Experimental and modelling investigations of the biogeochemistry of gas production from low and intermediate level radioactive waste

Joe Small (Corresponding Author), Mikko Nykyri, Mika Helin, Ulla Hovi, Tuija Sarlin, Merja Itävaara

Research output: Contribution to journalArticleScientificpeer-review

19 Citations (Scopus)

Abstract

The degradation of organic wastes and the corrosion of metallic wastes and steel containers in low and intermediate level radioactive waste (LLW/ILW) repositories are important processes that affect repository geochemistry and the speciation and transport of radionuclides. Gas is generated in association with these degradation processes and this has the potential to overpressure the repository, which can promote transport of groundwater and gas, and consequently radionuclide transport. Microbial activity plays an important role in organic degradation, corrosion and gas generation through the mediation of reduction–oxidation reactions.

A large-scale gas generation experiment has been established at the LLW/ILW repository, Olkiluoto, Finland to examine gas generation from LLW in waste drums disposed of in the operational VLJ Repository (VLJ is a Finnish acronym which translates to “reactor operating waste”). The experiment has monitored, for a period of 9 a, the rate and composition of gas generated, and the aqueous geochemistry and microbe populations present at various locations within the experiment. There is considerable heterogeneity within the experiment, such that pH is observed to vary from pH 5.5 to pH 10 between organic-rich waste and water associated with concrete. The heterogeneity results in competing anaerobic processes occurring together in the experiment but within different niches. Microbial activity initially dominant in organic waste has after 7 a reduced the alkalinity of the concrete influenced regions.

The experiment has been modelled using a biogeochemical reaction-transport code (GRM) using a blind testing approach. Using independent data, the model was able to reproduce, within a factor of two, the rate of gas production. In addition, the model represented the main anaerobic microbial processes leading to methanogenesis and the observed spatial and temporal variations in aqueous and gaseous species. In order to model the experiment, its heterogeneity was considered such that individual waste containers were represented and assumptions were made concerning transport rates of chemical species. Cellulose waste and H2 produced by corrosion provide microbial substrates for reduction processes and CH4 generation. However, gas generation is a complex interaction of waste degradation processes. Simple repository gas generation models that consider corrosion and cellulose degradation in isolation will tend to overestimate H2 content and gas generation. The GRM model is more realistic and utilises information concerning SO42-, NO3- and other oxidised species present in LLW/ILW to consider the competition between microbial groups for electron donors that reduce the extent of H2 and CH4 generation. Models such as GRM could be applied to other repository systems, such as for high level waste and spent nuclear fuel, to evaluate how H2 gas generation from corrosion and radiolysis may be affected by microbial activity. However, this will require estimation of appropriate microbial kinetic parameters for these more extreme environments.

Original languageEnglish
Pages (from-to)1383 - 1418
Number of pages36
JournalApplied Geochemistry
Volume23
Issue number6
DOIs
Publication statusPublished - 2008
MoE publication typeA1 Journal article-refereed

Fingerprint

Biogeochemistry
Radioactive Waste
biogeochemistry
Radioactive wastes
gas production
radioactive waste
Gases
repository
gas
modeling
corrosion
Corrosion
degradation
Degradation
microbial activity
experiment
Experiments
Geochemistry
Radioisotopes
Cellulose

Keywords

  • radioactive waste storage
  • radioactive wastes
  • low-level radioactive wastes
  • intermediate-level radioactive wastes
  • deep repository for nuclear fuel
  • repository
  • radionuclide migration
  • radionuclides
  • gas generation
  • organic wastes
  • degradation
  • geochemistry
  • radionuclide transport

Cite this

Small, Joe ; Nykyri, Mikko ; Helin, Mika ; Hovi, Ulla ; Sarlin, Tuija ; Itävaara, Merja. / Experimental and modelling investigations of the biogeochemistry of gas production from low and intermediate level radioactive waste. In: Applied Geochemistry. 2008 ; Vol. 23, No. 6. pp. 1383 - 1418.
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Experimental and modelling investigations of the biogeochemistry of gas production from low and intermediate level radioactive waste. / Small, Joe (Corresponding Author); Nykyri, Mikko; Helin, Mika; Hovi, Ulla; Sarlin, Tuija; Itävaara, Merja.

In: Applied Geochemistry, Vol. 23, No. 6, 2008, p. 1383 - 1418.

Research output: Contribution to journalArticleScientificpeer-review

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T1 - Experimental and modelling investigations of the biogeochemistry of gas production from low and intermediate level radioactive waste

AU - Small, Joe

AU - Nykyri, Mikko

AU - Helin, Mika

AU - Hovi, Ulla

AU - Sarlin, Tuija

AU - Itävaara, Merja

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AB - The degradation of organic wastes and the corrosion of metallic wastes and steel containers in low and intermediate level radioactive waste (LLW/ILW) repositories are important processes that affect repository geochemistry and the speciation and transport of radionuclides. Gas is generated in association with these degradation processes and this has the potential to overpressure the repository, which can promote transport of groundwater and gas, and consequently radionuclide transport. Microbial activity plays an important role in organic degradation, corrosion and gas generation through the mediation of reduction–oxidation reactions.A large-scale gas generation experiment has been established at the LLW/ILW repository, Olkiluoto, Finland to examine gas generation from LLW in waste drums disposed of in the operational VLJ Repository (VLJ is a Finnish acronym which translates to “reactor operating waste”). The experiment has monitored, for a period of 9 a, the rate and composition of gas generated, and the aqueous geochemistry and microbe populations present at various locations within the experiment. There is considerable heterogeneity within the experiment, such that pH is observed to vary from pH 5.5 to pH 10 between organic-rich waste and water associated with concrete. The heterogeneity results in competing anaerobic processes occurring together in the experiment but within different niches. Microbial activity initially dominant in organic waste has after 7 a reduced the alkalinity of the concrete influenced regions.The experiment has been modelled using a biogeochemical reaction-transport code (GRM) using a blind testing approach. Using independent data, the model was able to reproduce, within a factor of two, the rate of gas production. In addition, the model represented the main anaerobic microbial processes leading to methanogenesis and the observed spatial and temporal variations in aqueous and gaseous species. In order to model the experiment, its heterogeneity was considered such that individual waste containers were represented and assumptions were made concerning transport rates of chemical species. Cellulose waste and H2 produced by corrosion provide microbial substrates for reduction processes and CH4 generation. However, gas generation is a complex interaction of waste degradation processes. Simple repository gas generation models that consider corrosion and cellulose degradation in isolation will tend to overestimate H2 content and gas generation. The GRM model is more realistic and utilises information concerning SO42-, NO3- and other oxidised species present in LLW/ILW to consider the competition between microbial groups for electron donors that reduce the extent of H2 and CH4 generation. Models such as GRM could be applied to other repository systems, such as for high level waste and spent nuclear fuel, to evaluate how H2 gas generation from corrosion and radiolysis may be affected by microbial activity. However, this will require estimation of appropriate microbial kinetic parameters for these more extreme environments.

KW - radioactive waste storage

KW - radioactive wastes

KW - low-level radioactive wastes

KW - intermediate-level radioactive wastes

KW - deep repository for nuclear fuel

KW - repository

KW - radionuclide migration

KW - radionuclides

KW - gas generation

KW - organic wastes

KW - degradation

KW - geochemistry

KW - radionuclide transport

U2 - 10.1016/j.apgeochem.2007.11.020

DO - 10.1016/j.apgeochem.2007.11.020

M3 - Article

VL - 23

SP - 1383

EP - 1418

JO - Applied Geochemistry

JF - Applied Geochemistry

SN - 0883-2927

IS - 6

ER -