Singlet Oxygen Induced Site‐Specific Etching Boosts Nitrogen‐Carbon Sites for High‐Efficiency Oxygen Reduction
Guanying Ye, Suqin Liu, Kuangmin Zhao, Zhen He
Abstract
Abstract Targeted construction of carbon defects near the N dopants is an intriguing but challenging way to boost the electrocatalytic activity of N‐doped carbon toward oxygen reduction reaction (ORR). Here, we report a novel site‐specific etching strategy that features targeted anchoring of singlet oxygen ( 1 O 2 ) on the N‐adjacent atoms to directionally construct topological carbon defects neighboring the N dopants in N‐doped carbon ( 1 O 2 −N/C). This 1 O 2 −N/C exhibits the highest ORR half‐wave potential of 0.915 V RHE among all the reported metal‐free carbon catalysts. Pyridinic‐N bonded with a carbon pentagon of the neighboring topological carbon defects is identified as the primary active configuration, rendering enhanced adsorption of O 2 , optimized adsorption energy of the ORR intermediates, and a significantly decreased total energy barrier for ORR. This 1 O 2 ‐induced site‐specific etching strategy is also applicable to different precursors, showing a tremendous potential for targeted construction of high‐efficiency active sites in carbon‐based materials.