Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 43, Pages 23051-23067Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202110352
Keywords
CO2 reduction; electrocatalysis; N-2 reduction; turnover frequency; water splitting
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Funding
- Research Institute for Science and Engineering, Waseda University, Japan
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Turnover frequency (TOF) has long been used as an accurate indicator of the intrinsic activity of catalysts in electrocatalytic reactions, but is often not properly reported. While current density is significant in determining apparent activity, TOF can more accurately reflect intrinsic activity free from interfering phenomena, yet remains underused in electrocatalysis.
For decades, turnover frequency (TOF) has served as an accurate descriptor of the intrinsic activity of a catalyst, including those in electrocatalytic reactions involving both fuel generation and fuel consumption. Unfortunately, in most of the recent reports in this area, TOF is often not properly reported or not reported at all, in contrast to the overpotentials at a benchmarking current density. The current density is significant in determining the apparent activity, but it is affected by catalyst-centric parasitic reactions, electrolyte-centric competing reactions, and capacitance. Luckily, a properly calculated TOF can precisely give the intrinsic activity free from these phenomena in electrocatalysis. In this Viewpoint we ask: 1) What makes the commonly used activity markers unsuitable for intrinsic activity determination? 2) How can TOF reflect the intrinsic activity? 3) Why is TOF still underused in electrocatalysis? 4) What methods are used in TOF determination? and 5) What is essential in the more accurate calculation of TOF? Finally, the significance of normalizing TOF by Faradaic efficiency (FE) is stressed and we give our views on the development of universal analytical tools to determine the exact number of active sites and real surface area for all kinds of materials.
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