期刊
INORGANIC CHEMISTRY
卷 52, 期 16, 页码 9487-9495出版社
AMER CHEMICAL SOC
DOI: 10.1021/ic401143g
关键词
-
资金
- Office of Basic Energy Sciences of the U.S. Department of Energy as part of the Materials Science of Actinides Energy Frontier Research Center [DE-SC0001089]
Three uranium(VI)-bearing materials were synthesized hydrothermally using the organic ligand 4,4'-biphenyldicarboxylic acid: (UO2)(C14O4H8) (1); [(UO2)(2)(C14O4H8)(2)(OH)]center dot(NH4)(H2O) (2); (UO2)(2)(C14O4H8)(OH)(2) (3). Compound 1 was formed after 1 day at 180 C in an acidic environment (pH(i) = 4.03), and compounds 2 and 3 coformed after 3 days under basic conditions (pH(i) = 7.95). Coformation of all three compounds was observed at higher pH(i) (9.00). Ex situ Raman spectra of single crystals of 1-3 were collected and analyzed for signature peaks. In situ hydrothermal Raman data were also obtained and compared to the ex situ Raman spectra of the title compounds in an effort to acquire formation mechanism details. At pH(i) = 4.00, the formation of 1 was suggested by in situ Raman spectra. At an increased pH(i) (7.90), the in situ data implied the formation of compounds 1 and 3. The most basic conditions (pH(i) = 9.00) yielded a complex mixture of phases consistent with that of increased uranyl hydrolysis.
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