文章基本信息

标题：Multielectron, multisubstrate molecular catalysis of electrochemical reactions: Formal kinetic analysis in the total catalysis regime
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作者：Cyrille Costentin ; Daniel G. Nocera ; Casey N. Brodsky 等
期刊名称：Proceedings of the National Academy of Sciences
印刷版ISSN：0027-8424
电子版ISSN：1091-6490
出版年度：2017
卷号：114
期号：43
页码：11303-11308
DOI：10.1073/pnas.1711129114
语种：English
出版社：The National Academy of Sciences of the United States of America
摘要：Cyclic voltammetry responses are derived for two-electron, two-step homogeneous electrocatalytic reactions in the total catalysis regime. The models developed provide a framework for extracting kinetic information from cyclic voltammograms (CVs) obtained in conditions under which the substrate or cosubstrate is consumed in a multielectron redox process, as is particularly prevalent for very active catalysts that promote energy conversion reactions. Such determination of rate constants in the total catalysis regime is a prerequisite for the rational benchmarking of molecular electrocatalysts that promote multielectron conversions of small-molecule reactants. The present analysis is illustrated with experimental systems encompassing various limiting behaviors.
关键词：electrochemistry ; total catalysis ; energy conversion ; homogeneous mechanism ; cyclic voltammetry