Single-Atom Alloy Catalysts Designed by First-Principles Calculations and Artificial Intelligence

TL;DR

This paper introduces a rapid, accurate method combining first-principles calculations and AI to predict and discover highly efficient single-atom alloy catalysts, significantly expanding the pool of potential industrial catalysts.

Contribution

It presents a compressed-sensing data-analytics approach that outperforms existing linear models for predicting SAAC catalytic properties, enabling discovery of over two hundred new promising candidates.

Findings

Validated predictions for known SAACs like Pd/Cu and Pt/Au.

Identified over 200 new promising SAAC candidates.

Demonstrated the importance of breaking linear relationships in catalyst design.

Abstract

Single-atom metal alloy catalysts (SAACs) have recently become a very active new frontier in catalysis research. The simultaneous optimization of both facile dissociation of reactants and a balanced strength of intermediates' binding make them highly efficient and selective for many industrially important reactions. However, discovery of new SAACs is hindered by the lack of fast yet reliable prediction of the catalytic properties of the sheer number of candidate materials. In this work, we address this problem by applying a compressed-sensing data-analytics approach parameterized with density-functional inputs. Our approach is faster and more accurate than the current state-of-the-art linear relationships. Besides consistently predicting high efficiency of the experimentally studied Pd/Cu, Pt/Cu, Pd/Ag, Pt/Au, Pd/Au, Pt/Ni, Au/Ru, and Ni/Zn SAACs (the first metal is the dispersed component), we identify more than two hundred yet unreported candidates. Some of these new candidates are predicted to exhibit even higher stability and efficiency than the reported ones. Our study demonstrates the importance of breaking linear relationships to avoid bias in catalysis design, as well as provides a recipe for selecting best candidate materials from hundreds of thousands of transition-metal SAACs for various applications.