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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 
Wang, Shijie 
Wang, John 
Wee, Andrew T. S. 
Breese, Mark B. H. 
Pennycook, Stephen J. 
Venkatesan, Thirumalai 
Dong, Shuai
Xue, Jun Min 
Chen, Jingsheng 
Issue Date: 17-Jun-2018
Publisher: Nature Publishing Group
Citation: 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, Wang, Shijie, Wang, John, Wee, Andrew T. S., Breese, Mark B. H., Pennycook, Stephen J., Venkatesan, Thirumalai, Dong, Shuai, Xue, Jun Min, Chen, Jingsheng (2018-06-17). Electronic-reconstruction-enhanced hydrogen evolution catalysis in oxide polymorphs. NATURE COMMUNICATIONS 10. ScholarBank@NUS Repository.
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. � 2019, The Author(s).
ISSN: 2041-1723
DOI: 10.1038/s41467-019-11124-w
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