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Screening surface structure–electrochemical activity relationships of copper electrodes under CO2 electroreduction conditions
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Wahab, Oluwasegun J., Kang, Minkyung, Daviddi, Enrico, Walker, Marc and Unwin, Patrick R. (2022) Screening surface structure–electrochemical activity relationships of copper electrodes under CO2 electroreduction conditions. ACS Catalysis, 12 (11). pp. 6578-6588. doi:10.1021/acscatal.2c01650 ISSN 2155-5435.
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Official URL: https://doi.org/10.1021/acscatal.2c01650
Abstract
Understanding how crystallographic orientation influences the electrocatalytic performance of metal catalysts can potentially advance the design of catalysts with improved efficiency. Although single crystal electrodes are typically used for such studies, the one-at-a-time preparation procedure limits the range of secondary crystallographic orientations that can be profiled. This work employs scanning electrochemical cell microscopy (SECCM) together with co-located electron backscatter diffraction (EBSD) as a screening technique to investigate how surface crystallographic orientations on polycrystalline copper (Cu) correlate to activity under CO2 electroreduction conditions. SECCM measures spatially resolved voltammetry on polycrystalline copper covering low overpotentials of CO2 conversion to intermediates, thereby screening the different activity from low-index facets where H2 evolution is dominant to high-index facets where more reaction intermediates are expected. This approach allows the acquisition of 2500 voltammograms on approximately 60 different Cu surface facets identified with EBSD. The results show that the order of activity is (111) < (100) < (110) among the Cu primary orientations. The collection of data over a wide range of secondary orientations leads to the construction of an “electrochemical–crystallographic stereographic triangle” that provides a broad comprehension of the trends among Cu secondary surface facets rarely studied in the literature, [particularly (941) and (741)], and clearly shows that the electroreduction activity scales with the step and kink density of these surfaces. This work also reveals that the electrochemical stripping of the passive layer that is naturally formed on Cu in air is strongly grain-dependent, and the relative ease of stripping on low-index facets follows the order of (100) > (111) > (110). This allows a procedure to be implemented, whereby the oxide is removed (to an electrochemically undetectable level) prior to the kinetic analyses of electroreduction activity. SECCM screening allows for the most active surfaces to be ranked and prompts in-depth follow-up studies.
Item Type: | Journal Article | ||||||||||||
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Subjects: | Q Science > QD Chemistry | ||||||||||||
Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry | ||||||||||||
SWORD Depositor: | Library Publications Router | ||||||||||||
Library of Congress Subject Headings (LCSH): | Crystallography, Copper, Electrochemistry, Scanning electrochemical microscopy, Carbon dioxide | ||||||||||||
Journal or Publication Title: | ACS Catalysis | ||||||||||||
Publisher: | American Chemical Society (ACS) | ||||||||||||
ISSN: | 2155-5435 | ||||||||||||
Official Date: | 3 June 2022 | ||||||||||||
Dates: |
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Volume: | 12 | ||||||||||||
Number: | 11 | ||||||||||||
Page Range: | pp. 6578-6588 | ||||||||||||
DOI: | 10.1021/acscatal.2c01650 | ||||||||||||
Status: | Peer Reviewed | ||||||||||||
Publication Status: | Published | ||||||||||||
Access rights to Published version: | Open Access (Creative Commons) | ||||||||||||
Copyright Holders: | Copyright © 2022 The Authors. Published by American Chemical Society | ||||||||||||
Date of first compliant deposit: | 10 August 2022 | ||||||||||||
Date of first compliant Open Access: | 10 August 2022 | ||||||||||||
RIOXX Funder/Project Grant: |
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