Predictive model of surface adsorption in dissolution on transition metals and alloys

TL;DR

This paper develops a predictive model for surface adsorption during dissolution on transition metals and alloys, using electronic and cohesive properties to understand alloying effects and guide catalyst design.

Contribution

It introduces a novel model based on electronic gradients and cohesive properties to predict adsorption energies on various alloys, revealing mechanisms behind alloying effects.

Findings

Model accurately predicts adsorption energies across alloy types.

Uncovers synergistic effects of d-band and s-band properties on adsorption.

Provides insights for designing advanced alloy catalysts.

Abstract

Surface adsorption, which is often coupled with surface dissolution, is generally unpredictable on alloys due to the complicated alloying and dissolution effects. Herein, we introduce the electronic gradient and cohesive properties of surface sites to characterize the effects of alloying and dissolution. This enables us to build a predictive model for the quantitative determination of the adsorption energy in dissolution, which holds well for transition metals, near-surface alloys, binary alloys, and high-entropy alloys. Furthermore, this model uncovers a synergistic mechanism between the d-band upper-edge ratio, d-band width and s-band depth in determining the alloying and dissolution effects on adsorption. Our study not only provides fundamental mechanistic insights into surface adsorption on alloys but also offers a long-sought tool for the design of advanced alloy catalysts.