SlideShare a Scribd company logo
Spent Fuel and Waste Science and Technology
Experiments to Evaluate Colloid-
Facilitated Transport of Cesium Over
Long Time and Distance Scales
Katherine Telfeyan, Paul W. Reimus, S. Doug Ware
Los Alamos National Laboratory
Earth System Observations EES-14
Radiogeochemistry Group
Argillite/Crystalline Session
SFWST Working Group Meeting
May 23, 2017
Spent Fuel and
Waste Science and
Technology
2
Introduction
 Strongly-sorbing radionuclides are only likely to be transported from
nuclear repositories via colloid-facilitated transport
 Previous work on 137Cs sorption to colloids
– Sorption has a nonlinear dependence on 137Cs concentration
– Part of the 137Cs sorbed to colloids is desorbed very slowly or is
partially irreversible
GTSFieldExperiments
LabExperiments
Missana et al. (2004)
Argillite/Crystalline Session of SFWST Working Group Meeting6/23/2016
Spent Fuel and
Waste Science and
Technology
Introduction
 Discrepancy between 137Cs transport in the Grimsel Field System and in
laboratory experiments
– Higher Cs concentrations in laboratory (10-7 M, weak site dominance) compared
to field study (10-10 M, strong site dominance)
 High and low affinity sites
– 2-site sorption model for previous column experiments
3
0.0
0.2
0.4
0.6
0.8
1.0
1.2
0 100 200 300 400 500 600
C/Co
Volume, ml
H-3
H-3Model
Colloids
ColloidModel
Cesium
CesiumModel
0
0.2
0.4
0.6
0.8
1
0 50 100 150 200
C/Co
Cumulative Volume (mL)
Cs w/o colloids
Total Cs w/colloids
Dissolved Cs w/colloids
Cs w/o Col Model
Cs w/ Col Model
H-3
GTSFieldExperiments
LabExperiments
High Cs concentrations – Bentonite, Dittrich 2015Low Cs concentrations – Chancellor Colloids
Argillite/Crystalline Session of SFWST Working Group Meeting6/23/2016
Spent Fuel and
Waste Science and
Technology
Methods
 Mini columns (Dittrich et al., 2015)
– Allow for rapid interrogation of sorption parameters with minimal amounts of solid
material and waste generation
– Allow for multiple columns run in parallel
 2 sets of column experiments with Grimsel granodiorite
– 137Cs adsorbed to colloids in Chancellor cavity water
– Bentonite colloids presorbed with carrier-free 137Cs to study very low concentrations
(10-11 M)
 Measure eluent to determine 137Cs partitioning between the colloidal and dissolved
phase
– Colloid separation by ultracentrifugation (15,000 rpm) or filtration (0.02 µm)
– Colloid concentration by Hach turbidimeter
– 137Cs and 3H (conservative tracer) concentrations measured by liquid scintillation
counting
4
Argillite/Crystalline Session of SFWST Working Group Meeting6/23/2016
Spent Fuel and
Waste Science and
Technology
Column Experiments
5
Analysis
> Colloid concentration
> 137Cs with colloids and in
dissolved fraction
> 3H concentration
Pass eluent through additional columns
> Determine slow colloid filtration rates
> Determine 137Cs desorption rates
Colloid-free solution passed through all columns
> Determine desorption and recovery of 137Cs
Argillite/Crystalline Session of SFWST Working Group Meeting6/23/2016
Spent Fuel and
Waste Science and
Technology
Column Experiments
6
Argillite/Crystalline Session of SFWST Working Group Meeting6/23/2016
Spent Fuel and
Waste Science and
Technology
Batch Desorption Experiments
 Desorption of 137Cs from colloids in synthetic Grimsel groundwater
– What is the desorption rate of 137Cs from colloids in the absence of
solids?
– Is additional 137Cs desorbed in waters with elevated non-rad Cs
concentrations?
7
Argillite/Crystalline Session of SFWST Working Group Meeting6/23/2016
Spent Fuel and
Waste Science and
Technology
THANK YOU!
8
Argillite/Crystalline Session of SFWST Working Group Meeting6/23/2016

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14 experiments to evaluate colloid facilitated transport of cesium over long time and distance scales telfeyan lanl

  • 1. Spent Fuel and Waste Science and Technology Experiments to Evaluate Colloid- Facilitated Transport of Cesium Over Long Time and Distance Scales Katherine Telfeyan, Paul W. Reimus, S. Doug Ware Los Alamos National Laboratory Earth System Observations EES-14 Radiogeochemistry Group Argillite/Crystalline Session SFWST Working Group Meeting May 23, 2017
  • 2. Spent Fuel and Waste Science and Technology 2 Introduction  Strongly-sorbing radionuclides are only likely to be transported from nuclear repositories via colloid-facilitated transport  Previous work on 137Cs sorption to colloids – Sorption has a nonlinear dependence on 137Cs concentration – Part of the 137Cs sorbed to colloids is desorbed very slowly or is partially irreversible GTSFieldExperiments LabExperiments Missana et al. (2004) Argillite/Crystalline Session of SFWST Working Group Meeting6/23/2016
  • 3. Spent Fuel and Waste Science and Technology Introduction  Discrepancy between 137Cs transport in the Grimsel Field System and in laboratory experiments – Higher Cs concentrations in laboratory (10-7 M, weak site dominance) compared to field study (10-10 M, strong site dominance)  High and low affinity sites – 2-site sorption model for previous column experiments 3 0.0 0.2 0.4 0.6 0.8 1.0 1.2 0 100 200 300 400 500 600 C/Co Volume, ml H-3 H-3Model Colloids ColloidModel Cesium CesiumModel 0 0.2 0.4 0.6 0.8 1 0 50 100 150 200 C/Co Cumulative Volume (mL) Cs w/o colloids Total Cs w/colloids Dissolved Cs w/colloids Cs w/o Col Model Cs w/ Col Model H-3 GTSFieldExperiments LabExperiments High Cs concentrations – Bentonite, Dittrich 2015Low Cs concentrations – Chancellor Colloids Argillite/Crystalline Session of SFWST Working Group Meeting6/23/2016
  • 4. Spent Fuel and Waste Science and Technology Methods  Mini columns (Dittrich et al., 2015) – Allow for rapid interrogation of sorption parameters with minimal amounts of solid material and waste generation – Allow for multiple columns run in parallel  2 sets of column experiments with Grimsel granodiorite – 137Cs adsorbed to colloids in Chancellor cavity water – Bentonite colloids presorbed with carrier-free 137Cs to study very low concentrations (10-11 M)  Measure eluent to determine 137Cs partitioning between the colloidal and dissolved phase – Colloid separation by ultracentrifugation (15,000 rpm) or filtration (0.02 µm) – Colloid concentration by Hach turbidimeter – 137Cs and 3H (conservative tracer) concentrations measured by liquid scintillation counting 4 Argillite/Crystalline Session of SFWST Working Group Meeting6/23/2016
  • 5. Spent Fuel and Waste Science and Technology Column Experiments 5 Analysis > Colloid concentration > 137Cs with colloids and in dissolved fraction > 3H concentration Pass eluent through additional columns > Determine slow colloid filtration rates > Determine 137Cs desorption rates Colloid-free solution passed through all columns > Determine desorption and recovery of 137Cs Argillite/Crystalline Session of SFWST Working Group Meeting6/23/2016
  • 6. Spent Fuel and Waste Science and Technology Column Experiments 6 Argillite/Crystalline Session of SFWST Working Group Meeting6/23/2016
  • 7. Spent Fuel and Waste Science and Technology Batch Desorption Experiments  Desorption of 137Cs from colloids in synthetic Grimsel groundwater – What is the desorption rate of 137Cs from colloids in the absence of solids? – Is additional 137Cs desorbed in waters with elevated non-rad Cs concentrations? 7 Argillite/Crystalline Session of SFWST Working Group Meeting6/23/2016
  • 8. Spent Fuel and Waste Science and Technology THANK YOU! 8 Argillite/Crystalline Session of SFWST Working Group Meeting6/23/2016