期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 4, 期 19, 页码 7422-7429出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c6ta02419j
关键词
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资金
- National Basic Research Program of China (973 Program) [2012CB215500]
- National Natural Science Foundation of China [21373199, 21433003]
- Chinese Academy of Sciences [XDA09030104]
Developing highly active non-noble metal oxygen reduction reaction (ORR) catalysts is crucial for a variety of renewable energy applications including fuel cells and metal-air batteries. Heteroatom doped carbon materials, known as metal-free catalysts, show potential applications in the ORR, and may be promising replacement candidates for expensive, scarce platinum catalysts. Despite the inspiring progress made, the performance of the current metal-free carbon catalysts is still far from satisfactory for large-scale applications. Herein, we introduce an effective and robust ORR catalyst based on N, S co-doped carbon materials with abundant surface active sites. Electrochemical results indicate that the incorporation of sulfur into nitrogen-doped carbon (S-NCx) can dramatically improve the stability of the catalyst by improving the selectivity of O-2 electro-reduction to H2O. Density functional theory calculations reveal that sulfur doping lowers the energy barrier of O-2(ads) hydrogenation to form OOH(ads), thus leading to enhanced intrinsic activity. In particular, the correlation between ORR activity and nitrogen and sulfur species in these materials is studied in-depth, and it is found the ORR performance of S-NCx catalysts is significantly affected by pyridinic N and C-S-C contents.
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