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  5f Covalency Synergistically Boosting Oxygen Evolution of UCoO4 Catalyst

Lin, X., Huang, Y.-C., Hu, Z., Li, L., Zhou, J., Zhao, Q., et al. (2021). 5f Covalency Synergistically Boosting Oxygen Evolution of UCoO4 Catalyst. Journal of the American Chemical Society, 1-8. doi:10.1021/jacs.1c10311.

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 Creators:
Lin, Xiao1, Author
Huang, Yu-Cheng1, Author
Hu, Zhiwei2, Author              
Li, Lili1, Author
Zhou, Jing1, Author
Zhao, Qingyun1, Author
Huang, Haoliang1, Author
Sun, Jian1, Author
Pao, Chih-Wen1, Author
Chang, Yu-Chung1, Author
Lin, Hong-Ji1, Author
Chen, Chien-Te1, Author
Dong, Chung-Li1, Author
Wang, Jian-Qiang1, Author
Zhang, Linjuan1, Author
Affiliations:
1External Organizations, ou_persistent22              
2Zhiwei Hu, Physics of Correlated Matter, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863461              

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 Abstract: Electronic structure modulation among multiple metal sites is key to the design of efficient catalysts. Most studies have focused on regulating 3d transition-metal active ions through other d-block metals, while few have utilized f-block metals. Herein, we report a new class of catalyst, namely, UCoO4 with alternative CoO6 and Sf-related UO6 octahedra, as a unique example of a 5f-covalent compound that exhibits enhanced electrocatalytic oxygen evolution reaction (OER) activity because of the presence of the U 5f-O 2p-Co 3d network. UCoO4 exhibits a low overpotential of 250 mV at 10 mA cm(-2), surpassing other unitary cobalt-based catalysts ever reported. X-ray absorption spectroscopy revealed that the Co(2+)ion in pristine UCoO4 was converted to high-valence Co3+/4+, while U6+ remained unchanged during the OER, indicating that only Co was the active site. Density functional theory calculations demonstrated that the OER activity of Co3+/4+ was synergistically enhanced by the covalent bonding of U6+-5f in the U 5f-O 2p-Co 3d network. This study opens new avenues for the realization of electronic structure manipulation via unique Sf involvement.

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Language(s): eng - English
 Dates: 2021-12-092021-12-09
 Publication Status: Published in print
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: -
 Identifiers: ISI: 000730264000001
DOI: 10.1021/jacs.1c10311
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Title: Journal of the American Chemical Society
  Other : JACS
  Abbreviation : J. Am. Chem. Soc.
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: - Sequence Number: - Start / End Page: 1 - 8 Identifier: ISSN: 0002-7863
CoNE: https://pure.mpg.de/cone/journals/resource/954925376870