Proton-coupled electron transfer chemistry of hangman macrocycles: Hydrogen and oxygen evolution reactions

被引:38
|
作者
Dogutan, Dilek K. [1 ]
Bediako, D. Kwabena [1 ]
Graham, Daniel J. [1 ]
Lemon, Christopher M. [1 ]
Nocera, Daniel G. [1 ]
机构
[1] Harvard Univ, Dept Chem & Chem Biol, Cambridge, MA 02138 USA
基金
美国国家科学基金会;
关键词
porphyrin; corrole; catalyst; hangman effect; proton-coupled electron transfer (PCET); hydrogen evolution; oxygen evolution; renewable; solar fuels; ELECTROCATALYTIC REDUCTION; ELECTROCHEMICAL REDUCTION; PEROXIDE DISMUTATION; EFFICIENT SYNTHESIS; WATER OXIDATION; H-2; PRODUCTION; CORROLES; PORPHYRINS; COMPLEXES; CATALYSTS;
D O I
10.1142/S1088424614501016
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The splitting of water into its constituent elements is an important solar fuels conversion reaction for the storage of renewable energy. For each of the half reactions of the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), multiple protons and electrons must be coupled to avoid high-energy intermediates. To understand the mechanistic details of the PCET chemistry that underpins HER and OER, we have designed hangman porphyrin and corrole catalysts. In these hangman constructs, a pendant acid/base functionality within the secondary coordination sphere is "hung" above the macrocyclic redox platform on which substrate binds. The two critical thermodynamic properties of a PCET event, the redox potential and pK(a) may be tuned with the macrocycle and hanging group, respectively. This review outlines the synthesis of these catalysts, as well as the examination of the PCET kinetics of hydrogen and oxygen evolution by the hangman catalysts. The insights provided by these systems provide a guide for the design of future HER and OER catalysts that use a secondary coordination sphere to manage PCET.
引用
收藏
页码:1 / 8
页数:8
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