Identification of Intersite Distance Effects in Au-Ag Single-Atom Alloy Catalysts Using Single Nanoparticle Collision Electrochemistry.

ABSTRACT

Regulating the atomic density of single-atom alloys (SAAs) promotes the potential to significantly enhance the electrocatalytic activity. However, conventional methods for study on the electrocatalytic performance of SAAs versus the intersite distance demand exhaustive experiments and characterization. Herein, we present a combinatorial synthesis and analysis method to investigate the intersite distance effect of SAA electrocatalysts. We employ single-nanoparticle collision electrochemistry to realize in situ electrodeposition of a precisely tunable Au atomic density onto individual parent Ag nanoparticles, followed by instantaneous electrocatalytic measurement of the newborn Au-Ag SAAs. In this work, the utility of our method is confirmed by the identification of intersite distance effects of Au-Ag SAAs toward the oxygen reduction reaction. When the site distance between two neighboring Au atoms is 1.9 nm, Au-Ag SAAs exhibit optimal activity. This work provides a simple and efficient method for screening other SAA electrocatalysts with ideal intersite distance at the single-nanoparticle level.