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

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Wang, Xuesi, Xu, Chaochen, Jaroniec, Mietek, Zheng, Yao, Qiao, Shi-Zhang·2019·Nature Communications
DOI 10.1038/s41467-019-12773-7
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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 (H 3 O+) concentration in bulk phase, massive H 3 O+ intermediates are found generating on the catalytic surface during water dissociation and hydrogen adsorption processes. These H 3 O+ 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.

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Metadata

Authors
Wang, X., Xu, C., Jaroniec, M., Zheng, Y., & Qiao, S.-Z.
Venue
Nature Communications
Publisher
Springer Science and Business Media LLC
Published
2019-10-25
Volume
10
Issue
1
Pages
4876-4876
ISSN
2041-1723 (ISSN-L)
DOI
10.1038/s41467-019-12773-7
OpenAlex
W2982168748
Cited by
386
References
9
FWCI
8.40
Type
journal article
Language
en
Open access
gold
Licence

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CoChat. (2026). Citation check: Anomalous hydrogen evolution behavior in high-pH environment induced by locally generated hydronium ions. https://app.cochat.ai/papers/10.1038/s41467-019-12773-7
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Wang, X., Xu, C., Jaroniec, M., Zheng, Y., & Qiao, S.-Z. (2019). Anomalous hydrogen evolution behavior in high-pH environment induced by locally generated hydronium ions. Nature Communications. https://doi.org/10.1038/s41467-019-12773-7

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