Anomalous hydrogen evolution behavior in high-pH environment induced by locally generated hydronium ions

Xuesi Wang, Chaochen Xu, Mietek Jaroniec, Yao Zheng () and Shi-Zhang Qiao ()
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Xuesi Wang: The University of Adelaide
Chaochen Xu: The University of Adelaide
Mietek Jaroniec: Kent State University
Yao Zheng: The University of Adelaide
Shi-Zhang Qiao: The University of Adelaide

Nature Communications, 2019, vol. 10, issue 1, 1-8

Abstract: Abstract Most fundamental studies of electrocatalysis are based on the experimental and simulation results obtained for bulk model materials. Some of these mechanistic understandings are inapplicable for more active nanostructured electrocatalysts. Herein, considering the simplest and most typical electrocatalytic process, the hydrogen evolution reaction, an alternative reaction mechanism is proposed for nanomaterials based on the identification of a new intermediate, which differs from those commonly known for the bulk counterparts. In-situ Raman spectroscopy and electrochemical thermal/kinetic measurements were conducted on a series of nanomaterials under different conditions. In high-pH electrolytes with negligible hydronium (H3O+) concentration in bulk phase, massive H3O+ intermediates are found generating on the catalytic surface during water dissociation and hydrogen adsorption processes. These H3O+ intermediates create a unique acid-like local reaction environment on nanostructured catalytic surfaces and cut the energy barrier of the overall reaction. Such phenomena on nanostructured electrocatalysts explain their widely observed anomalously high activity under high-pH conditions.

Date: 2019
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DOI: 10.1038/s41467-019-12773-7

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