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通过双氮掺杂获得的氮掺杂碳干凝胶对氧还原反应的电催化性能增强。

Enhanced electrocatalytic performance of N-doped carbon xerogels obtained through dual nitrogen doping for the oxygen reduction reaction.

作者信息

Jin Hong, Luo Yongping, Zhou Laihong, Xiao Zonghu, Zhang Fayun, Huang Ping, Liu Chen

机构信息

School of New Energy Science and Engineering, Xinyu University Xinyu Jiangxi 338004 China

School of Mechanical and Electrical Engineering, Xinyu University Xinyu Jiangxi 338004 China

出版信息

RSC Adv. 2022 May 4;12(21):13440-13447. doi: 10.1039/d2ra01238c. eCollection 2022 Apr 28.

Abstract

The development of high efficiency and low-cost electrocatalysts for the oxygen reduction reaction (ORR) is urgently desired for many energy storage and conversion systems. Nitrogen-doped carbon xerogels (NCXs) which have been successfully applied as effective electrocatalysts for the ORR have continued to attract attention due to their competitive price and tunable surface chemistry. A new dual N-doped NCX (NCoNC) electrocatalyst is fabricated as a carbon based catalyst though a facile impregnation of peptone in a precursor and ammonia etching pyrolysis method. XPS analysis demonstrates that the NCoNC electrocatalyst not only has a high N doping amount, but also has an optimized chemical state composition of N doping, which play an important role in improving the microstructure and catalytic performance of the catalysts. XRD and HRTEM results show that the doped metal nano-particles are coated with a double carbon layer of graphene carbon (inner layer) and amorphous carbon (outer layer) forming serrated edges that facilitate the ORR process. The as-obtained NCoNC catalyst exhibits good electrocatalytic performance and excellent stability for the ORR in both acidic and alkaline environments. In particular, in alkaline electrolyte, the decrements of both the limiting current density and the half-wave potential of the NCoNC catalyst were significantly lower than those of a commercial Pt/C catalyst during accelerated aging tests. When serving as an air electrode in Zn-air batteries, the catalyst also exhibits superior catalytic performance with a peak power density of 78.2 mW cm and a stable open-circuit voltage of 1.37-1.43 V. This work presents a novel tactic to regulate the microstructure and composition of carbon-based electrocatalysts by the facile and scalable dual-effect nitrogen doping method which may be conducive to promoting and developing highly efficient and promising electrocatalysts for the ORR.

摘要

许多能量存储和转换系统迫切需要开发用于氧还原反应(ORR)的高效低成本电催化剂。氮掺杂碳干凝胶(NCXs)作为ORR的有效电催化剂已成功应用,因其价格具有竞争力且表面化学性质可调,一直备受关注。通过将蛋白胨轻松浸渍在前体中并采用氨蚀刻热解方法,制备了一种新型双氮掺杂NCX(NCoNC)电催化剂作为碳基催化剂。X射线光电子能谱(XPS)分析表明,NCoNC电催化剂不仅具有高氮掺杂量,而且具有优化的氮掺杂化学态组成,这对改善催化剂的微观结构和催化性能起着重要作用。X射线衍射(XRD)和高分辨率透射电子显微镜(HRTEM)结果表明,掺杂的金属纳米颗粒被石墨烯碳(内层)和无定形碳(外层)的双碳层包覆,形成锯齿状边缘,有利于ORR过程。所制备的NCoNC催化剂在酸性和碱性环境中均表现出良好的电催化性能和优异的ORR稳定性。特别是在碱性电解质中,在加速老化测试期间,NCoNC催化剂的极限电流密度和半波电位的下降明显低于商业Pt/C催化剂。当用作锌空气电池的空气电极时,该催化剂还表现出优异的催化性能,峰值功率密度为78.2 mW/cm²,开路电压稳定在1.37 - 1.43 V。这项工作提出了一种新颖的策略,通过简便且可扩展的双效氮掺杂方法来调节碳基电催化剂的微观结构和组成,这可能有助于促进和开发用于ORR的高效且有前景的电催化剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0938/9067370/7fbd3ac45307/d2ra01238c-f1.jpg

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