Phosphate-Induced Immobilization of Uranium in Hanford Sediments

Pan, Zezhen; Giammar, Daniel E.; Mehta, Vrajesh; Troyer, Lyndsay D.; Catalano, Jeffrey G.; Wang, Zheming

doi:10.1021/acs.est.6b02928

Phosphate-Induced Immobilization of Uranium in Hanford Sediments

Journal Article · Tue Nov 29 00:00:00 EST 2016 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.6b02928· OSTI ID:1346213

Pan, Zezhen ^[1]; ^[1]; Mehta, Vrajesh ^[1]; Troyer, Lyndsay D. ^[1]; ^[1]; Wang, Zheming ^[2]

Washington Univ., St. Louis, MO (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Phosphate can be added to subsurface environments to immobilize U(VI) contamination. The efficacy of immobilization depends on the site-specific groundwater chemistry and aquifer sediment properties. Batch and column experiments were performed with sediments from the Hanford 300 Area in Washington State and artificial groundwater prepared to emulate the conditions at the site. Batch experiments revealed enhanced U(VI) sorption with increasing phosphate addition. X-ray absorption spectroscopy measurements of samples from the batch experiments found that U(VI) was predominantly adsorbed at conditions relevant to the column experiments and most field sites (low U(VI) loadings, <25 μM), and U(VI) phosphate precipitation occurred only at high initial U(VI) (>25 μM) and phosphate loadings. While batch experiments showed the transition of U(VI) uptake from adsorption to precipitation, the column study was more directly relevant to the subsurface environment because of the high solid:water ratio in the column and the advective flow of water. In column experiments, nearly six times more U(VI) was retained in sediments when phosphate-containing groundwater was introduced to U(VI)-loaded sediments than when the groundwater did not contain phosphate. This enhanced retention persisted for at least one month after cessation of phosphate addition to the influent fluid. Sequential extractions and laser-induced fluorescence spectroscopy of sediments from the columns suggested that the retained U(VI) was primarily in adsorbed forms. Here, these results indicate that in situ remediation of groundwater by phosphate addition provides lasting benefit beyond the treatment period via enhanced U(VI) adsorption to sediments.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: AC02-06CH11357; AC05-76RL01830; SC0006857

OSTI ID:: 1346213

Alternate ID(s):: OSTI ID: 1755205
OSTI ID: 1358519

Report Number(s):: PNNL-SA--121196

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 24 Vol. 50; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: ENGLISH

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