Tunable Product Selectivity in Electrochemical CO2 Reduction on Well-Mixed Ni–Cu Alloys

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Tunable Product Selectivity in Electrochemical CO2 Reduction on Well-Mixed Ni–Cu Alloys
Title:
Tunable Product Selectivity in Electrochemical CO2 Reduction on Well-Mixed Ni–Cu Alloys
Other Titles:
ACS Applied Materials & Interfaces
Publication Date:
12 November 2021
Citation:
Song, H., Tan, Y. C., Kim, B., Ringe, S., & Oh, J. (2021). Tunable Product Selectivity in Electrochemical CO2 Reduction on Well-Mixed Ni–Cu Alloys. ACS Applied Materials & Interfaces, 13(46), 55272–55280. doi:10.1021/acsami.1c19224
Abstract:
Electrochemical reduction of CO2 on copper-based catalysts has become a promising strategy to mitigate greenhouse gas emissions and gain valuable chemicals and fuels. Unfortunately, however, the generally low product selectivity of the process decreases the industrial competitiveness compared to the established large-scale chemical processes. Here, we present random solid solution Cu1–xNix alloy catalysts that, due to their full miscibility, enable a systematic modulation of adsorption energies. In particular, we find that these catalysts lead to an increase of hydrogen evolution with the Ni content, which correlates with a significant increase of the selectivity for methane formation relative to C2 products such as ethylene and ethanol. From experimental and theoretical insights, we find the increased hydrogen atom coverage to facilitate Langmuir–Hinshelwood-like hydrogenation of surface intermediates, giving an impressive almost 2 orders of magnitude increase in the CH4 to C2H4 + C2H5OH selectivity on Cu0.87Ni0.13 at −300 mA cm–2. This study provides important insights and design concepts for the tunability of product selectivity for electrochemical CO2 reduction that will help to pave the way toward industrially competitive electrocatalyst materials.
License type:
Publisher Copyright
Funding Info:
This research / project is supported by the National Research Foundation - Carbon to X Project
Grant Reference no. : NRF-2020M3H7A1096388

i) Ministry of Science and ICT, Republic of Korea and the National Research Foundation of Korea - NRF-2021R1A2C3007280 ii) National Research Foundation of Korea & Ministry of Science and ICT -Grant No. 2021R1C1C1008776 iii) Ministry of Science and ICT DGIST Start-up Fund Program Grand No. 2021010045
Description:
This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials & Interfaces, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://dx.doi.org/10.1021/acsami.1c19224
ISSN:
1944-8252
1944-8244
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