Recent Progress toward Ab Initio Modeling of Electrocatalysis

Abstract

Electrode potential is the key factor for controlling electrocatalytic reactions at electrochemical interfaces, and moreover, it is also known that the pH and solutes (e.g., cations) of the solution have prominent effects on electrocatalysis. Understanding these effects requires microscopic information on the electrochemical interfaces, in which theoretical simulations can play an important role. This Perspective summarizes the recent progress in method development for modeling electrochemical interfaces, including different methods for describing the electrolytes at the interfaces and different schemes for charging up the electrode surfaces. In the final section, we provide an outlook for future development in modeling methods and their applications to electrocatalysis.

Machine Learning: A New Paradigm in Computational Electrocatalysis

“…A hydroxide species is discovered to be dynamically confined in a solvated “pseudo-adsorption” state at ∼10 Å from the active site and therefore the pseudoadsorbed species are long-range coupled to the redox reaction at the catalytic center. Importantly, the long-range interactions and charge transfer play important roles in an electrochemical interface, in which electrocatalytic reactions occur. The third-generation (3G) HDNNPs could solve this issue, especially tackle the long-range electrostatic interactions, to some extent.…”

“…A hydroxide species is discovered to be dynamically confined in a solvated "pseudoadsorption" state at ∼10 Å from the active site and therefore the pseudoadsorbed species are long-range coupled to the redox reaction at the catalytic center. Importantly, the longrange interactions and charge transfer play important roles in an electrochemical interface, 61 such as ACSF could be used to describe the atomic environments, and the atomic charges will be obtained by atomic charge NNs. Then the Ewald sum could be used to compute the long-range electrostatic energy without truncation for periodic systems while for nonperiodic systems, Coulomb law can be used.…”

Realistic Modelling of Dynamics at Nanostructured Interfaces Relevant to Heterogeneous Catalysis

“…Similarly, the interface between oxides and water was assessed for systems of different natures-namely, silica [18,19], ZnO [20][21][22], goethite [23], and alumina [24,25]. In the field of electrocatalysis, the dynamics at electrified metal surface-water [26][27][28][29][30][31] and oxide surface-water [32,33] interfaces have also been recently modelled and characterized in detail.…”

Superhydrophilicity of α-alumina surfaces results from tight binding of interfacial waters to specific aluminols

“…[15,16] Investigating the behavior of interfacial waters is essential to help the design and development of better materials to overcome the energy crisis or increase their biological compatibility. [17,18,19,20,21] Among oxide surfaces, α-alumina (corundum), the most stable form of Al 2 O 3 , has wide applications in ceramics industries, [22] as catalyst supports [23] and as desiccants. [24] Interest in water/α-alumina interfaces has grown in recent years.…”