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  Electrocatalyst with Dynamic Formation of the Dual-Active Site from the Dual Pathway Observed by in Situ Raman Spectroscopy

Jing, C., Yuan, T., Li, L., Li, J., Qian, Z., Zhou, J., et al. (2022). Electrocatalyst with Dynamic Formation of the Dual-Active Site from the Dual Pathway Observed by in Situ Raman Spectroscopy. ACS Catalysis, 12(16), 10276-10284. doi:10.1021/acscatal.2c01038.

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 Creators:
Jing, Chao1, Author
Yuan, Taotao1, Author
Li, Lili1, Author
Li, Jianfeng1, Author
Qian, Zhengxin1, Author
Zhou, Jing1, Author
Wang, Yifeng1, Author
Xi, Shibo1, Author
Zhang, Nian1, Author
Lin, Hong-Ji1, Author
Chen, Chien-Te1, Author
Hu, Zhiwei2, Author           
Li, Da-Wei1, Author
Zhang, Linjuan1, Author
Wang, Jian-Qiang1, 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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Free keywords: cobalt hydroxide, in situ Raman spectroscopy, oxygen evolution reaction, reaction-rate dependent pathways, structural transformation
 Abstract: Understanding the catalysis mechanism of the sluggish oxygen evolution reaction (OER) involved in water splitting is of vital importance for the development of clean hydrogen energy. Earth-abundant transition-metal (oxy)hydroxide with low cost and high performance is one of the most promising OER catalysts. These catalysts often dynamically and heterogeneously transform from inactive pre-catalysts into active phases under operation conditions, and thus, the operando/in situ method is needed for the direct observation. Herein, using in situ Raman spectroscopy and density functional theory simulation, we correlate the OER activity with the dynamic crystal- and electronic-structure reconstruction of nano-sheet cobalt hydroxide. A complicated dual-transformation path is observed as the applied voltage is gradually increased; the pristine single-phase α-Co(OH)2 catalyst transforms into the hydrous Co(OH)2 phase through hydroxide intercalation, then to mixed β/γ-CoOOH phases through dehydration and dehydrogenation, and finally to OER-active γ-CoOOHx and β-CoOOHy. Moreover, the observed spectral and Tafel behaviors at different scan rates manifest the rate-dependent formation of the dual-active-phase, demonstrating the correlation between the OER ability and thermodynamics of structural reconstruction, which is critical in the fabrication of high-activity catalysts. © 2022 American Chemical Society. All rights reserved.

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Language(s): eng - English
 Dates: 2022-08-052022-08-05
 Publication Status: Published in print
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: -
 Identifiers: DOI: 10.1021/acscatal.2c01038
 Degree: -

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Title: ACS Catalysis
  Abbreviation : ACS Catal.
Source Genre: Journal
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Publ. Info: Washington, DC : ACS
Pages: - Volume / Issue: 12 (16) Sequence Number: - Start / End Page: 10276 - 10284 Identifier: ISSN: 2155-5435
CoNE: https://pure.mpg.de/cone/journals/resource/2155-5435