Electric Double Layer Effects in Electrocatalysis: Insights from Ab Initio Simulation and Hierarchical Continuum Modeling

JACS Au, vol. 3, pp. 2640–2659

Abstract

Structures of the electric double layer (EDL) at electrocatalytic interfaces, which are modulated by the material properties, the electrolyte characteristics (e.g., the pH, the types and concentrations of ions), and the electrode potential, play crucial roles in the reaction kinetics. Understanding the EDL effects in electrocatalysis has attracted substantial research interest in recent years. However, the intrinsic relationships between the specific EDL structures and electrocatalytic kinetics remain poorly understood, especially on the atomic scale. In this Perspective, we briefly review the recent advances in deciphering the EDL effects mainly in hydrogen and oxygen electrocatalysis through a multiscale approach, spanning from the atomistic scale simulated by ab initio methods to the macroscale by a hierarchical approach. We highlight the importance of resolving the local reaction environment, especially the local hydrogen bond network, in understanding EDL effects. Finally, some of the remaining challenges are outlined, and an outlook for future developments in these exciting frontiers is provided.

Authors 4

1. Peng Li

   Wuhan University

   Affiliation as printed

   Hubei Key Laboratory of Electrochemical Power Sources, College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, China

2. Yuzhou Jiao

   Wuhan University

   Affiliation as printed

   Hubei Key Laboratory of Electrochemical Power Sources, College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, China

3. Jun Zh. Huang corresponding Aachen Theory of Electrocatalytic Interfaces Faculty of Georesources and Materials Engineering

   Forschungszentrum Jülich · RWTH Aachen University

   Affiliation as printed

   Institute of Energy and Climate Research, IEK-13: Theory and Computation of Energy Materials, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany

   Theory of Electrocatalytic Interfaces, Faculty of Georesources and Materials Engineering, RWTH Aachen University, 52062 Aachen, Germany

4. Shengli Chen corresponding

   Wuhan University

   Affiliation as printed

   Hubei Key Laboratory of Electrochemical Power Sources, College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, China