Abstract:Abstract-Citric acid is found along with uranyl in the subsurface of former nuclear facilities because of its use as a decontamination agent in the nuclear industry. Citrate's metal chelating properties affect the mobility of uranyl in the subsurface and consequently, citrate biodegradation may significantly impact uranyl fate and transport. Under the non-growth conditions considered, low (micromolar) uranyl concentrations inhibit the biodegradation of citrate by Pseudomonas fluorescens, a common subsurface de… Show more
“…4) would provide a source of high-affinity U(IV)-binding phosphate sites (52). Phosphate is also released from cell lysis and can precipitate with uranium (14,53). The intimate association of biomass and mackinawite (Fig.…”
Redox transitions of uranium [from U(VI) to U(IV)] in low-temperature sediments govern the mobility of uranium in the environment and the accumulation of uranium in ore bodies, and inform our understanding of Earth's geochemical history. The molecular-scale mechanistic pathways of these transitions determine the U(IV) products formed, thus influencing uranium isotope fractionation, reoxidation, and transport in sediments. Studies that improve our understanding of these pathways have the potential to substantially advance process understanding across a number of earth sciences disciplines. Detailed mechanistic information regarding uranium redox transitions in field sediments is largely nonexistent, owing to the difficulty of directly observing molecular-scale processes in the subsurface and the compositional/physical complexity of subsurface systems. Here, we present results from an in situ study of uranium redox transitions occurring in aquifer sediments under sulfate-reducing conditions. Based on molecular-scale spectroscopic, pore-scale geochemical, and macroscale aqueous evidence, we propose a biotic-abiotic transition pathway in which biomass-hosted mackinawite (FeS) is an electron source to reduce U(VI) to U(IV), which subsequently reacts with biomass to produce monomeric U(IV) species. A species resembling nanoscale uraninite is also present, implying the operation of at least two redox transition pathways. The presence of multiple pathways in low-temperature sediments unifies apparently contrasting prior observations and helps to explain sustained uranium reduction under disparate biogeochemical conditions. These findings have direct implications for our understanding of uranium bioremediation, ore formation, and global geochemical processes. metal reduction | roll front | sulfate reduction | sulfide | bioreduction
“…4) would provide a source of high-affinity U(IV)-binding phosphate sites (52). Phosphate is also released from cell lysis and can precipitate with uranium (14,53). The intimate association of biomass and mackinawite (Fig.…”
Redox transitions of uranium [from U(VI) to U(IV)] in low-temperature sediments govern the mobility of uranium in the environment and the accumulation of uranium in ore bodies, and inform our understanding of Earth's geochemical history. The molecular-scale mechanistic pathways of these transitions determine the U(IV) products formed, thus influencing uranium isotope fractionation, reoxidation, and transport in sediments. Studies that improve our understanding of these pathways have the potential to substantially advance process understanding across a number of earth sciences disciplines. Detailed mechanistic information regarding uranium redox transitions in field sediments is largely nonexistent, owing to the difficulty of directly observing molecular-scale processes in the subsurface and the compositional/physical complexity of subsurface systems. Here, we present results from an in situ study of uranium redox transitions occurring in aquifer sediments under sulfate-reducing conditions. Based on molecular-scale spectroscopic, pore-scale geochemical, and macroscale aqueous evidence, we propose a biotic-abiotic transition pathway in which biomass-hosted mackinawite (FeS) is an electron source to reduce U(VI) to U(IV), which subsequently reacts with biomass to produce monomeric U(IV) species. A species resembling nanoscale uraninite is also present, implying the operation of at least two redox transition pathways. The presence of multiple pathways in low-temperature sediments unifies apparently contrasting prior observations and helps to explain sustained uranium reduction under disparate biogeochemical conditions. These findings have direct implications for our understanding of uranium bioremediation, ore formation, and global geochemical processes. metal reduction | roll front | sulfate reduction | sulfide | bioreduction
“…Soares et al (2002) reported that S. cerevisiae NCNY 1190 releases P when it is exposed to Cd, Cu, and Pb. This release is attributed to uranium or heavy-metal toxicity (Soares et al, 2002;Bencheikh-Latmani and Leckie, 2003). Heavy metals induce lesions of the cell membrane of S. cerevisiae (Joho et al, 1984;Ohsumi et al, 1988), which may cause the cell to rupture.…”
Section: Accumulation Mechanisms Of U(vi) By Yeast S Cerevisiaementioning
“…However, no study is known concerning metaautunite formation due to uranium interaction with P. fluorescens strains. To our knowledge, only a few studies provided uranium sorption experiments using P. fluorescens strains (Krueger et al 1993;Bencheikh-Latmani and Leckie 2003;Francis et al 2004;Lütke et al 2012). These studies showed that the strain mainly accumulates uranium on the cell surface, where uranium is bound via protonated phosphoryl and carboxylic sites.…”
Section: Discussionmentioning
confidence: 99%
“…Krueger et al (1993) showed that the strain mainly accumulates uranium on the cell surface. In Bencheikh-Latmani and Leckie (2003), most of the uranyl is also associated with the outside of the cell. Similar results have been obtained by Francis et al (2004), where P. fluorescens was found to accumulate uranium in the periplasm along its plasma and outer membranes as fine-grained, platy uranium-crystals.…”
The interaction between the Pseudomonas fluorescens biofilm and U(VI) were studied using extended X-ray absorption fine structure spectroscopy (EXAFS), and time-resolved laser fluorescence spectroscopy (TRLFS). In EXAFS studies, the formation of a stable uranyl phosphate mineral, similar to autunite (Ca[UO2]2[PO4]2•2-6H2O) or meta-autunite (Ca[UO2]2[PO4]2•10-12H2O) was observed. This is the first time such a biomineralization process has been observed in P. fluorescens. Biomineralization occurs due to phosphate release from the cellular polyphosphate, likely as a cell's response to the added uranium. It differs significantly from the biosorption process occurring in the planktonic cells of the same strain. TRLFS studies of the uranium-contaminated nutrient medium identified aqueous Ca2UO2(CO3)3 and UO2(CO3)3 (4-) species, which in contrast to the biomineralization in the P. fluorescens biofilm, may contribute to the transport and migration of U(VI). The obtained results reveal that biofilms of P. fluorescens may play an important role in predicting the transport behavior of uranium in the environment. They will also contribute to the improvement of remediation methods in uranium-contaminated sites.
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