期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 140, 期 51, 页码 17977-17984出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.8b09436
关键词
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资金
- National Nuclear Security Administration of the U.S. Department of Energy [DE-AC52-06NA25396]
- Glenn T. Seaborg Institute
- distinguished Darleane Christian Hoffman Fellowship
- LANL Directors Post -Doctoral Fellowship
- Agnew National Security Fellowship
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
- Heavy Element Chemistry Program by the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy
- U.S. Department of Energy
- [DE-AC02-05CH11231]
Evaluating the nature of chemical bonding for actinide elements represents one of the most important and long-standing problems in actinide science. We directly address this challenge and contribute a Cl K-edge X-ray absorption spectroscopy and relativistic density functional theory study that quantitatively evaluates An-Cl covalency in AnCl(6)(2-)(An(IV) = Th, U, Np, Pu). The results showed significant mixing between Cl 3p- and An(IV) 5f- and 6d-orbitals (t(1u)*/t(2u)* and t(2g)*/e(g)*), with the 6d-orbitals showing more pronounced covalent bonding than the 5f-orbitals. Moving from Th to U, Np, and Pu markedly changed the amount of M-Cl orbital mixing, such that An(IV) 6d- and Cl 3p-mixing decreased and metal 5f- and Cl 3p-orbital mixing increased across this series.
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