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均一的 FeO/氮掺杂介孔碳球源自柠檬酸铁键合三聚氰胺树脂,作为高效协同氧还原催化剂。

Uniform FeO/Nitrogen-Doped Mesoporous Carbon Spheres Derived from Ferric Citrate-Bonded Melamine Resin as an Efficient Synergistic Catalyst for Oxygen Reduction.

机构信息

Key Laboratory of Material Chemistry for Energy Conversion and Storage (Huazhong University of Science and Technology), Ministry of Education, Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology , Wuhan, 430074, P.R. China.

出版信息

ACS Appl Mater Interfaces. 2017 Jan 11;9(1):335-344. doi: 10.1021/acsami.6b11608. Epub 2016 Dec 23.

Abstract

Developing a facile strategy to synthesize an efficient and inexpensive catalyst for the oxygen reduction reaction (ORR) is critical to the commercialization of many sustainable energy storage and conversion techniques. Herein, a novel and convenient strategy was presented to prepare FeO embedded into nitrogen-doped mesoporous carbon spheres (FeO/N-MCS) by the polycondensation between methylolmelamines and ammonium ferric citrate (AFC) and subsequent pyrolysis process. In particular, the polycondensation reaction was completely finished within a very short time (6.5 min), and the iron contents can be adjusted and had a great influence on the microstructure. Moreover, the FeO/N-MCS can be used as a robust catalyst for the ORR in alkaline media, and the catalyst with the iron content of 3.35 wt % exhibited excellent electrochemical performance in terms of more positive onset potential (E = 1.036 V vs RHE) and half-wave potential (E = 0.861 V) and much better methanol tolerance and long-term durability, in comparison with that of 20% Pt/C. The remarkable performance was ascribed to the characteristics of large specific surface area, mesoporous structure, high contents of pyridinic N and graphitic N, as well as strong electronic interaction between FeO and protective N-doped graphitic layers.

摘要

开发一种简便的策略来合成高效且廉价的氧气还原反应(ORR)催化剂对于许多可持续能源存储和转换技术的商业化至关重要。在此,提出了一种新颖且简便的策略,通过甲缩醛和柠檬酸铁铵(AFC)之间的缩聚反应以及随后的热解过程制备嵌入氮掺杂介孔碳球(FeO/N-MCS)中的 FeO。特别地,缩聚反应在很短的时间(6.5 分钟)内完全完成,并且铁含量可以进行调节,对微观结构有很大的影响。此外,FeO/N-MCS 可用作碱性介质中 ORR 的强大催化剂,铁含量为 3.35wt%的催化剂在起始电位(E=1.036 V vs RHE)和半波电位(E=0.861 V)更正、甲醇耐受性和长期耐久性方面表现出优异的电化学性能,优于 20%Pt/C。显著的性能归因于比表面积大、介孔结构、吡啶 N 和石墨 N 含量高以及 FeO 与保护性氮掺杂石墨层之间的强电子相互作用等特点。

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