期刊
ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 51, 期 24, 页码 14301-14310出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.7b02426
关键词
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资金
- UK EPSRC
- NERC LO-RISE consortium part of the NERC RATE [NE/L000547/1]
- NERC BIGRAD consortium [NE/H007768/1]
- Environment Agency and Radioactive Waste Management Ltd.
- NERC [NE/L000547/1, NE/H007768/1, NE/H005617/1, NE/L000253/2, NE/L00027X/1] Funding Source: UKRI
- STFC [ST/K001787/1, ST/K001752/1, ST/N002474/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [1231554] Funding Source: researchfish
- Natural Environment Research Council [NE/H005617/1, NE/L000253/2, NE/L00027X/1, NE/H007768/1, NE/L000547/1] Funding Source: researchfish
- Science and Technology Facilities Council [ST/N002474/1, ST/K001752/1, ST/K001787/1] Funding Source: researchfish
Technetium is a problematic contaminant at nuclear sites and little is known about how repeated microbiologically mediated redox cycling impacts its fate in the environment. We explore this question in sediments representative of the Seafield Ltd. site, UK, over multiple reduction and oxidation cycles spanning, similar to 1.5 years. We found the amount of Tc remobilised from the sediment into solution significantly decreased after repeated redox cycles. X-ray Absorption Spectroscopy (XAS) confirmed that sediment bound Tc was present as hydrous TcO2-like chains throughout experimentation and that Tc's increased resistance to remobilization (via reoxidation to soluble TcO4-) resulted from both shortening of TcO2 chains during redo): cycling and association of Tc(IV) with Fe phases in the sediment. We also observed that Tc(W) remaining in solution during bioreduction was likely associated with colloidal magnetite nanoparticles. These findings highlight crucial links between Tc and Fe biogeochemical cycles that have significant implications for Tc's long-term environmental mobility, especially under ephemeral redox conditions.
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