期刊
ENVIRONMENTAL SCIENCE & TECHNOLOGY
卷 50, 期 7, 页码 3382-3390出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.est.5b05571
关键词
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资金
- U.K. Natural Environment Research Council (NERC) BIGRAD consortium [NE/H007768/1]
- Diamond Light Source [SP9621, SP10163]
- EnvRadNet
- EPSRC [EP/I036389/1]
- EPSRC [EP/I036389/1] Funding Source: UKRI
- NERC [NE/H006494/2, NE/H007768/1, NE/H005617/1] Funding Source: UKRI
- STFC [ST/K001787/1, ST/N002474/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/I036389/1] Funding Source: researchfish
- Natural Environment Research Council [NE/H005617/1, NE/H006494/2, NE/H007768/1] Funding Source: researchfish
- Science and Technology Facilities Council [ST/N002474/1, ST/K001787/1] Funding Source: researchfish
The speciation and fate of neptunium as Np(V)O-2(+) during the crystallization of ferrihydrite to hematite and goethite was explored in a range of systems. Adsorption of NpO2+ to iron(III) (oxyhydr)oxide phases was reversible and, for ferrihydrite, occurred through the formation of mononuclear bidentate surface complexes. By contrast, chemical extractions and X-ray absorption spectroscopy (XAS) analyses showed the incorporation of Np(V) into the structure of hematite during its crystallization from ferrihydrite (pH 10 5) This occurred through direct replacement of octahedrally coordinated Fe(III) by Np(V) in neptunate-like coordination. Subsequent analyses on mixed goethite and hematite crystallization products (pH 9.5 and 11) showed that Np(V) was incorporated during crystallization. Conversely, there was limited evidence for Np(V) incorporation during goethite crystallization at the extreme pH of 13.3. This is likely due to the formation of a Np(V) hydroxide precipitate preventing incorporation into the goethite particles. Overall these data highlight the complex behavior of Np(V) during the crystallization, of iron(III) (oxyhydr)oxides, and demonstrate clear evidence for neptunium incorporation into environmentally important mineral phases. This extends our knowledge of the range of geochemical conditions under which there is potential for long-term immobilization of radiotoxic Np in natural and engineered environments.
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