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Title: Electronic-reconstruction-enhanced hydrogen evolution catalysis in oxide polymorphs
Authors: Li, Yangyang
Yu, Zhi Gen
Wang, Ling
Weng, Yakui
Tang, Chi Sin
Yin, Xinmao
Han, Kun
Wu, Haijun
Yu, Xiaojiang
Wong, Lai Mun
Wan, Dongyang
Wang, Xiao Renshaw
Chai, Jianwei
Zhang, Yong-Wei
Wee, Andrew T. S.
Wang, Shijie
Wang, John
Breese, Mark B. H.
Pennycook, Stephen J.
Venkatesan, Thirumalai
Dong, Shuai
Xue, Jun Min
Chen, Jingsheng
Keywords: Electrocatalysis
Catalyst Synthesis
Issue Date: 2019
Source: Li, Y., Yu, Z. G., Wang, L., Weng, Y., Tang, C. S., Yin, X., . . . Chen, J. (2019). Electronic-reconstruction-enhanced hydrogen evolution catalysis in oxide polymorphs. Nature Communications, 10(1), 3149-. doi:10.1038/s41467-019-11124-w
Series/Report no.: Nature Communications
Abstract: Transition metal oxides exhibit strong structure-property correlations, which has been extensively investigated and utilized for achieving efficient oxygen electrocatalysts. However, high-performance oxide-based electrocatalysts for hydrogen evolution are quite limited, and the mechanism still remains elusive. Here we demonstrate the strong correlations between the electronic structure and hydrogen electrocatalytic activity within a single oxide system Ti2O3. Taking advantage of the epitaxial stabilization, the polymorphism of Ti2O3 is extended by stabilizing bulk-absent polymorphs in the film-form. Electronic reconstructions are realized in the bulk-absent Ti2O3 polymorphs, which are further correlated to their electrocatalytic activity. We identify that smaller charge-transfer energy leads to a substantial enhancement in the electrocatalytic efficiency with stronger hybridization of Ti 3d and O 2p orbitals. Our study highlights the importance of the electronic structures on the hydrogen evolution activity of oxide electrocatalysts, and also provides a strategy to achieve efficient oxide-based hydrogen electrocatalysts by epitaxial stabilization of bulk-absent polymorphs.
DOI: 10.1038/s41467-019-11124-w
Rights: © 2019 The Author(s). Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit
Fulltext Permission: open
Fulltext Availability: With Fulltext
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SPMS Journal Articles

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