Interfacial electron transfer governs electrochemical heterogeneity at the single-entity level.Herein,we investigated the electronic coupling event during electrodissolution processes of single silver nanoentities on ...Interfacial electron transfer governs electrochemical heterogeneity at the single-entity level.Herein,we investigated the electronic coupling event during electrodissolution processes of single silver nanoentities on a Au electrode through a synchronized electrochemical-optical tracking platform.By implementing strategic control of interfacial gap distances and electrolyte composition,a marked differentiation of single-particle reaction dynamics can be achieved.The integration of superlocalization methodology reveals position-correlated optical centroid shifts during electrodissolution processes,demonstrating heterogeneous oxidation dynamics arising from spatially nonuniform surface oxide formation.Crucially,SAMmediated gap regulation enables the precise regulation of interfacial electric field enhancement.Our methodology resolves electronic coupling heterogeneity at subnanowire scale while proving molecular interlayer-dependent modulation of coupling lifetimes.This electrochemical-optical imaging strategy establishes nanoscale spatial mapping of electrochemical dynamics,quantitative correlation between interfacial structure and coupling efficiency,and real-time tracking of transient electronic states.These findings demonstrate the capability of advanced optical imaging methodologies in elucidating structure−activity relationships at nanoscale interfaces,providing mechanistic insights for single-entity electrochemistry and nanoscale energy conversion systems.展开更多
基金National Natural Science Foundation of China(NSFC,Grant Number:22222406,22174062).
文摘Interfacial electron transfer governs electrochemical heterogeneity at the single-entity level.Herein,we investigated the electronic coupling event during electrodissolution processes of single silver nanoentities on a Au electrode through a synchronized electrochemical-optical tracking platform.By implementing strategic control of interfacial gap distances and electrolyte composition,a marked differentiation of single-particle reaction dynamics can be achieved.The integration of superlocalization methodology reveals position-correlated optical centroid shifts during electrodissolution processes,demonstrating heterogeneous oxidation dynamics arising from spatially nonuniform surface oxide formation.Crucially,SAMmediated gap regulation enables the precise regulation of interfacial electric field enhancement.Our methodology resolves electronic coupling heterogeneity at subnanowire scale while proving molecular interlayer-dependent modulation of coupling lifetimes.This electrochemical-optical imaging strategy establishes nanoscale spatial mapping of electrochemical dynamics,quantitative correlation between interfacial structure and coupling efficiency,and real-time tracking of transient electronic states.These findings demonstrate the capability of advanced optical imaging methodologies in elucidating structure−activity relationships at nanoscale interfaces,providing mechanistic insights for single-entity electrochemistry and nanoscale energy conversion systems.
