A First-Principles Investigation of Goldene for Enhanced Hydrogen Evolution Reaction

TL;DR

This study uses first-principles calculations to analyze hydrogen adsorption on goldene, a novel 2D gold material, to evaluate its potential as an efficient catalyst for hydrogen evolution reactions.

Contribution

It provides the first theoretical investigation of hydrogen adsorption on goldene, including pristine, vacancy, and sulfur-functionalized variants, revealing key factors influencing HER activity.

Findings

Adsorption energies vary across different goldene variants.

Sulfur functionalization alters electronic properties and adsorption sites.

The study identifies optimal sites for hydrogen evolution on goldene.

Abstract

The recent synthesis of Goldene, a 2D sheet of gold exfoliated from $Ti_3AuC_2$, offers high specific surface area (~260 $m^2g^{-1}$), roughly twice that of fine nanodots (~100 $m^2g^{-1}$), and unique electronic properties due to its dense d-orbital. In this work, we investigate the adsorption of single atom catalyst (SAC) of hydrogen atom on pristine goldene (pG), monovacant goldene (vG), and sulfur-functionalized variants (thiol-pG and thiol-vG) using ab initio calculations. The adsorption energy of a single H atom and $\Delta G_H$, determines the efficiency of the Volmer step of the hydrogen evolution reaction (HER) and is a key descriptor for HER activity. We explore various potential sites for H adsorption and its impact on descriptors such as Bader charges, d-band shift and the exchange current density.