Benchmarking of homogeneous electrocatalysts: overpotential, turnover frequency, limiting turnover number

Journal of the American Chemical Society
Cyrille CostentinJean-Michel Savéant

Abstract

In relation to contemporary energy challenges, a number of molecular catalysts for the activation of small molecules, mainly based on transition metal complexes, have been developed. The time has thus come to develop tools allowing the benchmarking of these numerous catalysts. Two main factors of merit are addressed. One involves their intrinsic catalytic performances through the comparison of "catalytic Tafel plots" relating the turnover frequency to the overpotential independently of the characteristics of the electrochemical cell. The other examines the effect of deactivation of the catalyst during the course of electrolysis. It introduces the notion of the limiting turnover number as a second key element of catalyst benchmarking. How these two factors combine with one another to control the course of electrolysis is analyzed in detail, leading to procedures that allow their separate estimation from measurements of the current, the charge passed, and the decay of the catalyst concentration. Illustrative examples from literature data are discussed.

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Citations

Sep 29, 2015·Journal of the American Chemical Society·Cyrille CostentinJean-Michel Savéant
Sep 26, 2015·Inorganic Chemistry·Travis A WhiteClaudia Turro
Jun 30, 2016·Chemical Reviews·David SchilterThomas B Rauchfuss
Jan 20, 2017·Journal of the American Chemical Society·Amanda N OldacreTimothy R Cook
Jan 25, 2017·Journal of the American Chemical Society·Ken T NgoJonathan Rochford
Feb 9, 2017·Chemistry : a European Journal·R Morris BullockAaron M Appel
May 23, 2017·ACS Applied Materials & Interfaces·Cyrille Costentin, Jean-Michel Savéant
Dec 25, 2016·Chemistry : a European Journal·Santanu PattanayakSayam Sen Gupta
Jun 2, 2017·Chemical Science·Lianpeng Tong, Randolph P Thummel
Mar 20, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Indresh Kumar PandeySandeep Kaur-Ghumaan
Aug 21, 2018·Advanced Materials·Mu XiaoLianzhou Wang
Mar 9, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Elodie Anxolabéhère-MallartMarc Robert
Apr 26, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Changcheng JiangCharles W Machan
Sep 29, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Camille R SchneiderHannah S Shafaat
Feb 28, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·James D ShippJulia A Weinstein
Jul 1, 2020·Physical Chemistry Chemical Physics : PCCP·Andrea FioraniYasuaki Einaga
Aug 26, 2018·Proceedings of the National Academy of Sciences of the United States of America·Cyrille CostentinCédric Tard
Jun 6, 2020·Coordination Chemistry Reviews·Brian D McCarthySascha Ott
Apr 16, 2021·Journal of the American Chemical Society·Weiwei GuoBuxing Han
Feb 7, 2018·Chemical Reviews·Michael L PegisJames M Mayer
Jun 19, 2015·Journal of the American Chemical Society·Charles W MachanClifford P Kubiak
May 4, 2017·Journal of the American Chemical Society·Cyrille Costentin, Jean-Michel Savéant
Sep 16, 2021·Angewandte Chemie·Sengeni AnantharajSuguru Noda

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