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Instruments / Technical Area	Publication Details	Published	Actions
B18-Core EXAFS I20-Scanning-X-ray spectroscopy (XAS/XES)	Sulfidation and reoxidation of U(VI)-incorporated goethite: implications for U retention during sub-surface redox cycling Olwen Stagg , Katherine Morris , Luke T. Townsend , Kristina O. Kvashnina , Michael L. Baker , Ryan L. Dempsey , Liam Abrahamsen-Mills , Samuel Shaw Environmental Science & Technology 2 DOI: 10.1021/acs.est.2c05314 Diamond Proposal Number(s): [21441, 24074] Open Access Show Abstract ▼ Abstract: Over 60 years of nuclear activity have resulted in a global legacy of contaminated land and radioactive waste. Uranium (U) is a significant component of this legacy and is present in radioactive wastes and at many contaminated sites. U-incorporated iron (oxyhydr)oxides may provide a long-term barrier to U migration in the environment. However, reductive dissolution of iron (oxyhydr)oxides can occur on reaction with aqueous sulfide (sulfidation), a common environmental species, due to the microbial reduction of sulfate. In this work, U(VI)–goethite was initially reacted with aqueous sulfide, followed by a reoxidation reaction, to further understand the long-term fate of U species under fluctuating environmental conditions. Over the first day of sulfidation, a transient release of aqueous U was observed, likely due to intermediate uranyl(VI)–persulfide species. Despite this, overall U was retained in the solid phase, with the formation of nanocrystalline U(IV)O2 in the sulfidized system along with a persistent U(V) component. On reoxidation, U was associated with an iron (oxyhydr)oxide phase either as an adsorbed uranyl (approximately 65%) or an incorporated U (35%) species. These findings support the overarching concept of iron (oxyhydr)oxides acting as a barrier to U migration in the environment, even under fluctuating redox conditions.	Nov 2022

Instruments / Technical Area

Publication Details

Published

Actions

B18-Core EXAFS
I20-Scanning-X-ray spectroscopy (XAS/XES)

Sulfidation and reoxidation of U(VI)-incorporated goethite: implications for U retention during sub-surface redox cycling

Olwen Stagg , Katherine Morris , Luke T. Townsend , Kristina O. Kvashnina , Michael L. Baker , Ryan L. Dempsey , Liam Abrahamsen-Mills , Samuel Shaw

Environmental Science & Technology 2

DOI: 10.1021/acs.est.2c05314

Diamond Proposal Number(s): [21441, 24074]