期刊
ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 46, 期 17, 页码 9428-9436出版社
AMER CHEMICAL SOC
DOI: 10.1021/es3015502
关键词
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资金
- DoE-OBES Geosciences and Chemical Sciences
- U.S. DOE, Office of Biological and Environmental Research (BER), Subsurface Biogeochemistry program [WP 10094]
- DOE Office of Basic Energy Sciences
- DOE-BER
- NIH, National Institute of General Medical Sciences [41GM103393]
- National Center for Research Resources [P41RR001209]
U(VI) doped hematite was synthesized and exposed to two different organic reductants with E-0 of 0.23 and 0.70 V. A combination of HAADF-TEM and EXAFS provided evidence that uranium was incorporated in hematite in uranate, likely octahedral coordination. XPS indicated that structurally incorporated U(VI) was reduced to U(V), whereas non-incorporated U(VI) was reduced to U(IV). Specifically, the experiments indicate that U(V) was the dominant oxidation state of uranium in hematite around Eh -0.24 to -0.28 V and pH 7.7-8.6 for at least up to 5 weeks of reaction time. U(V), but not U(IV), was also detected in hematite at Eh +0.21 V (pH 7.1-7.3). The results support the hypothesis, based on previous experimental and theoretical work, that the stability field of U(V) is widened relative to U(IV) and U(VI) in uranate coordination environments where the coordination number of U is less than 8.
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