Engineering unsymmetrically coordinated Cu-S ₁N ₃ single atom sites with enhanced oxygen reduction activity

Abstract

Atomic interface regulation is thought to be an efficient method to adjust the performance of single atom catalysts. Herein, a practical strategy was reported to rationally design single copper atoms coordinated with both sulfur and nitrogen atoms in metal-organic framework derived hierarchically porous carbon (S-Cu-ISA/SNC). The atomic interface configuration of the copper site in S-Cu-ISA/SNC is detected to be an unsymmetrically arranged Cu-S ₁N ₃ moiety. The catalyst exhibits excellent oxygen reduction reaction activity with a half-wave potential of 0.918 V vs. RHE. Additionally, through in situ X-ray absorption fine structure tests, we discover that the low-valent Cuprous-S ₁N ₃ moiety acts as an active center during the oxygen reduction process. Our discovery provides a universal scheme for the controllable synthesis and performance regulation of single metal atom catalysts toward energy applications.

Abstract

Engineering the coordination environment of single atom catalysts offers to opportunity to optimize electrocatalytic activity. In this work, the authors prepare an unsymmetrical Cu-S ₁N ₃ single atom site on porous carbon with high performance in the oxygen reduction reaction.