期刊
SMALL
卷 16, 期 47, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202004342
关键词
heteroatom active sites; metal-free electrocatalysts; N, P, F self-doping; oxygen evolution reaction; oxygen reduction reaction
类别
资金
- National Natural Science Foundation of China [51773035]
- Shanghai Rising-Star Program [18QA1400200]
- Shanghai Scientific and Technological Innovation Project [18JC1410600]
The construction of multi-heteroatom-doped metal-free carbon with a reversibly oxygen-involving electrocatalytic performance is highly desirable for rechargeable metal-air batteries. However, the conventional approach for doping heteroatoms into the carbon matrix remains a huge challenge owing to multistep postdoping procedures. Here, a self-templated carbonization strategy to prepare a nitrogen, phosphorus, and fluorine tri-doped carbon nanosphere (NPF-CNS) is developed, during which a heteroatom-enriched covalent triazine polymer serves as a self-doping precursor with C, N, P, and F elements simultaneously, avoiding the tedious and inefficient postdoping procedures. Introducing F enhances the electronic structure and surface wettability of the as-obtained catalyst, beneficial to improve the electrocatalytic performance. The optimized NPF-CNS catalyst exhibits a superb electrocatalytic oxygen reduction reaction (ORR) activity, long-term durability in pH-universal conditions as well as outstanding oxygen evolution reaction (OER) performance in an alkaline electrolyte. These superior ORR/OER bifunctional electrocatalytic activities are attributed to the predesigned heteroatom catalytic active sites and high specific surface areas of NPF-CNS. As a demonstration, a zinc-air battery using the NPF-CNS cathode displays a high peak power density of 144 mW cm(-2) and great stability during 385 discharging/charging cycles, surpassing that of the commercial Pt/C catalyst.
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