Contaminant release, mixing and microbial fluctuations initiated by infiltrating water within a replica field-scale legacy radioactive waste trench

SCIENCE OF THE TOTAL ENVIRONMENT(2022)

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摘要
Numerous legacy near-surface radioactive waste sites dating from the mid 20th century have yet to be remediated and present a global contamination concern. Typically, there is insufficient understanding of contaminant release and re-distribution, with invasive investigations often impractical due to the risk of disturbing the often significantly radiotoxic contaminants. Consequently, a replica waste trench (-5.4 m3), constructed adjacent to a legacy radioactive waste site (Little Forest Legacy Site, LFLS), was used to assist our understanding of the release and mixing processes of neodymium (Nd) - a chemical analogue for plutonium(III) and americium(III), two significant radionuclides in many contaminated environments. In order to clarify the behaviour of contaminants released from buried objects such as waste containers, a steel drum, representative of the hundreds of buried drums within the LFLS, was placed within the trench. Dissolved neodymium nitrate was introduced as a point-source contaminant to the base of the trench, outside the steel drum. Hydrologic conditions were manipulated to simulate natural rainfall intensities with dissolved lithium bromide added as a tracer. Neodymium was primarily retained both at its point of release at the bottom of the trench (> 97 %) as well as at a steel container corrosion point, simulated through the emplacement of steel wool. How-ever, over the 8-month field experiment, advective mixing initiated by surface water intrusions rapidly redistributed a small proportion of Nd to shallower waters (-1.5-1.7 %), as well as throughout the buried steel drum. Suspended par-ticulate forms of Nd (> 0.2 mu m) were measured at all depths in the suboxic trench and were persistent across the entire study. Analyses of the microbial communities showed that their relative abundances and metabolic functions were strongly influenced by the prevailing geochemical conditions as a result of fluctuating water depths associated with rainfall events. The site representing steel corrosion exhibited divergent biogeochemical results with anomalous changes (sharp decrease) observed in both dissolved contaminant concentration as well as microbial diversity and functionality. This research demonstrates that experimental trenches provide a safe and unique method for simulating the behaviour of subsurface radioactive contaminants with results demonstrating the initial retention, partial shallow water redistribution, and stability of particulate form(s) of this radioactive analogue. These results have relevance for appropriate management and remediation strategies for the adjacent legacy site as well as for similar sites across the globe.
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关键词
Contaminated site,Field experiment,Analogue,Neodymium,Bromide
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