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稳定封装在氮掺杂碳中的铂纳米晶体作为催化氧还原反应的双活性位点

Stabilizing Pt Nanocrystals Encapsulated in N-Doped Carbon as Double-Active Sites for Catalyzing Oxygen Reduction Reaction.

作者信息

Liu Jing, Li Wenqiang, Cheng Ruilin, Wu Qian, Zhao Jiahuan, He Daping, Mu Shichun

出版信息

Langmuir. 2019 Feb 19;35(7):2580-2586. doi: 10.1021/acs.langmuir.8b03947. Epub 2019 Feb 7.

Abstract

Polypropylene fiber, a cheap source of nitrogen-doped carbon, is introduced to design robust nitrogen-doped carbon-encapsulated small Pt nanocrystals with Pt and nitrogen-carbon double-active centers toward oxygen reduction reaction (ORR). Ascribed to the separation effect of the polypropylene fiber, even suffering from a high-temperature carbonization treatment at 720 °C for 90 min, the polypropylene fiber-derived carbon-encapsulated Pt nanocrystal maintains a small particle size (3 nm diameter on average). As expected, its ORR mass activity is up to 116.5 mA/mg at 0.9 V. After 8000 cycles, the half-wave potential of the prepared catalyst declines only by 14 mV compared with 43 mV for the commercial Pt/C catalyst. The significantly improved electrochemical properties of the as-prepared catalyst are resulted from the nitrogen-doped carbon-encapsulated Pt nanocrystal structure, which is benefited to adsorption and activation of oxygen due to the presence of nitrogen-doped carbon as the important active site for ORR besides Pt metal. In addition, the migration, aggregation, and growth of Pt nanoparticles are prohibited in terms of the outer nitrogen-doped carbon protection layer, greatly enhancing the stability of the catalyst.

摘要

引入廉价的氮掺杂碳源聚丙烯纤维,以设计具有铂和氮 - 碳双活性中心的坚固的氮掺杂碳包覆小铂纳米晶体,用于氧还原反应(ORR)。由于聚丙烯纤维的分离作用,即使在720℃下进行90分钟的高温碳化处理,聚丙烯纤维衍生的碳包覆铂纳米晶体仍保持较小的粒径(平均直径3nm)。正如预期的那样,其ORR质量活性在0.9V时高达116.5mA/mg。经过8000次循环后,制备的催化剂的半波电位仅下降14mV,而商业Pt/C催化剂下降43mV。所制备催化剂的电化学性能显著改善源于氮掺杂碳包覆铂纳米晶体结构,除了铂金属外,由于存在作为ORR重要活性位点的氮掺杂碳,有利于氧的吸附和活化。此外,外部氮掺杂碳保护层阻止了铂纳米颗粒的迁移、聚集和生长,大大提高了催化剂的稳定性。

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