Atomically precise Ni clusters inducing active NiN2 sites with uniform-large vacancies towards efficient CO2-to-CO conversion

Guangyuan Xu, Xingjie Peng, Chuanqiang Wu, Shibo Xi, Huixin Xiang, Lei Feng, Zhendong Liu, Yi Duan, Lijin Gan, Si Chen, Yuan Kong (), Yanzhe Ma, Fujing Nie, Jie Zhao, Xiao Hai, Wei Wei, Meng Zhou, Tianfu Wang (), Chuanhao Yao (), Wu Zhou and Huan Yan ()
Additional contact information
Guangyuan Xu: University of Science and Technology of China
Xingjie Peng: University of Chinese Academy of Sciences
Chuanqiang Wu: Anhui University
Shibo Xi: A*STAR
Huixin Xiang: Fujian Normal University and Strait Laboratory of Flexible Electronics (SLoFE)
Lei Feng: University of Science and Technology of China
Zhendong Liu: University of Science and Technology of China
Yi Duan: University of Science and Technology of China
Lijin Gan: University of Science and Technology of China
Si Chen: University of Science and Technology of China
Yuan Kong: University of Science and Technology of China
Yanzhe Ma: University of Science and Technology of China
Fujing Nie: University of Science and Technology of China
Jie Zhao: University of Science and Technology of China
Xiao Hai: Peking University
Wei Wei: Chinese Academy of Sciences
Meng Zhou: University of Science and Technology of China
Tianfu Wang: Shanghai Jiao Tong University
Chuanhao Yao: Fujian Normal University and Strait Laboratory of Flexible Electronics (SLoFE)
Wu Zhou: University of Chinese Academy of Sciences
Huan Yan: University of Science and Technology of China

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract CO2 electroreduction to CO promises to give an efficient strategy for CO2 fixation and transformation. However, current reported active sites fail to deliver sufficient activity with high CO Faradic efficiency (FEco) over a wide range of potential. Here, we show a general synthetic protocol to fabricate a batch of highly pure and active NiN2 catalysts with precise engineering of the uniform-large (UL) vacancy around the active sites, which is accomplished through the ‘pre-deposition + pyrolysis’ of various atomically precise Ni clusters (Nin) and in-situ etching of the support by the ‘nano bomb’ (sulfur-ligand in the clusters). The NiN2 sites with UL vacancies could achieve a high turnover frequency (TOF) of 350000 h−1 with ~100% FEco in a wide potential range of 1500 mV. In-situ infrared spectra and theoretical calculations reveal that a highly pure NiN2 site with UL vacancy contributes to this remarkable catalytic performance compared to the counterparts. This general synthetic strategy enables us to simultaneously engineer active sites and surrounding vacancies with the employment of atomically precise metal clusters, thereby enhancing catalytic performance for other specific reactions.

Date: 2025
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DOI: 10.1038/s41467-025-59079-5

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