摘要

The catalytic activity of main‐group metal is hard to promote because of the intrinsic lack of host d orbitals available to be combined. Herein, under the guidance of theoretical predictions, we find atom‐dispersed antimony sites (Sb?N4 moieties) can be activated to achieve high oxygen reduction reaction (ORR) activity using a functional group regulation strategy. Correspondingly, we manage to synthesize a main‐group Sb single‐atom catalysts (SACs) that comprises Sb?N4 active moieties functionalized by epoxy groups in the second microenvironment and incorporated in N‐doped graphene (Sb1/NG(O)). The electron‐rich epoxy group can adjust the electronic structure of Sb?N4 active moieties, thereby optimizing the adsorption of the intermediate. The Sb SACs are comparable to industrial Pt/C under alkaline conditions. This discovery provides new opportunities to manipulate and improve the catalytic activity of main‐group‐element electrocatalysts.(#br)Single antimony sites functionalized by epoxy groups in N‐doped graphene were designed to activate the oxygen reduction reaction (ORR). The electron‐rich epoxy group can adjust the electronic structure of the Sb?N4 active moieties, optimizing the adsorption of the intermediates to approach the top of the volcano plot. This discovery provides new way to improve the catalytic activity of main‐group‐element electrocatalysts.

  • 单位
    晶体材料国家重点实验室