Surface charge as activity descriptors for electrochemical CO₂ reduction to multi-carbon products on organic-functionalised Cu
Intensive research in electrochemical CO2 reduction reaction has resulted in the discovery of numerous high-performance catalysts selective to multi-carbon products, with most of these catalysts still being purely transition metal based. Herein, we present high and stable multi-carbon products selec...
| Main Authors: | , , , , , , , , , , , , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2023
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| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/169752 |
| _version_ | 1811684493577158656 |
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| author | Lim, Carina Yi Jing Yilmaz, Meltem Arce-Ramos, Juan Manuel Handoko, Albertus D. Teh, Wei Jie Zheng, Yuangang Khoo, Jonathan Zi Hui Lin, Ming Isaacs, Mark Tam, Dexter Teck Lip Bai, Yang Ng, Chee Koon Yeo, Boon Siang Sankar, Gopinathan Parkin, Ivan P. Hippalgaonkar, Kedar Sullivan, Michael B. Zhang, Jia Lim, Yee-Fun |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering Lim, Carina Yi Jing Yilmaz, Meltem Arce-Ramos, Juan Manuel Handoko, Albertus D. Teh, Wei Jie Zheng, Yuangang Khoo, Jonathan Zi Hui Lin, Ming Isaacs, Mark Tam, Dexter Teck Lip Bai, Yang Ng, Chee Koon Yeo, Boon Siang Sankar, Gopinathan Parkin, Ivan P. Hippalgaonkar, Kedar Sullivan, Michael B. Zhang, Jia Lim, Yee-Fun |
| author_sort | Lim, Carina Yi Jing |
| collection | NTU |
| description | Intensive research in electrochemical CO2 reduction reaction has resulted in the discovery of numerous high-performance catalysts selective to multi-carbon products, with most of these catalysts still being purely transition metal based. Herein, we present high and stable multi-carbon products selectivity of up to 76.6% across a wide potential range of 1 V on histidine-functionalised Cu. In-situ Raman and density functional theory calculations revealed alternative reaction pathways that involve direct interactions between adsorbed histidine and CO2 reduction intermediates at more cathodic potentials. Strikingly, we found that the yield of multi-carbon products is closely correlated to the surface charge on the catalyst surface, quantified by a pulsed voltammetry-based technique which proved reliable even at very cathodic potentials. We ascribe the surface charge to the population density of adsorbed species on the catalyst surface, which may be exploited as a powerful tool to explain CO2 reduction activity and as a proxy for future catalyst discovery, including organic-inorganic hybrids. |
| first_indexed | 2024-10-01T04:29:30Z |
| format | Journal Article |
| id | ntu-10356/169752 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T04:29:30Z |
| publishDate | 2023 |
| record_format | dspace |
| spelling | ntu-10356/1697522023-08-04T15:45:43Z Surface charge as activity descriptors for electrochemical CO₂ reduction to multi-carbon products on organic-functionalised Cu Lim, Carina Yi Jing Yilmaz, Meltem Arce-Ramos, Juan Manuel Handoko, Albertus D. Teh, Wei Jie Zheng, Yuangang Khoo, Jonathan Zi Hui Lin, Ming Isaacs, Mark Tam, Dexter Teck Lip Bai, Yang Ng, Chee Koon Yeo, Boon Siang Sankar, Gopinathan Parkin, Ivan P. Hippalgaonkar, Kedar Sullivan, Michael B. Zhang, Jia Lim, Yee-Fun School of Materials Science and Engineering Institute of Materials Research and Engineering, A*STAR Engineering::Materials Density Functional Theory Raman Spectrometry Intensive research in electrochemical CO2 reduction reaction has resulted in the discovery of numerous high-performance catalysts selective to multi-carbon products, with most of these catalysts still being purely transition metal based. Herein, we present high and stable multi-carbon products selectivity of up to 76.6% across a wide potential range of 1 V on histidine-functionalised Cu. In-situ Raman and density functional theory calculations revealed alternative reaction pathways that involve direct interactions between adsorbed histidine and CO2 reduction intermediates at more cathodic potentials. Strikingly, we found that the yield of multi-carbon products is closely correlated to the surface charge on the catalyst surface, quantified by a pulsed voltammetry-based technique which proved reliable even at very cathodic potentials. We ascribe the surface charge to the population density of adsorbed species on the catalyst surface, which may be exploited as a powerful tool to explain CO2 reduction activity and as a proxy for future catalyst discovery, including organic-inorganic hybrids. Agency for Science, Technology and Research (A*STAR) National Research Foundation (NRF) Published version This work is supported by A*STAR (The Accelerated Catalyst Development Platform (A19E9a0103), Accelerated Materials Development for Manufacturing (A1898b0043) and Career Development Award (202D800037)), as well as the National Research Foundation, Singapore, and A*STAR under its LCERFI program (Award No U2102d2002). B.S.Y. acknowledges support from Ministry of Education, Singapore (A-0004135-00-00). M.Y. acknowledges studentship from A*STAR Research Attachment Programme. 2023-08-02T01:06:43Z 2023-08-02T01:06:43Z 2023 Journal Article Lim, C. Y. J., Yilmaz, M., Arce-Ramos, J. M., Handoko, A. D., Teh, W. J., Zheng, Y., Khoo, J. Z. H., Lin, M., Isaacs, M., Tam, D. T. L., Bai, Y., Ng, C. K., Yeo, B. S., Sankar, G., Parkin, I. P., Hippalgaonkar, K., Sullivan, M. B., Zhang, J. & Lim, Y. (2023). Surface charge as activity descriptors for electrochemical CO₂ reduction to multi-carbon products on organic-functionalised Cu. Nature Communications, 14(1). https://dx.doi.org/10.1038/s41467-023-35912-7 2041-1723 https://hdl.handle.net/10356/169752 10.1038/s41467-023-35912-7 14 2-s2.0-85146683811 1 14 en A1898b0043 202D800037 U2102d2002 Nature Communications © The Author(s) 2023, corrected publication 2023. Open Access. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/ licenses/by/4.0/. application/pdf |
| spellingShingle | Engineering::Materials Density Functional Theory Raman Spectrometry Lim, Carina Yi Jing Yilmaz, Meltem Arce-Ramos, Juan Manuel Handoko, Albertus D. Teh, Wei Jie Zheng, Yuangang Khoo, Jonathan Zi Hui Lin, Ming Isaacs, Mark Tam, Dexter Teck Lip Bai, Yang Ng, Chee Koon Yeo, Boon Siang Sankar, Gopinathan Parkin, Ivan P. Hippalgaonkar, Kedar Sullivan, Michael B. Zhang, Jia Lim, Yee-Fun Surface charge as activity descriptors for electrochemical CO₂ reduction to multi-carbon products on organic-functionalised Cu |
| title | Surface charge as activity descriptors for electrochemical CO₂ reduction to multi-carbon products on organic-functionalised Cu |
| title_full | Surface charge as activity descriptors for electrochemical CO₂ reduction to multi-carbon products on organic-functionalised Cu |
| title_fullStr | Surface charge as activity descriptors for electrochemical CO₂ reduction to multi-carbon products on organic-functionalised Cu |
| title_full_unstemmed | Surface charge as activity descriptors for electrochemical CO₂ reduction to multi-carbon products on organic-functionalised Cu |
| title_short | Surface charge as activity descriptors for electrochemical CO₂ reduction to multi-carbon products on organic-functionalised Cu |
| title_sort | surface charge as activity descriptors for electrochemical co₂ reduction to multi carbon products on organic functionalised cu |
| topic | Engineering::Materials Density Functional Theory Raman Spectrometry |
| url | https://hdl.handle.net/10356/169752 |
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