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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
- 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. Converting solar energy to hydrogen fuel requires light-absorbers that well-match the wavelengths of incoming sunlight. Here, authors prepare a broadband visible-light-absorbing molecular complex that efficiently produces hydrogen from water.
- Publication
Nature Communications, 2019, Vol 10, Issue 1, pN.PAG
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-019-11124-w