Characterizing CO 2 Reduction Catalysts on Gas Diffusion Electrodes: Comparing Activity, Selectivity, and Stability of Transition Metal Catalysts.

Autor:	Sassenburg M; Materials for Energy Conversion and Storage (MECS), Department of Chemical Engineering, Delft University of Technology, 2629 ZH Delft, The Netherlands., de Rooij R; Materials for Energy Conversion and Storage (MECS), Department of Chemical Engineering, Delft University of Technology, 2629 ZH Delft, The Netherlands., Nesbitt NT; Materials for Energy Conversion and Storage (MECS), Department of Chemical Engineering, Delft University of Technology, 2629 ZH Delft, The Netherlands., Kas R; Materials for Energy Conversion and Storage (MECS), Department of Chemical Engineering, Delft University of Technology, 2629 ZH Delft, The Netherlands.; Department of Chemical and Biological Engineering and Renewable and Sustainable Energy Institute (RASEI), University of Colorado Boulder, Boulder, Colorado 80303, United States., Chandrashekar S; Materials for Energy Conversion and Storage (MECS), Department of Chemical Engineering, Delft University of Technology, 2629 ZH Delft, The Netherlands., Firet NJ; Materials for Energy Conversion and Storage (MECS), Department of Chemical Engineering, Delft University of Technology, 2629 ZH Delft, The Netherlands., Yang K; Materials for Energy Conversion and Storage (MECS), Department of Chemical Engineering, Delft University of Technology, 2629 ZH Delft, The Netherlands., Liu K; Materials for Energy Conversion and Storage (MECS), Department of Chemical Engineering, Delft University of Technology, 2629 ZH Delft, The Netherlands., Blommaert MA; Materials for Energy Conversion and Storage (MECS), Department of Chemical Engineering, Delft University of Technology, 2629 ZH Delft, The Netherlands., Kolen M; Materials for Energy Conversion and Storage (MECS), Department of Chemical Engineering, Delft University of Technology, 2629 ZH Delft, The Netherlands., Ripepi D; Materials for Energy Conversion and Storage (MECS), Department of Chemical Engineering, Delft University of Technology, 2629 ZH Delft, The Netherlands., Smith WA; Materials for Energy Conversion and Storage (MECS), Department of Chemical Engineering, Delft University of Technology, 2629 ZH Delft, The Netherlands.; Department of Chemical and Biological Engineering and Renewable and Sustainable Energy Institute (RASEI), University of Colorado Boulder, Boulder, Colorado 80303, United States., Burdyny T; Materials for Energy Conversion and Storage (MECS), Department of Chemical Engineering, Delft University of Technology, 2629 ZH Delft, The Netherlands.
Jazyk:	angličtina
Zdroj:	ACS applied energy materials [ACS Appl Energy Mater] 2022 May 23; Vol. 5 (5), pp. 5983-5994. Date of Electronic Publication: 2022 May 03.
DOI:	10.1021/acsaem.2c00160
Abstrakt:	Continued advancements in the electrochemical reduction of CO 2 (CO 2 RR) have emphasized that reactivity, selectivity, and stability are not explicit material properties but combined effects of the catalyst, double-layer, reaction environment, and system configuration. These realizations have steadily built upon the foundational work performed for a broad array of transition metals performed at 5 mA cm -2 , which historically guided the research field. To encompass the changing advancements and mindset within the research field, an updated baseline at elevated current densities could then be of value. Here we seek to re-characterize the activity, selectivity, and stability of the five most utilized transition metal catalysts for CO 2 RR (Ag, Au, Pd, Sn, and Cu) at elevated reaction rates through electrochemical operation, physical characterization, and varied operating parameters to provide a renewed resource and point of comparison. As a basis, we have employed a common cell architecture, highly controlled catalyst layer morphologies and thicknesses, and fixed current densities. Through a dataset of 88 separate experiments, we provide comparisons between CO-producing catalysts (Ag, Au, and Pd), highlighting CO-limiting current densities on Au and Pd at 72 and 50 mA cm -2 , respectively. We further show the instability of Sn in highly alkaline environments, and the convergence of product selectivity at elevated current densities for a Cu catalyst in neutral and alkaline media. Lastly, we reflect upon the use and limits of reaction rates as a baseline metric by comparing catalytic selectivity at 10 versus 200 mA cm -2 . We hope the collective work provides a resource for researchers setting up CO 2 RR experiments for the first time. Competing Interests: The authors declare no competing financial interest. (© 2022 The Authors. Published by American Chemical Society.)
Databáze:	MEDLINE
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