Understanding hydrogen electrocatalysis by probing the hydrogen-bond network of water at the electrified Pt–solution interface

Qiang Sun, Nicholas J. Oliveira, Soonho Kwon, Sergiy Tyukhtenko, Jason J. Guo, Nathalie Myrthil, Steven A. Lopez, Ian Kendrick, Sanjeev Mukerjee, Lu Ma, Steven N. Ehrlich, Jingkun Li (), William A. Goddard (), Yushan Yan () and Qingying Jia ()
Additional contact information
Qiang Sun: Northeastern University
Nicholas J. Oliveira: University of Delaware
Soonho Kwon: California Institute of Technology
Sergiy Tyukhtenko: Northeastern University
Jason J. Guo: Northeastern University
Nathalie Myrthil: Northeastern University
Steven A. Lopez: Northeastern University
Ian Kendrick: Northeastern University
Sanjeev Mukerjee: Northeastern University
Lu Ma: Brookhaven National Laboratory
Steven N. Ehrlich: Brookhaven National Laboratory
Jingkun Li: East China University of Science and Technology
William A. Goddard: California Institute of Technology
Yushan Yan: University of Delaware
Qingying Jia: Northeastern University

Nature Energy, 2023, vol. 8, issue 8, 859-869

Abstract: Abstract Rational construction of the electrode–solution interface where electrochemical processes occur is of paramount importance in electrochemistry. Efforts to gain better control and understanding of the interface have been hindered by lack of probing methods. Here we show that the hydrogen evolution and oxidation reactions (HER/HOR) catalysed by platinum in base can be promoted by introduction of N-methylimidazoles at the platinum–water interface. In situ spectroscopic characterization together with simulations indicate that the N-methylimidazoles facilitate diffusion of hydroxides across the interface by holding the second layer of water close to platinum surfaces, thereby promoting the HER/HOR. We thus propose that the HER/HOR kinetics of platinum in acid and base is governed by diffusion of protons and hydroxides, respectively, through the hydrogen-bond network of interfacial water by the Grotthuss mechanism. Moreover, we demonstrate a 40% performance improvement of an anion exchange membrane electrolyser by adding 1,2-dimethylimidazole into the alkali fed into its platinum cathode.

Date: 2023
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DOI: 10.1038/s41560-023-01302-y

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