Electronic-reconstruction-enhanced hydrogen evolution catalysis in oxide polymorphs

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Electronic-reconstruction-enhanced hydrogen evolution catalysis in oxide polymorphs
Title:
Electronic-reconstruction-enhanced hydrogen evolution catalysis in oxide polymorphs
Other Titles:
Nature Communications
Publication Date:
17 July 2019
Citation:
Li, Y., Yu, Z. G., Wang, L., Weng, Y., Tang, C. S., Yin, X., Han, K., Wu, H., Yu, X., Wong, L. M., Wan, D., Wang, X. R., Chai, J., Zhang, Y.-W., Wang, S., Wang, J., Wee, A. T. S., Breese, M. B. H., Pennycook, S. J., … Chen, J. (2019). Electronic-reconstruction-enhanced hydrogen evolution catalysis in oxide polymorphs. Nature Communications, 10(1). https://doi.org/10.1038/s41467-019-11124-w
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.
License type:
Attribution 4.0 International (CC BY 4.0)
Funding Info:
This research / project is supported by the National Research Foundation - Competitive Research Programme
Grant Reference no. : NRF-CRP10-2012-02

This research / project is supported by the A*STAR - AME Programmatic Fund
Grant Reference no. : A1898b0043

This research / project is supported by the Ministry of Education - Academic Research Fund Tier 1
Grant Reference no. : RG108/17

This research / project is supported by the National Research Foundation - Competitive Research Program
Grant Reference no. : NRF-CRP15-2015-01

This research / project is supported by the Ministry of Education - MOE Tier 2 programme
Grant Reference no. : MOE2018-T2-2-043

This research / project is supported by the A*STAR - Advanced manufacturing programme -individual research grant
Grant Reference no. : AMEIRG18-0022
Description:
ISSN:
2041-1723