Atomically Local Electric Field Induced Interface Water Reorientation for Alkaline Hydrogen Evolution Reaction

Angew Chem Int Ed Engl. 2023 Jun 26;62(26):e202300873. doi: 10.1002/anie.202300873. Epub 2023 Mar 30.

Abstract

The slow water dissociation process in alkaline electrolyte severely limits the kinetics of HER. The orientation of H2 O is well known to affect the dissociation process, but H2 O orientation is hard to control because of its random distribution. Herein, an atomically asymmetric local electric field was designed by IrRu dizygotic single-atom sites (IrRu DSACs) to tune the H2 O adsorption configuration and orientation, thus optimizing its dissociation process. The electric field intensity of IrRu DSACs is over 4.00×1010 N/C. The ab initio molecular dynamics simulations combined with in situ Raman spectroscopy analysis on the adsorption behavior of H2 O show that the M-H bond length (M=active site) is shortened at the interface due to the strong local electric field gradient and the optimized water orientation promotes the dissociation process of interfacial water. This work provides a new way to explore the role of single atomic sites in alkaline hydrogen evolution reaction.

Keywords: Alkaline HER; Atomic Charge Distribution; Interfacial Water Orientation; Single-Atom Site; Water Dissociation.

MeSH terms

  • Adsorption
  • Electricity*
  • Hydrogen*
  • Kinetics
  • Water

Substances

  • Hydrogen
  • Water