Surface charge as activity descriptors for electrochemical CO2 reduction to multi-carbon products on organic-functionalised Cu
Abstract 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 produ...
| Main Authors: | , , , , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2023-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-35912-7 |
| _version_ | 1827899752061075456 |
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| author | Carina Yi Jing Lim Meltem Yilmaz Juan Manuel Arce-Ramos Albertus D. Handoko Wei Jie Teh Yuangang Zheng Zi Hui Jonathan Khoo Ming Lin Mark Isaacs Teck Lip Dexter Tam Yang Bai Chee Koon Ng Boon Siang Yeo Gopinathan Sankar Ivan P. Parkin Kedar Hippalgaonkar Michael B. Sullivan Jia Zhang Yee-Fun Lim |
| author_facet | Carina Yi Jing Lim Meltem Yilmaz Juan Manuel Arce-Ramos Albertus D. Handoko Wei Jie Teh Yuangang Zheng Zi Hui Jonathan Khoo Ming Lin Mark Isaacs Teck Lip Dexter Tam Yang Bai Chee Koon Ng Boon Siang Yeo Gopinathan Sankar Ivan P. Parkin Kedar Hippalgaonkar Michael B. Sullivan Jia Zhang Yee-Fun Lim |
| author_sort | Carina Yi Jing Lim |
| collection | DOAJ |
| description | Abstract 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 | 2024-03-12T23:22:02Z |
| format | Article |
| id | doaj.art-2c718d61d24d45b8abee949e2f302094 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-12T23:22:02Z |
| publishDate | 2023-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-2c718d61d24d45b8abee949e2f3020942023-07-16T11:21:01ZengNature PortfolioNature Communications2041-17232023-01-0114111110.1038/s41467-023-35912-7Surface charge as activity descriptors for electrochemical CO2 reduction to multi-carbon products on organic-functionalised CuCarina Yi Jing Lim0Meltem Yilmaz1Juan Manuel Arce-Ramos2Albertus D. Handoko3Wei Jie Teh4Yuangang Zheng5Zi Hui Jonathan Khoo6Ming Lin7Mark Isaacs8Teck Lip Dexter Tam9Yang Bai10Chee Koon Ng11Boon Siang Yeo12Gopinathan Sankar13Ivan P. Parkin14Kedar Hippalgaonkar15Michael B. Sullivan16Jia Zhang17Yee-Fun Lim18Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR)Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR)Institute of High Performance Computing, Agency for Science, Technology and Research (A*STAR)Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR)Department of Chemistry, National University of SingaporeInstitute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR)Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR)Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR)Research Complex at Harwell, Rutherford Appleton LaboratoryInstitute of Sustainability for Chemical, Engineering and Environment, Agency of Science, Technology and Research (A*STAR)Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR)Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR)Department of Chemistry, National University of SingaporeDepartment of Chemistry, University College LondonDepartment of Chemistry, University College LondonInstitute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR)Institute of High Performance Computing, Agency for Science, Technology and Research (A*STAR)Institute of High Performance Computing, Agency for Science, Technology and Research (A*STAR)Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR)Abstract 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.https://doi.org/10.1038/s41467-023-35912-7 |
| spellingShingle | Carina Yi Jing Lim Meltem Yilmaz Juan Manuel Arce-Ramos Albertus D. Handoko Wei Jie Teh Yuangang Zheng Zi Hui Jonathan Khoo Ming Lin Mark Isaacs Teck Lip Dexter Tam Yang Bai Chee Koon Ng Boon Siang Yeo Gopinathan Sankar Ivan P. Parkin Kedar Hippalgaonkar Michael B. Sullivan Jia Zhang Yee-Fun Lim Surface charge as activity descriptors for electrochemical CO2 reduction to multi-carbon products on organic-functionalised Cu Nature Communications |
| 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 |
| url | https://doi.org/10.1038/s41467-023-35912-7 |
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