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  Searching General Sufficient-and-Necessary Conditions for Ultrafast Hydrogen-Evolving Electrocatalysis

Guan, D., Zhou, J., Hu, Z., Zhou, W., Xu, X., Zhong, Y., et al. (2019). Searching General Sufficient-and-Necessary Conditions for Ultrafast Hydrogen-Evolving Electrocatalysis. Advanced Functional Materials, 29: 1900704, pp. 1-8. doi:10.1002/adfm.201900704.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0003-BCAE-6 Version Permalink: http://hdl.handle.net/21.11116/0000-0003-BCF8-2
Genre: Journal Article

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 Creators:
Guan, Daqin1, Author
Zhou, Jing1, Author
Hu, Zhiwei2, Author              
Zhou, Wei1, Author
Xu, Xiaomin1, Author
Zhong, Yijun1, Author
Liu, Bo1, Author
Chen, Yuhui1, Author
Xu, Meigui1, Author
Lin, Hong-Ji1, Author
Chen, Chien-Te1, Author
Wang, Jian-Qiang1, Author
Shao, Zongping1, 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: active sites, hydrogen evolution reaction, non-noble metal perovskite oxides, ordered oxygen vacancies, oxygen 2p holes
 Abstract: The development of cost-effective and high-performance electrocatalysts for the hydrogen evolution reaction (HER) is one critical step toward successful transition into a sustainable green energy era. Different from previous design strategies based on single parameter, here the necessary and sufficient conditions are proposed to develop bulk non-noble metal oxides which are generally considered inactive toward HER in alkaline solutions: i) multiple active sites for different reaction intermediates and ii) a short reaction path created by ordered distribution and appropriate numbers of these active sites. Computational studies predict that a synergistic interplay between the ordered oxygen vacancies (at pyramidal high-spin Co 3+ sites) and the O 2p ligand holes (OLH; at metallic octahedral intermediate-spin Co 4+ sites) in RBaCo 2 O 5.5+ δ (δ = 1/4; R = lanthanides) can produce a near-ideal HER reaction path to adsorb H 2 O and release H 2 , respectively. Experimentally, the as-synthesized (Gd 0.5 La 0.5 )BaCo 2 O 5.75 outperforms the state-of-the-art Pt/C catalyst in many aspects. The proof-of-concept results reveal that the simultaneous possession of ordered oxygen vacancies and an appropriate number of OLH can realize a near-optimal synergistic catalytic effect, which is pivotal for rational design of oxygen-containing materials. © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

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Language(s): eng - English
 Dates: 2019-03-252019-03-25
 Publication Status: Published in print
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Method: -
 Identifiers: DOI: 10.1002/adfm.201900704
 Degree: -

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Title: Advanced Functional Materials
  Other : Adv. Funct. Mater.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH Verlag GmbH
Pages: - Volume / Issue: 29 Sequence Number: 1900704 Start / End Page: 1 - 8 Identifier: ISSN: 1616-301X
CoNE: https://pure.mpg.de/cone/journals/resource/954925596563