Promoting ethylene production over a wide potential window on Cu crystallites induced and stabilized via current shock and charge delocalization

Hao Sun, Ling Chen, Likun Xiong, Kun Feng, Yufeng Chen, Xiang Zhang, Xuzhou Yuan, Baiyu Yang, Zhao Deng, Yu Liu, Mark H. Rümmeli, Jun Zhong (), Yan Jiao () and Yang Peng ()
Additional contact information
Hao Sun: Soochow University
Ling Chen: The University of Adelaide
Likun Xiong: Soochow University
Kun Feng: Soochow University
Yufeng Chen: Soochow University
Xiang Zhang: Soochow University
Xuzhou Yuan: Soochow University
Baiyu Yang: Soochow University
Zhao Deng: Soochow University
Yu Liu: Soochow University
Mark H. Rümmeli: Soochow University
Jun Zhong: Soochow University
Yan Jiao: The University of Adelaide
Yang Peng: Soochow University

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: Abstract Electrochemical CO2 reduction (CO2RR) in a product-orientated and energy-efficient manner relies on rational catalyst design guided by mechanistic understandings. In this study, the effect of conducting support on the CO2RR behaviors of semi-conductive metal-organic framework (MOF) — Cu3(HITP)2 are carefully investigated. Compared to the stand-alone MOF, adding Ketjen Black greatly promotes C2H4 production with a stabilized Faradaic efficiency between 60-70% in a wide potential range and prolonged period. Multicrystalline Cu nano-crystallites in the reconstructed MOF are induced and stabilized by the conducting support via current shock and charge delocalization, which is analogous to the mechanism of dendrite prevention through conductive scaffolds in metal ion batteries. Density functional theory calculations elucidate that the contained multi-facets and rich grain boundaries promote C–C coupling while suppressing HER. This study underlines the key role of substrate-catalyst interaction, and the regulation of Cu crystalline states via conditioning the charge transport, in steering the CO2RR pathway.

Date: 2021
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DOI: 10.1038/s41467-021-27169-9

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