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In Situ Phosphatizing of Triphenylphosphine Encapsulated within Metal–Organic Frameworks to Design Atomic Co1–P1N3 Interfacial Structure for Promoting Catalytic Performance

Wan, Jiawei, Zhao, Zhenghang, Shang, Huishan, Peng, Bo, Chen, Wenxing, Pei, Jiajing, Zheng, Lirong, Dong, Juncai, Cao, Rui, Sarangi, Ritimukta, Jiang, Zhuoli, Zhou, Danni, Zhuang, Zhongbin, Zhang, Jiatao, Wang, Dingsheng, Li, Yadong·2020·Journal of the American Chemical Society

Abstract

The engineering coordination environment offers great opportunity in performance tunability of isolated metal single-atom catalysts. For the most popular metal–N x (MN x ) structure, the replacement of N atoms by some other atoms with relatively weak electronegativity has been regarded as a promising strategy for optimizing the coordination environment of an active metal center and promoting its catalytic performance, which is still a challenge. Herein, we proposed a new synthetic strategy of an in situ phosphatizing of triphenylphosphine encapsulated within metal–organic frameworks for designing atomic Co 1 –P 1 N 3 interfacial structure, where a cobalt single atom is costabilized by one P atom and three N atoms (denoted as Co-SA/P-in situ). In the acidic media, the Co-SA/P-in situ catalyst with Co 1 –P 1 N 3 interfacial structure exhibits excellent activity and durability for the hydrogen evolution reaction (HER) with a low overpotential of 98 mV at 10 mA cm –2 and a small Tafel slope of 47 mV dec –1, which are greatly superior to those of catalyst with Co 1 –N 4 interfacial structure. We discover that the bond-length-extended high-valence Co 1 –P 1 N 3 atomic interface structure plays a crucial role in boosting the HER performance, which is supported by in situ X-ray absorption fine structure (XAFS) measurements and density functional theory (DFT) calculation. We hope this work will promote the development of high performance metal single-atom catalysts.

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Metadata

Authors
Wan, J., Zhao, Z., Shang, H., Peng, B., Chen, W., Pei, J., Zheng, L., Dong, J., Cao, R., Sarangi, R., Jiang, Z., Zhou, D., Zhuang, Z., Zhang, J., Wang, D., & Li, Y.
Venue
Journal of the American Chemical Society
Published
2020-04-17
Volume
142
Issue
18
Pages
8431-8439
ISSN
  • 0002-7863 (ISSN-L)
  • 1520-5126
OpenAlex
W3017139771
Cited by
422
References
9
FWCI
11.61
Type
journal article
Language
en
Open access
closed

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CoChat. (2026). Citation check: In Situ Phosphatizing of Triphenylphosphine Encapsulated within Metal–Organic Frameworks to Design Atomic Co1–P1N3 Interfacial Structure for Promoting Catalytic Performance. https://app.cochat.ai/papers/10.1021/jacs.0c02229
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Wan, J., Zhao, Z., Shang, H., Peng, B., Chen, W., Pei, J., Zheng, L., Dong, J., Cao, R., Sarangi, R., Jiang, Z., Zhou, D., Zhuang, Z., Zhang, J., Wang, D., & Li, Y. (2020). In Situ Phosphatizing of Triphenylphosphine Encapsulated within Metal–Organic Frameworks to Design Atomic Co1–P1N3 Interfacial Structure for Promoting Catalytic Performance. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.0c02229

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