Journal
JOURNAL OF POWER SOURCES
Volume 549, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.jpowsour.2022.232122
Keywords
Coupling sites; Active sites; Metal-free carbon; Electrocatalysis; ORR catalysts
Funding
- National Natural Science Foundation of China
- Natural Science Foundation of Hunan Province
- Hunan Provincial Science and Technology Plan Project
- Postgraduate Scientific Research Innovation Project of Hunan Province
- [51972345]
- [22278444]
- [2021JJ30790]
- [2018RS3008]
- [2021zzts0065]
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The construction of synergistic coupling sites of intrinsic carbon defects and N dopants is crucial for enhancing the catalytic activities of metal-free carbon-based materials in the oxygen reduction reaction. Researchers have developed an etching-directed nitrogen doping strategy to construct carbon defect/N dopant coupling sites, where nitrogen is doped directionally at the freshly created intrinsic carbon defects during the synthesis of N-doped carbon. The resulting N-doped carbon catalyst with such coupling sites exhibits remarkable ORR catalytic activity and excellent long-term durability.
Construction of synergistic coupling sites of intrinsic carbon defects and N dopants in N-doped carbon is of great significance to improve the catalytic activities of metal-free carbon-based materials toward oxygen reduction reaction (ORR). However, the carbon-defect construction and N doping by existing strategies are usually inde-pendent processes, resulting in a random arrangement of the intrinsic carbon defects and N-dopants (i.e., hardly forming the coupling sites) in the resultant carbon materials. Herein, an etching-directed nitrogen doping strategy for constructing carbon defect/N dopant coupling sites is developed, in which nitrogen is directionally doped at the freshly created intrinsic carbon defects during the synthesis of N-doped carbon. The as-prepared N -doped carbon catalyst enriched with such coupling sites renders a remarkable ORR catalytic activity with an ORR half-wave potential of 0.891 V vs. RHE and an excellent long-term durability (3% current loss after 15,000 s at 0.6 V vs. RHE). Experimental characterizations and theoretical calculations reveal the formation mechanism of the coupling sites as well as the origin of their high catalytic activities toward ORR. This etching-directed ni-trogen doping strategy shows great universality for the controllable construction of active sites in carbon-based materials derived from different precursors for electrochemical energy storage and conversion applications.
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