Abstract
© 2019 by the authors. 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.
Original language | English |
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Article number | 32 |
Journal | Inorganics |
Volume | 7 |
DOIs | |
Publication status | Published - 1 Jan 2019 |
Keywords
- DFT
- Marcus theory
- Mechanisms
- Single-electron transfer
- Water oxidation