Solvation at metal/water interfaces: An ab initio molecular dynamics benchmark of common computational approaches

Abstract

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The Sabatier Principle in Electrocatalysis: Basics, Limitations, and Extensions

“…Currently, continuum solvation models such as Vaspsol (Mathew et al, 2014(Mathew et al, , 2019, COSMO (Klamt and Schüürmann, 1993), or Jaguar (Bochevarov et al, 2013) are commonly used to describe solvation at the electrode/electrolyte interface (Abidi et al, 2020;Basdogan et al, 2020b;Groß, 2020). However at least in the case of the intermediates relevant to the ORR and CO 2 reduction reactions on Cu, Au, and Pt, the widely used continuum solvation models did not improve the accuracy of binding energies compared to the respective calculations in vacuum (Heenen et al, 2020). Due to the complexity and computational costs of AIMD, solvation models by the inclusion of machine-learning techniques have been developed (Basdogan et al, 2020b), which are a promising alternative to continuum solvation models.…”

Sulfate, Bisulfate, and Hydrogen Co-adsorption on Pt(111) and Au(111) in an Electrochemical Environment

“…In this manner we were able to construct (bi)sulfate adsorbate configurations with coverages between 0.05 and 0.33. To consider solvent effects we used an implicit solvation model (Petrosyan et al, 2005(Petrosyan et al, , 2007Letchworth-Weaver and Arias, 2012;Gunceler et al, 2013;Sakong et al, 2015;Bramley et al, 2020;Heenen et al, 2020) as implemented in the VASP code (Mathew et al, 2014). For the permittivity of the solvent we used the one of clean water (80 As Vm ).…”

Recent Progress in the Development of Screening Methods to Identify Electrode Materials for the Oxygen Evolution Reaction

“…Solvation effects are of crucial importance to the theoretical description of electrocatalytic processes. [94][95][96] Commonly, the effect of the surrounding electrolyte solution on the stabilization of adsorbates is completely neglected, described by computationally inexpensive continuum solvent models, or is assumed to be constant when screening electrodes in a homologous series of materials. All these procedures are incomplete, considering that solvation energies of adsorbates are not transferable between different surfaces and catalysts.…”

“…All these procedures are incomplete, considering that solvation energies of adsorbates are not transferable between different surfaces and catalysts. [96] Ab initio molecular dynamics (MD) simulations allow proper assessment of solvation energies, but this approach is very costly. Therefore, the inclusion of ab initio MD techniques for an improved assessment of solvent contributions to the stabilization of reaction intermediates, for example, the OH, O, and OOH adsorbates within oxygen electrocatalysis, may consist of a two-step scheme.…”