Control of cerium oxidation state through metal complex secondary structures
Abstract
A series of alkali metal cerium diphenylhydrazido complexes, Mx(py)y[Ce(PhNNPh)4], M = Li, Na, and K, x = 4 (Li and Na) or 5 (K), and y = 4 (Li), 8 (Na), or 7 (K), were synthesized to probe how a secondary coordination sphere would modulate electronic structures at a cerium cation. The resulting electronic structures of the heterobimetallic cerium diphenylhydrazido complexes were found to be strongly dependent on the identity of the alkali metal cations. When M = Li+ or Na+, the cerium(III) starting material was oxidized with concomitant reduction of 1,2-diphenylhydrazine to aniline. Reduction of 1,2-diphenylhydrazine was not observed when M = K+, and the complex remained in the cerium(III) oxidation state. Oxidation of the cerium(III) diphenylhydrazido complex to the Ce(IV) diphenylhydrazido one was achieved through a simple cation exchange reaction of the alkali metals. As a result, UV-Vis spectroscopy, FTIR spectroscopy, electrochemistry, magnetic susceptibility, and DFT studies were used to probe the oxidation state and the electronic changes that occurred at the metal centre.
- Authors:
-
- Univ. of Pennsylvania, Philadelphia, PA (United States)
- Publication Date:
- Research Org.:
- Univ. of Pennsylvania, Philadelphia, PA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- Contributing Org.:
- National Science Foundation (NSF), Washington, DC (United States)
- OSTI Identifier:
- 1221895
- Grant/Contract Number:
- SC0006518
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemical Science
- Additional Journal Information:
- Journal Name: Chemical Science; Journal ID: ISSN 2041-6520
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Levin, Jessica R., Dorfner, Walter L., Carroll, Patrick J., and Schelter, Eric J. Control of cerium oxidation state through metal complex secondary structures. United States: N. p., 2015.
Web. doi:10.1039/C5SC02607E.
Levin, Jessica R., Dorfner, Walter L., Carroll, Patrick J., & Schelter, Eric J. Control of cerium oxidation state through metal complex secondary structures. United States. https://doi.org/10.1039/C5SC02607E
Levin, Jessica R., Dorfner, Walter L., Carroll, Patrick J., and Schelter, Eric J. Tue .
"Control of cerium oxidation state through metal complex secondary structures". United States. https://doi.org/10.1039/C5SC02607E. https://www.osti.gov/servlets/purl/1221895.
@article{osti_1221895,
title = {Control of cerium oxidation state through metal complex secondary structures},
author = {Levin, Jessica R. and Dorfner, Walter L. and Carroll, Patrick J. and Schelter, Eric J.},
abstractNote = {A series of alkali metal cerium diphenylhydrazido complexes, Mx(py)y[Ce(PhNNPh)4], M = Li, Na, and K, x = 4 (Li and Na) or 5 (K), and y = 4 (Li), 8 (Na), or 7 (K), were synthesized to probe how a secondary coordination sphere would modulate electronic structures at a cerium cation. The resulting electronic structures of the heterobimetallic cerium diphenylhydrazido complexes were found to be strongly dependent on the identity of the alkali metal cations. When M = Li+ or Na+, the cerium(III) starting material was oxidized with concomitant reduction of 1,2-diphenylhydrazine to aniline. Reduction of 1,2-diphenylhydrazine was not observed when M = K+, and the complex remained in the cerium(III) oxidation state. Oxidation of the cerium(III) diphenylhydrazido complex to the Ce(IV) diphenylhydrazido one was achieved through a simple cation exchange reaction of the alkali metals. As a result, UV-Vis spectroscopy, FTIR spectroscopy, electrochemistry, magnetic susceptibility, and DFT studies were used to probe the oxidation state and the electronic changes that occurred at the metal centre.},
doi = {10.1039/C5SC02607E},
journal = {Chemical Science},
number = ,
volume = ,
place = {United States},
year = {Tue Aug 11 00:00:00 EDT 2015},
month = {Tue Aug 11 00:00:00 EDT 2015}
}
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Fig. 1: 30% probability thermal ellipsoid plots of Li4(py)4[Ce(PhNNPh)4] (1) (left), Na4(py)8[Ce(PhNNPh)4] (2) (middle), and K5(py)7[Ce(PhNNPh)4] (3) (right) with the phenyl and pyridine rings shown in wire frame. Hydrogen atoms were omitted for clarity. Selected bond distances for 1 (Å): Ce(1)– N(1) 2.4408(13), Ce(1)–N(2) 2.4199(13), N(1)–N(2) 1.451(2), Li(2)–N(1) 2.018(3), Li(2)–N(10)more »
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Reduction of a Cerium(III) Siloxide Complex To Afford a Quadruple-Decker Arene-Bridged Cerium(II) Sandwich
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