Universitat Autònoma de Barcelona
Altres ajuts: CERCA Programme/Generalitat de Catalunya
The presence of single-electron transfer (SET) steps in water oxidation processes catalyzed by first-row transition metal complexes has been recently recognized, but the computational characterization of this type of process is not trivial. We report a systematic theoretical study based on density functional theory (DFT) calculations on the reactivity of a specific copper complex active in water oxidation that reacts through two consecutive single-electron transfers. Both inner-sphere (through transition state location) and outer-sphere (through Marcus theory) mechanisms are analyzed. The first electron transfer is found to operate through outer-sphere, and the second one through inner-sphere. The current work proposes a scheme for the systematic study of single-electron transfer in water oxidation catalysis and beyond.
English
Marcus theory; DFT; Single-electron transfer; Water oxidation; Mechanisms
Ministerio de Economía y Competitividad CTQ2017-87792-R
Ministerio de Economía y Competitividad BES-2015-073012
Ministerio de Economía y Competitividad SVP-2014-068662
Inorganics ; Vol. 7, Issue 3 (March 2019), art. 32
open access
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