Molecular Recognition Regulates Coordination Structure of Single‐Atom Sites

Abstract

AbstractCoordination engineering for single‐atom sites has drawn increasing attention, yet its chemical synthesis remains a tough issue, especially for tailorable coordination structures. Herein, a molecular recognition strategy is proposed to fabricate single‐atom sites with regulable local coordination structures. Specifically, a heteroatom‐containing ligand serves as the guest molecule to induce coordination interaction with the metal‐containing host, precisely settling the heteroatoms into the local structure of single‐atom sites. As a proof of concept, thiophene is selected as the guest molecule, and sulfur atoms are successfully introduced into the local coordination structure of iron single‐atom sites. Ultrahigh oxygen reduction electrocatalytic activity is achieved with a half‐wave potential of 0.93 V versus reversible hydrogen electrode. Furthermore, the strategy possesses excellent universality towards diversified types of single‐atom sites. This work makes breakthroughs in the fabrication of single‐atom sites and affords new opportunities in structural regulation at the atomic level.