Dual atomic catalysts from COF-derived carbon for CO2RR by Suppressing HER through Synergistic Effects

Liu, Minghao; Liu, Sijia; Xu, Qing; Miao, Qiyang; Yang, Shuai; Hanson, Svenja; Chen, George Zheng; He, Jun; Jiang, Zheng; Zeng, Gaofeng

Abstract

The electrochemical carbon dioxide reduction reaction (CO2RR) for high-value-added products is a promising strategy to tackle excessive CO2 emissions. However, the activity of and selectivity for catalysts for CO2RR still need to be improved because of the competing reaction (hydrogen evolution reaction). In this study, for the first time, we have demonstrated dual atomic catalytic sites for CO2RR from a core–shell hybrid of the covalent–organic framework and the metal–organic framework. Due to abundant dual atomic sites (with CoN4O and ZnN4 of 2.47 and 11.05 wt.%, respectively) on hollow carbon, the catalyst promoted catalysis of CO2RR, with the highest Faradic efficiency for CO of 92.6% at –0.8 V and a turnover frequency value of 1370.24 h–1 at –1.0 V. More importantly, the activity and selectivity of the catalyst were well retained for 30 h. The theoretical calculation further revealed that CoN4O was the main site for CO2RR, and the activity of and selectivity for Zn sites were also improved because of the synergetic roles.

Citation

Liu, M., Liu, S., Xu, Q., Miao, Q., Yang, S., Hanson, S., Chen, G. Z., He, J., Jiang, Z., & Zeng, G. (2023). Dual atomic catalysts from COF-derived carbon for CO2RR by Suppressing HER through Synergistic Effects. Carbon Energy, 5(6), Article e300. https://doi.org/10.1002/cey2.300

• Journal Article Type: Article
• Acceptance Date: Sep 1, 2022
• Online Publication Date: Jan 6, 2023
• Publication Date: 2023-06
• Deposit Date: Oct 17, 2022
• Publicly Available Date: Jan 6, 2023
• Journal: Carbon Energy
• Electronic ISSN: 2637-9368
• Publisher: Wiley Open Access
• Peer Reviewed: Peer Reviewed
• Volume: 5
• Issue: 6
• Article Number: e300
• DOI: https://doi.org/10.1002/cey2.300
• Keywords: Covalent organic frameworks, Metal organic frameworks, Single atom catalysts, Carbon dioxide reduction reaction, Dual atomic catalysts, Materials Chemistry, Energy (miscellaneous), Materials Science (miscellaneous), Renewable Energy, Sustainability and th
• Public URL: https://nottingham-repository.worktribe.com/output/12599833
• Publisher URL: https://onlinelibrary.wiley.com/doi/10.1002/cey2.300