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Issue 28, 2019
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Proton-coupled multi-electron transfer and its relevance for artificial photosynthesis and photoredox catalysis

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Abstract

The conversion of CO2, H2O, or N2 to energy-rich compounds such as CH3OH, H2 or NH3 requires the properly orchestrated transfer of multiple electrons and protons. Artificial photosynthetic systems therefore must be able to synchronize the rapid primary photoinduced transfer of single electrons to the slower catalytic (multi-electron) turnover of substrates, and this generates a need for temporary accumulation and storage of redox equivalents. This is a very difficult task, particularly in absence of sacrificial reagents. Toward this end, proton-coupled multi-electron transfer (PCMET) driven by light is now receiving increased attention. This invited Feature article considers recent pertinent studies of donor–sensitizer–acceptor compounds and inorganic–organic hybrid systems, as well as some recent photoredox catalysis studies of proton-coupled multi-electron reductions. Key principles for successful light-driven accumulation and storage of redox equivalents are discussed, and the relevance of PCMET for the formation of solar fuels and for photoredox catalysis is emphasized.

Graphical abstract: Proton-coupled multi-electron transfer and its relevance for artificial photosynthesis and photoredox catalysis

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Article information


Submitted
29 Jan 2019
Accepted
20 Feb 2019
First published
27 Feb 2019

This article is Open Access

Chem. Commun., 2019,55, 4004-4014
Article type
Feature Article

Proton-coupled multi-electron transfer and its relevance for artificial photosynthesis and photoredox catalysis

A. Pannwitz and O. S. Wenger, Chem. Commun., 2019, 55, 4004 DOI: 10.1039/C9CC00821G

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