Rapid Interchangeable Hydrogen, Hydride, and Proton Species at the Interface of Transition Metal Atom on Oxide Surface

Wu, S. and Tseng, K.-Y. and Kato, R. and Wu, T.-S. and Large, A. and Peng, Y.-K. and Xiang, W. and Fang, H. and Mo, J. and Wilkinson, I. and Soo, Y.-L. and Held, G. and Suenaga, K. and Li, T. and Chen, H.-Y.T. and Tsang, S.C.E.

Volume: 143 Pages: 9105-9112
DOI: 10.1021/jacs.1c02859
Published: 2021

Hydrogen spillover is the phenomenon where a hydrogen atom, generated from the dissociative chemisorption of dihydrogen on the surface of a metal species, migrates from the metal to the catalytic support. This phenomenon is regarded as a promising avenue for hydrogen storage, yet the atomic mechanism for how the hydrogen atom can be transferred to the support has remained controversial for decades. As a result, the development of catalytic support for such a purpose is only limited to typical reducible oxide materials. Herein, by using a combination of in situ spectroscopic and imaging technique, we are able to visualize and observe the atomic pathway for which hydrogen travels via a frustrated Lewis pair that has been constructed on a nonreducible metal oxide. The interchangeable status between the hydrogen, proton, and hydride is carefully characterized and demonstrated. It is envisaged that this study has opened up new design criteria for hydrogen storage material. © 2021 American Chemical Society.

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