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Interfacial Structure of Water as a New Descriptor of the Hydrogen Evolution Reaction
Author(s) -
Shen Linfan,
Lu Bangan,
Li Yuyang,
Liu Jia,
Huangfu Zhichao,
Peng Hao,
Ye Jinyu,
Qu Ximing,
Zhang Junming,
Li Guang,
Cai Wenbin,
Jiang Yanxia,
Sun Shigang
Publication year - 2020
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202007567
Subject(s) - dissociation (chemistry) , electrolyte , chemistry , catalysis , kinetics , molecule , adsorption , hydrogen bond , dangling bond , proton , self ionization of water , nanoparticle , hydrogen , chemical engineering , inorganic chemistry , electrode , organic chemistry , physics , engineering , quantum mechanics
Driven by the persisting poor understanding of the sluggish kinetics of the hydrogen evolution reaction (HER) on Pt in alkaline media, a direct correlation of the interfacial water structure and activity is still yet to be established. Herein, using Pt and Pt–Ni nanoparticles we first demonstrate a strong dependence of the proton donor structure on the HER activity and pH. The structure of the first layer changes from the proton acceptors to the donors with increasing pH. In the base, the reactivity of the interfacial water varied its structure, and the activation energies of water dissociation increased in the sequence: the dangling O−H bonds < the trihedrally coordinated water < the tetrahedrally coordinated water. Moreover, optimizing the adsorption of H and OH intermediates can re‐orientate the interfacial water molecules with their H atoms pointing towards the electrode surface, thereby enhancing the kinetics of HER. Our results clarified the dynamic role of the water structure at the electrode–electrolyte interface during HER and the design of highly efficient HER catalysts.