Asymmetric dinitrogen-coordinated nickel single-atomic sites for efficient CO2 electroreduction
Abstract Developing highly efficient, selective and low-overpotential electrocatalysts for carbon dioxide (CO2) reduction is crucial. This study reports an efficient Ni single-atom catalyst coordinated with pyrrolic nitrogen and pyridinic nitrogen for CO2 reduction to carbon monoxide (CO). In flow c...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2023-06-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-39505-2 |
| _version_ | 1797795574417719296 |
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| author | Yuzhu Zhou Quan Zhou Hengjie Liu Wenjie Xu Zhouxin Wang Sicong Qiao Honghe Ding Dongliang Chen Junfa Zhu Zeming Qi Xiaojun Wu Qun He Li Song |
| author_facet | Yuzhu Zhou Quan Zhou Hengjie Liu Wenjie Xu Zhouxin Wang Sicong Qiao Honghe Ding Dongliang Chen Junfa Zhu Zeming Qi Xiaojun Wu Qun He Li Song |
| author_sort | Yuzhu Zhou |
| collection | DOAJ |
| description | Abstract Developing highly efficient, selective and low-overpotential electrocatalysts for carbon dioxide (CO2) reduction is crucial. This study reports an efficient Ni single-atom catalyst coordinated with pyrrolic nitrogen and pyridinic nitrogen for CO2 reduction to carbon monoxide (CO). In flow cell experiments, the catalyst achieves a CO partial current density of 20.1 mA cmgeo −2 at −0.15 V vs. reversible hydrogen electrode (VRHE). It exhibits a high turnover frequency of over 274,000 site−1 h−1 at −1.0 VRHE and maintains high Faradaic efficiency of CO (FECO) exceeding 90% within −0.15 to −0.9 VRHE. Operando synchrotron-based infrared and X-ray absorption spectra, and theoretical calculations reveal that mono CO-adsorbed Ni single sites formed during electrochemical processes contribute to the balance between key intermediates formation and CO desorption, providing insights into the catalyst’s origin of catalytic activity. Overall, this work presents a Ni single-atom catalyst with good selectivity and activity for CO2 reduction while shedding light on its underlying mechanism. |
| first_indexed | 2024-03-13T03:20:01Z |
| format | Article |
| id | doaj.art-4b456c7052ef40789375ee3715eb862d |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-13T03:20:01Z |
| publishDate | 2023-06-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-4b456c7052ef40789375ee3715eb862d2023-06-25T11:22:20ZengNature PortfolioNature Communications2041-17232023-06-0114111010.1038/s41467-023-39505-2Asymmetric dinitrogen-coordinated nickel single-atomic sites for efficient CO2 electroreductionYuzhu Zhou0Quan Zhou1Hengjie Liu2Wenjie Xu3Zhouxin Wang4Sicong Qiao5Honghe Ding6Dongliang Chen7Junfa Zhu8Zeming Qi9Xiaojun Wu10Qun He11Li Song12National Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of ChinaNational Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of ChinaNational Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of ChinaNational Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of ChinaNational Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of ChinaNational Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of ChinaNational Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of ChinaBeijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of SciencesNational Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of ChinaNational Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of ChinaHefei National Laboratory for Physical Science at the Microscale, Collaborative Innovation of Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Sciences, University of Science and Technology of ChinaNational Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of ChinaNational Synchrotron Radiation Laboratory, CAS Center for Excellence in Nanoscience, University of Science and Technology of ChinaAbstract Developing highly efficient, selective and low-overpotential electrocatalysts for carbon dioxide (CO2) reduction is crucial. This study reports an efficient Ni single-atom catalyst coordinated with pyrrolic nitrogen and pyridinic nitrogen for CO2 reduction to carbon monoxide (CO). In flow cell experiments, the catalyst achieves a CO partial current density of 20.1 mA cmgeo −2 at −0.15 V vs. reversible hydrogen electrode (VRHE). It exhibits a high turnover frequency of over 274,000 site−1 h−1 at −1.0 VRHE and maintains high Faradaic efficiency of CO (FECO) exceeding 90% within −0.15 to −0.9 VRHE. Operando synchrotron-based infrared and X-ray absorption spectra, and theoretical calculations reveal that mono CO-adsorbed Ni single sites formed during electrochemical processes contribute to the balance between key intermediates formation and CO desorption, providing insights into the catalyst’s origin of catalytic activity. Overall, this work presents a Ni single-atom catalyst with good selectivity and activity for CO2 reduction while shedding light on its underlying mechanism.https://doi.org/10.1038/s41467-023-39505-2 |
| spellingShingle | Yuzhu Zhou Quan Zhou Hengjie Liu Wenjie Xu Zhouxin Wang Sicong Qiao Honghe Ding Dongliang Chen Junfa Zhu Zeming Qi Xiaojun Wu Qun He Li Song Asymmetric dinitrogen-coordinated nickel single-atomic sites for efficient CO2 electroreduction Nature Communications |
| title | Asymmetric dinitrogen-coordinated nickel single-atomic sites for efficient CO2 electroreduction |
| title_full | Asymmetric dinitrogen-coordinated nickel single-atomic sites for efficient CO2 electroreduction |
| title_fullStr | Asymmetric dinitrogen-coordinated nickel single-atomic sites for efficient CO2 electroreduction |
| title_full_unstemmed | Asymmetric dinitrogen-coordinated nickel single-atomic sites for efficient CO2 electroreduction |
| title_short | Asymmetric dinitrogen-coordinated nickel single-atomic sites for efficient CO2 electroreduction |
| title_sort | asymmetric dinitrogen coordinated nickel single atomic sites for efficient co2 electroreduction |
| url | https://doi.org/10.1038/s41467-023-39505-2 |
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