Electronic-reconstruction-enhanced hydrogen evolution catalysis in oxide polymorphs

Yangyang Li, Zhi Gen Yu, Ling Wang, Yakui Weng, Chi Sin Tang, Xinmao Yin, Kun Han, Haijun Wu, Xiaojiang Yu, Lai Mun Wong, Dongyang Wan, Xiao Renshaw Wang, Jianwei Chai, Yong-Wei Zhang, Shijie Wang, John Wang, Andrew T. S. Wee, Mark B. H. Breese, Stephen J. Pennycook, Thirumalai Venkatesan, Shuai Dong, Jun Min Xue and Jingsheng Chen ()
Additional contact information
Yangyang Li: National University of Singapore
Zhi Gen Yu: Institute of High Performance Computing
Ling Wang: National University of Singapore
Yakui Weng: Nanjing University of Posts and Telecommunications (NUPT)
Chi Sin Tang: National University of Singapore
Xinmao Yin: National University of Singapore
Kun Han: Nanyang Technological University
Haijun Wu: National University of Singapore
Xiaojiang Yu: National University of Singapore
Lai Mun Wong: A*STAR (Agency for Science, Technology and Research)
Dongyang Wan: National University of Singapore
Xiao Renshaw Wang: Nanyang Technological University
Jianwei Chai: A*STAR (Agency for Science, Technology and Research)
Yong-Wei Zhang: Institute of High Performance Computing
Shijie Wang: A*STAR (Agency for Science, Technology and Research)
John Wang: National University of Singapore
Andrew T. S. Wee: National University of Singapore
Mark B. H. Breese: National University of Singapore
Stephen J. Pennycook: National University of Singapore
Thirumalai Venkatesan: National University of Singapore
Shuai Dong: Southeast University
Jun Min Xue: National University of Singapore
Jingsheng Chen: National University of Singapore

Nature Communications, 2019, vol. 10, issue 1, 1-11

Abstract: 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.

Date: 2019
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DOI: 10.1038/s41467-019-11124-w

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