Engineering Single-Atom Cobalt Catalysts toward Improved Electrocatalysis
Abstract
In this paper, the development of cost-effective catalysts to replace noble metal is attracting increasing interests in many fields of catalysis and energy, and intensive efforts are focused on the integration of transition-metal sites in carbon as noble-metal-free candidates. Recently, the discovery of single-atom dispersed catalyst (SAC) provides a new frontier in heterogeneous catalysis. However, the electrocatalytic application of SAC is still subject to several theoretical and experimental limitations. Further advances depend on a better design of SAC through optimizing its interaction with adsorbates during catalysis. Here, distinctive from previous studies, favorable 3d electronic occupation and enhanced metal-adsorbates interactions in single-atom centers via the construction of nonplanar coordination is achieved, which is confirmed by advanced X-ray spectroscopic and electrochemical studies. The as-designed atomically dispersed cobalt sites within nonplanar coordination show significantly improved catalytic activity and selectivity toward the oxygen reduction reaction, approaching the benchmark Pt-based catalysts. More importantly, the illustration of the active sites in SAC indicates metal-natured catalytic sites and a media-dependent catalytic pathway. Achieving structural and electronic engineering on SAC that promotes its catalytic performances provides a paradigm to bridge the gap between single-atom catalysts design and electrocatalytic applications.
- Authors:
-
[2]
- Chinese Academy of Sciences, Shanghai (People's Republic of China); Univ. of Chinese Academy of Sciences, Beijing (People's Republic of China)
- Chinese Academy of Sciences, Shanghai (People's Republic of China)
- Argonne National Lab. (ANL), Lemont, IL (United States)
- Illinois Institute of Technology, Chicago, IL (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States); Northern Illinois Univ., DeKalb, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- National Key Basic Research Program of China; USDOE
- OSTI Identifier:
- 1474147
- Alternate Identifier(s):
- OSTI ID: 1423700
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Small
- Additional Journal Information:
- Journal Volume: 14; Journal Issue: 15; Journal ID: ISSN 1613-6810
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; electrocatalysis; media-dependence; metal-adsorbate interactions; selectivity; single-atom dispersed catalysts
Citation Formats
Wan, Gang, Yu, Pengfei, Chen, Hangrong, Wen, Jianguo, Sun, Cheng-jun, Zhou, Hua, Zhang, Nian, Li, Qianru, Zhao, Wanpeng, Xie, Bing, Li, Tao, and Shi, Jianlin. Engineering Single-Atom Cobalt Catalysts toward Improved Electrocatalysis. United States: N. p., 2018.
Web. doi:10.1002/smll.201704319.
Wan, Gang, Yu, Pengfei, Chen, Hangrong, Wen, Jianguo, Sun, Cheng-jun, Zhou, Hua, Zhang, Nian, Li, Qianru, Zhao, Wanpeng, Xie, Bing, Li, Tao, & Shi, Jianlin. Engineering Single-Atom Cobalt Catalysts toward Improved Electrocatalysis. United States. https://doi.org/10.1002/smll.201704319
Wan, Gang, Yu, Pengfei, Chen, Hangrong, Wen, Jianguo, Sun, Cheng-jun, Zhou, Hua, Zhang, Nian, Li, Qianru, Zhao, Wanpeng, Xie, Bing, Li, Tao, and Shi, Jianlin. Mon .
"Engineering Single-Atom Cobalt Catalysts toward Improved Electrocatalysis". United States. https://doi.org/10.1002/smll.201704319. https://www.osti.gov/servlets/purl/1474147.
@article{osti_1474147,
title = {Engineering Single-Atom Cobalt Catalysts toward Improved Electrocatalysis},
author = {Wan, Gang and Yu, Pengfei and Chen, Hangrong and Wen, Jianguo and Sun, Cheng-jun and Zhou, Hua and Zhang, Nian and Li, Qianru and Zhao, Wanpeng and Xie, Bing and Li, Tao and Shi, Jianlin},
abstractNote = {In this paper, the development of cost-effective catalysts to replace noble metal is attracting increasing interests in many fields of catalysis and energy, and intensive efforts are focused on the integration of transition-metal sites in carbon as noble-metal-free candidates. Recently, the discovery of single-atom dispersed catalyst (SAC) provides a new frontier in heterogeneous catalysis. However, the electrocatalytic application of SAC is still subject to several theoretical and experimental limitations. Further advances depend on a better design of SAC through optimizing its interaction with adsorbates during catalysis. Here, distinctive from previous studies, favorable 3d electronic occupation and enhanced metal-adsorbates interactions in single-atom centers via the construction of nonplanar coordination is achieved, which is confirmed by advanced X-ray spectroscopic and electrochemical studies. The as-designed atomically dispersed cobalt sites within nonplanar coordination show significantly improved catalytic activity and selectivity toward the oxygen reduction reaction, approaching the benchmark Pt-based catalysts. More importantly, the illustration of the active sites in SAC indicates metal-natured catalytic sites and a media-dependent catalytic pathway. Achieving structural and electronic engineering on SAC that promotes its catalytic performances provides a paradigm to bridge the gap between single-atom catalysts design and electrocatalytic applications.},
doi = {10.1002/smll.201704319},
journal = {Small},
number = 15,
volume = 14,
place = {United States},
year = {Mon Mar 05 00:00:00 EST 2018},
month = {Mon Mar 05 00:00:00 EST 2018}
}
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Figures / Tables:
Figure 1: Synthesis and composition of the SAC (a) Schematic illustration of the supportassisted pyrolysis synthesis approach for catalyst CoNC700. (b) The Co K-edge X-ray absorption near edge structure (XANES) of catalyst CoNC700, cobalt phthalocyanine (CoPC), and cobalt tetramethoxyphenylporphyrin (CoTMPP), and Co foil; (c) Fitting of the Co-N/O bonding inmore »
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