Quasi-Copper-Mers Enable High-Performance Catalysis for CO2 Reduction

Quasi-Copper-Mers Enable High-Performance Catalysis for CO2 Reduction

Advanced Science

10.1002/advs.202303297

http://dx.doi.org/10.1002/advs.202303297

Jing Yang, Ximeng Liu, Zhao Li, Shibo Xi, Jianguo Sun, Hao Yuan, Weihao Liu, Tuo Wang, Yulin Gao, Haimei Wang, Junjie Wang, Jun Song Chen, Rui Wu, Yong‐Wei Zhang, John Wang

09 August 2023

Yang, J., Liu, X., Li, Z., Xi, S., Sun, J., Yuan, H., Liu, W., Wang, T., Gao, Y., Wang, H., Wang, J., Chen, J. S., Wu, R., Zhang, Y., & Wang, J. (2023). Quasi‐Copper‐Mers Enable High‐Performance Catalysis for CO2 Reduction. Advanced Science, 10(29). Portico. https://doi.org/10.1002/advs.202303297

AbstractAs the atmospheric carbon dioxide (CO2) level keeps hitting the new record, humanity is facing an ever‐daunting challenge to efficiently mitigate CO2 from the atmosphere. Though electrochemical CO2 reduction presents a promising pathway to convert CO2 to valuable fuels and chemicals, the general lack of suitable electrocatalysts with high activity and selectivity severely constrains this approach. Herein, a novel class of electrocatalysts is investigated, the quasi‐copper‐mers, in which the CuN4 rather than Cu atom itself serve as the basic building block. The respective quasi‐copper‐monomers, ‐dimers, and ‐trimers hosted in a graphene‐like substrate are first synthesized and then performed both experimental characterization and density functional theory (DFT) calculations to examine their atomic structures, evaluate their electrocatalytical performance and understand their underlying mechanisms. The experimental results show that the quasi‐copper‐trimers not only outperform the quasi‐copper‐dimer and quasi‐copper‐monomer when catalyzing CO2 to CO, it also shows a superior selectivity against the competing hydrogen evolution reaction (HER). The DFT calculations not only support the experimental observations, but also reveal the volcano curve and the physical origin for the qausi‐copper‐trimer superiority. The present work thus presents a new strategy in the design of high‐performance electrocatalysts with high activity and selectivity.

Attribution 4.0 International (CC BY 4.0)

This research / project is supported by the Ministry of Education - Tier 1
Grant Reference no. : A-8000186-01-00

This research / project is supported by the A*STAR - SERC Central Research Fund (CRF)
Grant Reference no. : NA

This research / project is supported by the National Research Foundation - Competitive Research Programme
Grant Reference no. : NRF-CRP26-2021-0003

support from the Italy-Singapore Science and Technology Co-operation (Grant no. R23101R040)

https://oar.a-star.edu.sg/communities-collections/articles/19889

2198-3844

Institute of High Performance Computing 

https://doi.org/10.1002/advs.202303297