Heterogeneous Molecular Catalysis of Electrochemical Reactions: Volcano Plots and Catalytic Tafel Plots

ACS Applied Materials & Interfaces
Cyrille Costentin, Jean-Michel Savéant

Abstract

We analyze here, in the framework of heterogeneous molecular catalysis, the reasons for the occurrence or nonoccurrence of volcanoes upon plotting the kinetics of the catalytic reaction versus the stabilization free energy of the primary intermediate of the catalytic process. As in the case of homogeneous molecular catalysis or catalysis by surface-active metallic sites, a strong motivation of such studies relates to modern energy challenges, particularly those involving small molecules, such as water, hydrogen, oxygen, proton, and carbon dioxide. This motivation is particularly pertinent for what concerns heterogeneous molecular catalysis, since it is commonly preferred to homogeneous molecular catalysis by the same molecules if only for chemical separation purposes and electrolytic cell architecture. As with the two other catalysis modes, the main drawback of the volcano plot approach is the basic assumption that the kinetic responses depend on a single descriptor, viz., the stabilization free energy of the primary intermediate. More comprehensive approaches, investigating the responses to the maximal number of experimental factors, and conveniently expressed as catalytic Tafel plots, should clearly be preferred. This is more...Continue Reading

References

Oct 18, 2006·Proceedings of the National Academy of Sciences of the United States of America·Nathan S Lewis, Daniel G Nocera
Sep 25, 2009·Inorganic Chemistry·Daniel G Nocera
Apr 1, 2009·Nature Chemistry·Harry B Gray
Aug 17, 2012·Nature·Steven Chu, Arun Majumdar
Nov 21, 2012·Chemical Society Reviews·Vincent Artero, Marc Fontecave
Jul 6, 2014·Beilstein Journal of Nanotechnology·Paola QuainoWolfgang Schmickler
Mar 11, 2015·Journal of the American Chemical Society·Cyrille CostentinJean-Michel Savéant
Jul 4, 2015·Physical Chemistry Chemical Physics : PCCP·Cyrille Costentin, Jean-Michel Savéant
May 4, 2017·Journal of the American Chemical Society·Cyrille Costentin, Jean-Michel Savéant

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