Modulating intramolecular electron and proton transfer kinetics for promoting carbon dioxide conversion

Yajie Yuan; Yazhen Zhao; Shuai Yang; Sheng Han; Chenbao Lu; Huiping Ji; Tianfu Wang; Changchun Ke; Qing Xu; Jinhui Zhu; Xiaodong Zhuang

doi:10.1039/D1CC06731A

Modulating intramolecular electron and proton transfer kinetics for promoting carbon dioxide conversion†

Yajie Yuan,^ab Yazhen Zhao,^b Shuai Yang,^c Sheng Han,

*^a Chenbao Lu,

*^b Huiping Ji,*^b Tianfu Wang,

^b Changchun Ke,*^d Qing Xu,

^e Jinhui Zhu

^bf and Xiaodong Zhuang

^b

Author affiliations

* Corresponding authors

^a School of Chemical and Environmental Engineering, Shanghai Institute of Technology, Shanghai 201418, China

^b The Meso-Entropy Matter Lab, State Key Laboratory of Metal Matrix Composites, School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, Shanghai, China
E-mail: castle@sjtu.edu.cn

^c Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201210, P. R. China

^d Institute of Fuel Cells, School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China

^e CAS Key Laboratory of Low-Carbon Conversion Science and Engineering, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201210, P. R. China

^f College of Chemistry, Zhengzhou University, Zhengzhou, Henan 450001, China

Abstract

A novel pentagon-heptagon paired azulene group that possesses a large dipole moment is immobilized onto a porphyrin. The as-prepared azulene iron porphyrin exhibits a narrower bandgap and higher electrocatalytic CO₂ reduction activity than the pristine iron porphyrin. The maximum CO faradaic efficiency reaches 99.9%, which is the state-of-the-art value among molecular catalysts.

Chemical Communications

Modulating intramolecular electron and proton transfer kinetics for promoting carbon dioxide conversion†

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Modulating intramolecular electron and proton transfer kinetics for promoting carbon dioxide conversion

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