Büchele, S, Martín, AJ, Mitchell, S et al. (5 more authors) (2020) Structure Sensitivity and Evolution of Nickel-Bearing Nitrogen-Doped Carbons in the Electrochemical Reduction of CO2. ACS Catalysis, 10 (5). pp. 3444-3454. ISSN 2155-5435
Abstract
The emergence of nickel single atoms on nitrogen-doped carbons as high-performance catalysts amenable to rationalization due to their well-defined structure could lead to applicable technologies for the electrocatalytic CO2 reduction reaction (eCO2RR). However, real materials are unlikely to display a uniform site structure, which limits the scope of current efforts focused on idealized models for future implementation. Here, we prepare distinct nickel entities (single atoms or nanoparticles) on nitrogen-doped carbons and evaluate them in eCO2RR. Single atoms demonstrate a characteristic high selectivity to CO. However, this is not altered by the presence of metal nanoparticles formed upon reducing the nitrogen content of the carrier. In contrast, nanoparticles incorporated via a colloidal route promote the parasitic hydrogen evolution reaction. In these systems, the CO selectivity evolves upon repeated exposure to potential, reaching values comparable to single atoms. By introducing CO stripping voltammetry as a characterization tool for this class of materials, we identify a decreased metallic surface, suggesting that the nanoparticle surface is altered by CO. The findings highlight the critical role of dynamic effects in catalyst design for eCO2RR.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Keywords: | electrocatalytic CO2 reduction; single-atom catalysis; nickel speciation; nitrogen-doped carbons; structure−activity relationships |
Dates: |
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Institution: | The University of Leeds |
Academic Units: | The University of Leeds > Faculty of Engineering & Physical Sciences (Leeds) > School of Chemical & Process Engineering (Leeds) |
Depositing User: | Symplectic Publications |
Date Deposited: | 19 Feb 2020 14:40 |
Last Modified: | 14 Feb 2021 01:38 |
Status: | Published |
Publisher: | American Chemical Society |
Identification Number: | 10.1021/acscatal.9b05333 |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:157340 |