Atomic Site-Specific Eigenstrain for Efficient Electrocatalysis

Abstract

Abstract Strain engineering is a powerful approach to tailoring the performance of metal electrocatalysts. Despite substantial advancements in controlling the average surface strain and establishing its correlation with catalytic activity, the impact of strain at individual active sites remains elusive. Here, we demonstrate the influence of site-specific strain on catalytic reactivity in Pt nanoclusters by quantitatively modulating and mapping the atomic-scale strain. We reveal a volcano-shaped relationship between eigenstrain─a descriptor of local anisotropic strain states─and intrinsic activity, confirmed through hydrogen electrocatalysis on Pt nanoclusters. Specifically, Pt atoms with optimal eigenstrain exhibit up to 2 orders of magnitude higher activity than strain-free sites, arising from electronic structure modification by inhomogeneous strain fields. These findings provide a quantitative framework for understanding site-specific strain phenomena and guide the rational design of strain-optimized metal catalysts.