Cascade anchoring strategy for general mass production of high-loading single-atomic metal-nitrogen catalysts
Abstract
Although single-atomically dispersed metal-Nx on carbon support (M-NC) has great potential in heterogeneous catalysis, the scalable synthesis of such single-atom catalysts (SACs) with high-loading metal-Nx is greatly challenging since the loading and single-atomic dispersion have to be balanced at high temperature for forming metal-Nx. Herein, we develop a general cascade anchoring strategy for the mass production of a series of M-NC SACs with a metal loading up to 12.1 wt%. Systematic investigation reveals that the chelation of metal ions, physical isolation of chelate complex upon high loading, and the binding with N-species at elevated temperature are essential to achieving high-loading M-NC SACs. As a demonstration, high-loading Fe-NC SAC shows superior electrocatalytic performance for O2 reduction and Ni-NC SAC exhibits high electrocatalytic activity for CO2 reduction. The strategy paves a universal way to produce stable M-NC SAC with high-density metal-Nx sites for diverse high-performance applications.
- Authors:
-
- Chinese Academy of Sciences (CAS), Beijing (China); Univ. of Chinese Academy of Sciences, Beijing (China)
- Chinese Academy of Sciences (CAS), Beijing (China); Sichuan Normal Univ., Chengdu (China)
- Univ. of Chinese Academy of Sciences, Beijing (China); Chinese Academy of Sciences (CAS), Beijing (China)
- Chinese Academy of Sciences (CAS), Beijing (China)
- Univ. of Chinese Academy of Sciences, Beijing (China); Chinese Academy of Sciences, Shanghai (China)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1559195
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Zhao, Lu, Zhang, Yun, Huang, Lin-Bo, Liu, Xiao-Zhi, Zhang, Qing-Hua, He, Chao, Wu, Ze-Yuan, Zhang, Lin-Juan, Wu, Jinpeng, Yang, Wanli, Gu, Lin, Hu, Jin-Song, and Wan, Li-Jun. Cascade anchoring strategy for general mass production of high-loading single-atomic metal-nitrogen catalysts. United States: N. p., 2019.
Web. doi:10.1038/s41467-019-09290-y.
Zhao, Lu, Zhang, Yun, Huang, Lin-Bo, Liu, Xiao-Zhi, Zhang, Qing-Hua, He, Chao, Wu, Ze-Yuan, Zhang, Lin-Juan, Wu, Jinpeng, Yang, Wanli, Gu, Lin, Hu, Jin-Song, & Wan, Li-Jun. Cascade anchoring strategy for general mass production of high-loading single-atomic metal-nitrogen catalysts. United States. https://doi.org/10.1038/s41467-019-09290-y
Zhao, Lu, Zhang, Yun, Huang, Lin-Bo, Liu, Xiao-Zhi, Zhang, Qing-Hua, He, Chao, Wu, Ze-Yuan, Zhang, Lin-Juan, Wu, Jinpeng, Yang, Wanli, Gu, Lin, Hu, Jin-Song, and Wan, Li-Jun. Wed .
"Cascade anchoring strategy for general mass production of high-loading single-atomic metal-nitrogen catalysts". United States. https://doi.org/10.1038/s41467-019-09290-y. https://www.osti.gov/servlets/purl/1559195.
@article{osti_1559195,
title = {Cascade anchoring strategy for general mass production of high-loading single-atomic metal-nitrogen catalysts},
author = {Zhao, Lu and Zhang, Yun and Huang, Lin-Bo and Liu, Xiao-Zhi and Zhang, Qing-Hua and He, Chao and Wu, Ze-Yuan and Zhang, Lin-Juan and Wu, Jinpeng and Yang, Wanli and Gu, Lin and Hu, Jin-Song and Wan, Li-Jun},
abstractNote = {Although single-atomically dispersed metal-Nx on carbon support (M-NC) has great potential in heterogeneous catalysis, the scalable synthesis of such single-atom catalysts (SACs) with high-loading metal-Nx is greatly challenging since the loading and single-atomic dispersion have to be balanced at high temperature for forming metal-Nx. Herein, we develop a general cascade anchoring strategy for the mass production of a series of M-NC SACs with a metal loading up to 12.1 wt%. Systematic investigation reveals that the chelation of metal ions, physical isolation of chelate complex upon high loading, and the binding with N-species at elevated temperature are essential to achieving high-loading M-NC SACs. As a demonstration, high-loading Fe-NC SAC shows superior electrocatalytic performance for O2 reduction and Ni-NC SAC exhibits high electrocatalytic activity for CO2 reduction. The strategy paves a universal way to produce stable M-NC SAC with high-density metal-Nx sites for diverse high-performance applications.},
doi = {10.1038/s41467-019-09290-y},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {Wed Mar 20 00:00:00 EDT 2019},
month = {Wed Mar 20 00:00:00 EDT 2019}
}
Web of Science
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