Catalytic Activity Maps for Alloy Nanoparticles

10 February 2022, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

To enable rational design of alloy nanoparticle catalysts, we develop an approach to generate catalytic activity maps of alloy nanoparticles on a grid of particle size and composition. The catalytic activity maps are created by using a quaternary cluster expansion to explicitly predict adsorbate binding energies on alloy nanoparticles of varying shape, size, and atomic order while accounting for interactions among the adsorbates. This cluster expansion is used in kinetic Monte Carlo simulations to predict nanoparticle structures and turnover frequencies on all surface sites. We demonstrate our approach on Pt–Ni octahedral nanoparticle catalysts for the oxygen reduction reaction (ORR), revealing the nanoparticle size and composition predicted to maximize ORR activity.

Keywords

rational design
intermetallic
solid-solution
cluster expansion
density functional theory
Pt–Ni catalysts
oxygen reduction reaction

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