Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 134, Issue 27, Pages 11235-11242Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja303560c
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Funding
- Agence Nationale de la Recherche [ANR 2010 BLAN 0808]
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The search for efficient catalysts to face modern energy challenges requires evaluation and comparison through reliable methods. Catalytic current efficiencies may be the combination of many factors besides the intrinsic chemical properties of the catalyst. Defining turnover number and turnover frequency (TOP) as reflecting these intrinsic chemical properties, it is shown that catalysts are not characterized by their TOF and their overpotential (eta) as separate parameters but rather that the parameters are linked together by a definite relationship. The log TOF-eta relationship can often be linearized, giving rise to a Tafel law, which allows the characterization of the catalyst by the value of the TOF at zero overpotential (TOF0). Foot-of-the-wave analysis of the cyclic voltammetric catalytic responses allows the determination of the TOP, log TOF-eta relationship, and TOF0, regardless of the side-phenomena that interfere at high current densities, preventing the expected catalytic current plateau from being reached. Strategies for optimized preparative-scale electrolyses may then be devised on these bases. The validity of this methodology is established on theoretical grounds and checked experimentally with examples taken from the catalytic reduction of CO2 by iron(0) porphyrins.
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