期刊
INORGANIC CHEMISTRY
卷 54, 期 6, 页码 2830-2837出版社
AMER CHEMICAL SOC
DOI: 10.1021/ic503000z
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资金
- U.S. Department of Energy, Office of Science, Early Career Research Program [DE-SC0006518]
- Research Corporation for Science Advancement
- University of Pennsylvania
- National Science Foundation [OCI-1053575]
- Office of Science (OS), Office of Basic Energy Sciences, of the U.S. Department of Energy (DOE) [DE-AC02-05CH11231]
Understanding of the sensitivity of the red-action potential of Cerium(IV) cations to ligand field, strength has yet to benefit from systematic variation of the ligand environment. Detailed analyses for a series of seven cerium(W) tetralds(pyridyl-nitroxide) compounds and their cerium(III) analogues in varying ligand field Strengths are presented. Electrochemical, spectroscopic, and computational results reveal a dose correlation of electronic properties with ligand substituents. Together with electrochernical data for reported eight-coordinate compounds, DET calculations reveal a broad range of the cerium(IV/III) redox potentials correlated to ligand field strengths, establishing a semiempirical, predictive model for the modulation of cerium redox thermodynamics and ligand field strengths. Applications over a variety of scientific disciplines make use of the fundamental redox thermodynamics of cerium. Such applications will benefit from a combined experimental and theoretical approach for assessing redox cycling of cerium compounds.
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