He Zhimin, Wei Peng, Chen Ning, Han Jiantao, Lu Xing
State Key Laboratory of Materials Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, 430074, P.R. China.
Chemistry. 2021 Jan 18;27(4):1423-1429. doi: 10.1002/chem.202004535. Epub 2020 Dec 16.
The development of highly efficient metal-free electrocatalysts for the oxygen reduction reaction (ORR) has attracted great attention for the creation of electrochemical energy devices. In this study, one-dimensional (1 D) fullerene nanofibers prepared from liquid-liquid interfacial precipitation are first fabricated into fullerene-derived carbon nanofiber films (FCNFs) through a simple filtration procedure. Then, pyrolysis of the FCNFs in the presence of ammonia and sulfur produces N- and S-co-doped porous carbon nanofiber films (N,S-PCNFs). As excellent metal-free electrocatalysts for the ORR, N,S-PCNFs exhibit remarkable catalytic activity, superior stability, and excellent methanol tolerance in both alkaline and acidic solution. Such a high ORR performance benefits from the robust porous nanofiber network structure with high concentrations of active N- and S- groups and abundant defects. Notably, upon practical use of N,S-PCNFs as catalysts in Zn-air batteries, a high power density and a large operating voltage are achieved, with a performance comparable to that of the commercial Pt/C catalyst. This work presents a facile strategy for the creation of a new class of energy nanomaterials based on fullerenes, demonstrating their practical uses in electrocatalytic ORR processes and Zn-air batteries.
开发用于氧还原反应(ORR)的高效无金属电催化剂,对于创建电化学能源装置而言备受关注。在本研究中,首先通过简单的过滤程序,将由液-液界面沉淀法制备的一维(1D)富勒烯纳米纤维制成富勒烯衍生的碳纳米纤维膜(FCNFs)。然后,在氨和硫存在的情况下对FCNFs进行热解,制得氮和硫共掺杂的多孔碳纳米纤维膜(N,S-PCNFs)。作为用于ORR的优异无金属电催化剂,N,S-PCNFs在碱性和酸性溶液中均表现出显著的催化活性、卓越的稳定性以及出色的甲醇耐受性。如此高的ORR性能得益于具有高浓度活性氮和硫基团以及大量缺陷的坚固多孔纳米纤维网络结构。值得注意的是,当将N,S-PCNFs实际用作锌空气电池的催化剂时,可实现高功率密度和大工作电压,其性能与商业Pt/C催化剂相当。这项工作提出了一种基于富勒烯创建新型能源纳米材料的简便策略,证明了它们在电催化ORR过程和锌空气电池中的实际应用。