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Singlet Oxygen Induced Site-Specific Etching Boosts Nitrogen-Carbon Sites for High-Efficiency Oxygen Reduction |
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| Authors: | Guanying Ye Prof. Suqin Liu Kuangmin Zhao Prof. Zhen He |
| Affiliation: | 1. College of Chemistry and Chemical Engineering, Central South University, 410083 Changsha, Hunan, P. R. China Contribution: Conceptualization (lead), Data curation (lead), Formal analysis (lead), Investigation (lead), Validation (lead), Writing - original draft (lead);2. College of Chemistry and Chemical Engineering, Central South University, 410083 Changsha, Hunan, P. R. China;3. College of Chemistry and Chemical Engineering, Central South University, 410083 Changsha, Hunan, P. R. China Contribution: Investigation (supporting), Validation (supporting) |
| 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 (1O2) on the N-adjacent atoms to directionally construct topological carbon defects neighboring the N dopants in N-doped carbon (1O2−N/C). This 1O2−N/C exhibits the highest ORR half-wave potential of 0.915 VRHE 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 O2, optimized adsorption energy of the ORR intermediates, and a significantly decreased total energy barrier for ORR. This 1O2-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. |
| Keywords: | Carbon Defect Electrocatalysis N-Doped Carbon ORR Targeted Etching |