4.8 Article

Engineering a Local Free Water Enriched Microenvironment for Surpassing Platinum Hydrogen Evolution Activity

期刊

出版社

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202206077

关键词

Electrochemical Double Layer; High Current Densities; Hydrogen Evolution; Local Hydrogen Bond; Surface Hydroxyl

资金

  1. National Natural Science Foundation of China [22071069, 21825103, 11904353]
  2. Foundation of Basic and Applied Basic Research of Guangdong Province [2019B1515120087]
  3. Analytical and Testing Center in Huazhong University of Science and Technology

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In this study, we propose a method of manipulating the catalyst-electrolyte interface to enhance alkaline hydrogen evolution activity by introducing local force fields through surface hydroxyl groups. We show that the local hydrogen bond induced by the surface hydroxyl group can drag H2O molecules across the inner Helmholtz plane (IHP) to continuously supply reactants to catalytic sites. Additionally, the hydroxyl group coupled with the Ni/Ni3C heterostructure lowers the water dissociation energy by polarization effects. As a result, hydroxyl-rich catalysts exhibit higher activity than Pt/C at high current density in alkaline medium.
Manipulating the catalyst-electrolyte interface to push reactants into the inner Helmholtz plane (IHP) is highly desirable for efficient electrocatalysts, however, it has rarely been implemented due to the elusive electrochemical IHP and inherent inert catalyst surface. Here, we propose the introduction of local force fields by the surface hydroxyl group to engineer the electrochemical microenvironment and enhance alkaline hydrogen evolution activity. Taking a hydroxyl group immobilized Ni/Ni3C heterostructure as a prototype, we reveal that the local hydrogen bond induced by the surface hydroxyl group drags 4-coordinated hydrogen-bonded H2O molecules across the IHP to become free H2O and thus continuously supply reactants forcatalytic sites catalytic sites. In addition, the hydroxyl group coupled with the Ni/Ni3C heterostructure further lowers the water dissociation energy by polarization effects. As a direct outcome, hydroxyl-rich catalysts surpass Pt/C activity at high current density (500 mA cm(-2) @ approximate to 276 mV) in alkaline medium.

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