TY - JOUR
T1 - Biomineralization of uranium-phosphates fueled by microbial degradation of isosaccharinic acid (ISA)
AU - Kuippers, Gina
AU - Morris, Katherine
AU - Townsend, Luke
AU - Bots, Pieter
AU - Kvashnina, Kristina
AU - Bryan, Nicholas D
AU - Lloyd, Jonathan
PY - 2021/4/20
Y1 - 2021/4/20
N2 - Geological disposal is the globally preferred long-term solution for higher activity radioactive wastes (HAW) including Intermediate Level Waste (ILW). In a cementitious disposal system, cellulosic waste items present in ILW may undergo alkaline hydrolysis, producing significant quantities of isosaccharinic acid (ISA), a chelating agent for radionuclides. Although microbial degradation of ISA has been demonstrated, its impact upon the fate of radionuclides in a geological disposal facility (GDF) is a topic of ongoing research. This study investigates the fate of U(VI) in pH-neutral, anoxic, microbial enrichment cultures, approaching conditions similar to the far field of a GDF, containing ISA as the sole carbon source, and elevated phosphate concentrations, incubated both (i) under fermentation and (ii) Fe(III)- reducing conditions. In the ISA-fermentation experiment, U(VI) was precipitated as insoluble U(VI)-phosphates, whereas under Fe(III)-reducing conditions, the majority of the uranium was precipitated as reduced U(IV)-phosphates, presumably formed via enzymatic reduction mediated by metal-reducing bacteria, including Geobacter species. Overall, this suggests the establishment of a microbially-mediated “bio- barrier” extending into the far field geosphere surrounding a GDF is possible and this bio-barrier has the potential to evolve in response to GDF evolution and can have a controlling impact on the fate of radionuclides.
AB - Geological disposal is the globally preferred long-term solution for higher activity radioactive wastes (HAW) including Intermediate Level Waste (ILW). In a cementitious disposal system, cellulosic waste items present in ILW may undergo alkaline hydrolysis, producing significant quantities of isosaccharinic acid (ISA), a chelating agent for radionuclides. Although microbial degradation of ISA has been demonstrated, its impact upon the fate of radionuclides in a geological disposal facility (GDF) is a topic of ongoing research. This study investigates the fate of U(VI) in pH-neutral, anoxic, microbial enrichment cultures, approaching conditions similar to the far field of a GDF, containing ISA as the sole carbon source, and elevated phosphate concentrations, incubated both (i) under fermentation and (ii) Fe(III)- reducing conditions. In the ISA-fermentation experiment, U(VI) was precipitated as insoluble U(VI)-phosphates, whereas under Fe(III)-reducing conditions, the majority of the uranium was precipitated as reduced U(IV)-phosphates, presumably formed via enzymatic reduction mediated by metal-reducing bacteria, including Geobacter species. Overall, this suggests the establishment of a microbially-mediated “bio- barrier” extending into the far field geosphere surrounding a GDF is possible and this bio-barrier has the potential to evolve in response to GDF evolution and can have a controlling impact on the fate of radionuclides.
U2 - 10.1021/acs.est.0c03594
DO - 10.1021/acs.est.0c03594
M3 - Article
SN - 0013-936X
VL - 55
JO - Environmental Science & Technology
JF - Environmental Science & Technology
IS - 8
M1 - 4597–4606
ER -