)
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-80% -60% -40% -20% 0% 20% 40% 60% 80%
exchangeable cation population (%)
MX80
MX80
MX80 granulate
Kunigel V1 (JNB)
Calcigel (CAL)
Ibeco Seal (IBE)
MX80 granulate +quartz
Febex
Friedland (FRI)
Ikosorb (IKO)
MX80
Callovo-Oxfordian
Rokle (Rawra)
Asha 505
Dep. CAN
Rokle (Rawra)
Kunigel V1 (JNB)
MX80
MX80 granulate +quartz
MX80 granulate
Febex
Callovo-Oxfordian
Calcigel (CAL)
Asha 505
Friedland (FRI)
Ibeco Seal (IBE)
Dep. CAN
Ikosorb (IKO)
MX80
MX80
Na+ K+ Mg2+ Ca2+
0% 20% 40% 60% 80% 100%
exchangeable cation population (%)
MX80
MX80
MX80 granulate
Kunigel V1 (JNB)
Calcigel (CAL)
Ibeco Seal (IBE)
MX80 granulate +quartz
Febex
Friedland (FRI)
Ikosorb (IKO)
MX80
Callovo-Oxfordian
Rokle (Rawra)
Asha 505
Dep. CAN
Rokle (Rawra)
Kunigel V1 (JNB)
MX80
MX80 granulate +quartz
MX80 granulate
Febex
Callovo-Oxfordian
Calcigel (CAL)
Asha 505
Friedland (FRI)
Ibeco Seal (IBE)
Dep. CAN
Ikosorb (IKO)
MX80
MX80
Na+ K+ Mg2+ Ca2+
0% 20% 40% 60% 80% 100%
exchangeable cation population (%)
MX80
MX80
MX80 granulate
Kunigel V1 (JNB)
Calcigel (CAL)
Ibeco Seal (IBE)
MX80 granulate +quartz
Febex
Friedland (FRI)
Ikosorb (IKO)
MX80
Callovo-Oxfordian
Rokle (Rawra)
Asha 505
Dep. CAN
Rokle (Rawra)
Kunigel V1 (JNB)
MX80
MX80 granulate +quartz
MX80 granulate
Febex
Callovo-Oxfordian
Calcigel (CAL)
Asha 505
Friedland (FRI)
Ibeco Seal (IBE)
Dep. CAN
Ikosorb (IKO)
MX80
MX80
Na+ K+ Mg2+ Ca2+a b c
-80% -60% -40% -20% 0% 20% 40% 60% 80%
exchangeable cation population (%)
MX80
MX80
MX80 granulate
Kunigel V1 (JNB)
Calcigel (CAL)
Ibeco Seal (IBE)
MX80 granulate +quartz
Febex
Friedland (FRI)
Ikosorb (IKO)
MX80
Callovo-Oxfordian
Rokle (Rawra)
Asha 505
Dep. CAN
Rokle (Rawra)
Kunigel V1 (JNB)
MX80
MX80 granulate +quartz
MX80 granulate
Febex
Callovo-Oxfordian
Calcigel (CAL)
Asha 505
Friedland (FRI)
Ibeco Seal (IBE)
Dep. CAN
Ikosorb (IKO)
MX80
MX80
Na+ K+ Mg2+ Ca2+
0% 20% 40% 60% 80% 100%
exchangeable cation population (%)
MX80
MX80
MX80 granulate
Kunigel V1 (JNB)
Calcigel (CAL)
Ibeco Seal (IBE)
MX80 granulate +quartz
Febex
Friedland (FRI)
Ikosorb (IKO)
MX80
Callovo-Oxfordian
Rokle (Rawra)
Asha 505
Dep. CAN
Rokle (Rawra)
Kunigel V1 (JNB)
MX80
MX80 granulate +quartz
MX80 granulate
Febex
Callovo-Oxfordian
Calcigel (CAL)
Asha 505
Friedland (FRI)
Ibeco Seal (IBE)
Dep. CAN
Ikosorb (IKO)
MX80
MX80
Na+ K+ Mg2+ Ca2+
0% 20% 40% 60% 80% 100%
exchangeable cation population (%)
MX80
MX80
MX80 granulate
Kunigel V1 (JNB)
Calcigel (CAL)
Ibeco Seal (IBE)
MX80 granulate +quartz
Febex
Friedland (FRI)
Ikosorb (IKO)
MX80
Callovo-Oxfordian
Rokle (Rawra)
Asha 505
Dep. CAN
Rokle (Rawra)
Kunigel V1 (JNB)
MX80
MX80 granulate +quartz
MX80 granulate
Febex
Callovo-Oxfordian
Calcigel (CAL)
Asha 505
Friedland (FRI)
Ibeco Seal (IBE)
Dep. CAN
Ikosorb (IKO)
MX80
MX80
Na+ K+ Mg2+ Ca2+a b c
initially after exp. differenceEC %
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initially after exp. difference
-60 -40 -20 0 20 40 60
exchangeable cation population (meq/100 g)
MX80
MX80
MX80 granulate
Kunigel V1 (JNB)
Calcigel (CAL)
Ibeco Seal (IBE)
MX80 granulate +quartz
Febex
Friedland (FRI)
Ikosorb (IKO)
MX80
Callovo-Oxfordian
Rokle (Rawra)
Asha 505
Dep. CAN
Rokle (Rawra)
Kunigel V1 (JNB)
MX80
MX80 granulate +quartz
MX80 granulate
Febex
Callovo-Oxfordian
Calcigel (CAL)
Asha 505
Friedland (FRI)
Ibeco Seal (IBE)
Dep. CAN
Ikosorb (IKO)
MX80
MX80
Na+ K+ Mg2+ Ca2+
0 20 40 60 80 100
exchangeable cation population (meq/100 g)
MX80
MX80
MX80 granulate
Kunigel V1 (JNB)
Calcigel (CAL)
Ibeco Seal (IBE)
MX80 granulate +quartz
Febex
Friedland (FRI)
Ikosorb (IKO)
MX80
Callovo-Oxfordian
Rokle (Rawra)
Asha 505
Dep. CAN
Rokle (Rawra)
Kunigel V1 (JNB)
MX80
MX80 granulate +quartz
MX80 granulate
Febex
Callovo-Oxfordian
Calcigel (CAL)
Asha 505
Friedland (FRI)
Ibeco Seal (IBE)
Dep. CAN
Ikosorb (IKO)
MX80
MX80
Na+ K+ Mg2+ Ca2+
0 20 40 60 80 100 120
exchangeable cation population (meq/100 g)
MX80
MX80
MX80 granulate
Kunigel V1 (JNB)
Calcigel (CAL)
Ibeco Seal (IBE)
MX80 granulate +quartz
Febex
Friedland (FRI)
Ikosorb (IKO)
MX80
Callovo-Oxfordian
Rokle (Rawra)
Asha 505
Dep. CAN
Rokle (Rawra)
Kunigel V1 (JNB)
MX80
MX80 granulate +quartz
MX80 granulate
Febex
Callovo-Oxfordian
Calcigel (CAL)
Asha 505
Friedland (FRI)
Ibeco Seal (IBE)
Dep. CAN
Ikosorb (IKO)
MX80
MX80
Na+ K+ Mg2+ Ca2+
EC meq/100 g
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chloride transport
Figures taken from ABM status report
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lesson learned I• horizontal variation of ECs and Cl- was small • CEC was lowered (5 %)• Na+: 48% initially, 39 % after exp. (36->26)• Mg2+: 18% initially, 15 % after exp. (13->10)• Ca2+: 32% initially, 45 % after exp. (24->34)• K+: 3% initially, no changes (2)
(values in meq/100 g)• 8 non-examined Na+ blocks: 6MX80, IKO, JNB
plus COX
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lesson learned II• Ca2+ gain pronounced in upper 7 blocks• Blocks 24-30:
- Na+: 63% initially, 33 % after exp.- Ca2+: 20% initially, 53 % after exp.
• The smallest absolute redistribution of all bentonites was found in MX80 at position 2 (14 meq/100 g). • For the same material also up to 46 meq/100 g were recorded at the other end of the test parcel.
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lesson learned III• No correlation of the extent of the redistribution of the exchangeable cation population with the peak temperatures could be identified • The total amounts of redistributed cations do not correlate with the CEC (R²=0.01)
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gaines and losses of individual blocks
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influence of neighbouring blocks gains and losseswith the same prefix:CAL, FRI, IBE, Rokle;example: CAL
gains and losseswith opposite prefixes:Asha, Dep.CAN, Febexexample: Febex
Na+, K+, Ca2+, Mg2+ Na+, K+, Ca2+, Mg2+
neighboring upper blocksandwiched block A (at position x)neighboring lower block
neighboring upper blocksandwiched block A (at position y)neighboring lower block
gains and losseswith the same prefix:CAL, FRI, IBE, Rokle;example: CAL
gains and losseswith opposite prefixes:Asha, Dep.CAN, Febexexample: Febex
Na+, K+, Ca2+, Mg2+ Na+, K+, Ca2+, Mg2+
neighboring upper blocksandwiched block A (at position x)neighboring lower block
neighboring upper blocksandwiched block A (at position y)neighboring lower block
An+>>Bn+,Cn+An+ ≈ Bn+ ≈ Cn+
(not for ASHA)
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lesson learned IV• The influence of neighbouring blocks on cation redistribution during the ABM experiment was low • Obviously not only the material composition of the adjacent blocks was important for the adsorption behaviour but the position within the test parcel
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vertical exchangeable cation profile
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0 20 40 60
meq/100 g
dis
tan
ce
fro
m c
on
tac
t (c
m)
Na+
K+
Mg2+
Ca2+
0 20 40 60 80
% / CEC
dis
tan
ce
fro
m c
on
tac
t (c
m)
Na+
K+
Mg2+
Ca2+
reference material
reference material
0 20 40 60
meq/100 g
dis
tan
ce
fro
m c
on
tac
t (c
m)
Na+
K+
Mg2+
Ca2+
0 20 40 60 80
% / CEC
dis
tan
ce
fro
m c
on
tac
t (c
m)
Na+
K+
Mg2+
Ca2+
reference material
reference material
% / CEC meq/100 g
CEC of IKO is approximately 15-20% larger than MX80
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lesson learned V• In vertical exchangeable cation profiles of the two adjacent blocks MX80 (No. 11) and IKO (No. 10) all exchangeable cations show bi-modal concentration distributions with gaps of
2% / 5% / 7% for Mg2+ / Ca2+ / Na+
-> different selectivities?
• Mg2+ was transported from IKO into MX80 but not into FRI
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influence of the cement plug on top of the parcel
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0% 50% 100%
1.25
3.5
5.5
7.5
9.5
11.5
13.5
15.5
17.5
19.5
MX
80
blo
ck
29
& 3
0
Ca %K %Mg %Na %
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• Vertical trend was confirmed (less samples)
• Horizontally no changes but ≈ 5-10 % less Ca2+ in the outer parts (closer to the rock)
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Malmö, ABM meeting May 2012
lesson learned VI• The so-called top blocks (No. 29 and 30) showed the opposite behaviour than expected.
• Ca2+ and Mg2+ increased downwards from the outer part of block 30 to the lower part of block 29 while Na+ decreased. Mg2+ increased from 6 to 14 %.
• Horizontally no changes but ≈ 5-10 % less Ca2+ in the outer parts (closer to the rock), however MX80 contains soluble Ca-minerals which could have overprinted Ca2+.
• This vertical process is still unclear because overall Ca2+ was enriched in the upper parcel region, so what was the driving force (temperature ?)?
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Ca2+ sources• Ca2+ increased while Na+ and Mg2+ decreased
• ÄSPÖ water: ≈ 2500 mg/L Na+ and Ca2+ each, ≈ 8500 mg/L Cl-, and ≈ 500 mg/L SO42
-; Mg2+, Br-, and K+ (all < 100 mg/L)
• Carbonates: high TIC in Dep.CAN, IBE but didn’t change in bulk blocks
• Sulfates: high total S in Dep.CAN, FRI but didn’t change largely in bulk blocks
![Page 29: Malmö, ABM meeting May 2012 Mineralogical investigations of the alternative buffer material test – II. Exchangeable cation population rearrangement Dohrmann,](https://reader035.vdocuments.mx/reader035/viewer/2022062221/56649ee45503460f94bf3333/html5/thumbnails/29.jpg)
Malmö, ABM meeting May 2012
Thank you