Atomically precise Ni clusters inducing active NiN2 sites with uniform-large vacancies towards efficient CO2-to-CO conversion
CO<sub>2</sub> electroreduction to CO promises to give an efficient strategy for CO<sub>2</sub> 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 NiN<sub>2</sub> 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 (Ni<sub>n</sub>) and in-situ etching of the support by the 'nano bomb' (sulfur-ligand in the clusters). The NiN<sub>2</sub> sites with UL vacancies could achieve a high turnover frequency (TOF) of 350000 h<sup>-1</sup> with ~100% FEco in a wide potential range of 1500 mV. In-situ infrared spectra and theoretical calculations reveal that a highly pure NiN<sub>2</sub> 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.
Authors
- Huixin Xiang
- Chuanhao Yao (ORCID: https://orcid.org/0000-0001-6858-6560)
- Li‐Yong Gan (ORCID: https://orcid.org/0000-0002-1879-1918)
- Xiao Hai (ORCID: https://orcid.org/0000-0002-7631-9769)
- Guangyuan Xu
- Meng Zhou (ORCID: https://orcid.org/0000-0001-5187-9084)
- Lei Feng (ORCID: https://orcid.org/0000-0002-1823-1566)
- Yuan Kong (ORCID: https://orcid.org/0000-0002-5637-2511)
- Shibo Xi (ORCID: https://orcid.org/0000-0002-8521-3237)
- Xingjie Peng
- Chuanqiang Wu (ORCID: https://orcid.org/0000-0002-8549-9685)
- Yi Duan (ORCID: https://orcid.org/0000-0001-6936-5233)
- Jie Zhao (ORCID: https://orcid.org/0000-0002-6086-9387)
- Wu Zhou (ORCID: https://orcid.org/0000-0002-6803-1095)
- Huan Yan (ORCID: https://orcid.org/0000-0002-3734-5913)
- Su‐Huai Wei (ORCID: https://orcid.org/0000-0003-1563-4738)
- Tianfu Wang (ORCID: https://orcid.org/0000-0003-0026-5458)
- F.L. Nie (ORCID: https://orcid.org/0009-0004-0896-8099)
- Yanzhe Ma
- Zhendong Liu (ORCID: https://orcid.org/0000-0001-9201-911X)
- Si Chen (ORCID: https://orcid.org/0009-0008-6971-5457)
Institutions
- Agency for Science, Technology and Research (SG)
- University of Science and Technology of China (CN)
- Anhui University (CN)
- Shanghai Jiao Tong University (CN)
- Chinese Academy of Sciences (CN)
- Peking University (CN)
- Suzhou Institute of Nano-tech and Nano-bionics (CN)
- Hefei National Center for Physical Sciences at Nanoscale (CN)
- Rex Medical (United States) (US)
- University of Chinese Academy of Sciences (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-04-22
- DOI
- https://doi.org/10.1038/s41467-025-59079-5
- Citations
- 16
- Primary Topic
- CO2 Reduction Techniques and Catalysts
- Type
- article
- Field-Weighted Citation Impact
- 5.82
Funders
- National Natural Science Foundation of China
- Chinese Academy of Sciences
- Natural Science Foundation of Fujian Province
- University of Science and Technology of China
- Fujian Normal University
- University of Chinese Academy of Sciences
- Natural Science Foundation of Ningbo
- Natural Science Foundation of Anhui Province
- National Key Research and Development Program of China