Asymmetric dinitrogen-coordinated nickel single-atomic sites for efficient CO2 electroreduction

Yuzhu Zhou, Quan Zhou, Hengjie Liu, Wenjie Xu, Zhouxin Wang, Sicong Qiao, Honghe Ding, Dongliang Chen, Junfa Zhu, Zeming Qi, Xiaojun Wu, Qun He () and Li Song ()
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Yuzhu Zhou: University of Science and Technology of China
Quan Zhou: University of Science and Technology of China
Hengjie Liu: University of Science and Technology of China
Wenjie Xu: University of Science and Technology of China
Zhouxin Wang: University of Science and Technology of China
Sicong Qiao: University of Science and Technology of China
Honghe Ding: University of Science and Technology of China
Dongliang Chen: Chinese Academy of Sciences
Junfa Zhu: University of Science and Technology of China
Zeming Qi: University of Science and Technology of China
Xiaojun Wu: University of Science and Technology of China
Qun He: University of Science and Technology of China
Li Song: University of Science and Technology of China

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-39505-2

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