无掺杂石墨碳封装Fe_(3)C纳米颗粒的制备及其氧还原性能  

Fabrication of Fe_(3)C nanoparticles encapsulated in undoped graphite carbon and their catalysis for oxygen reduction

作　　者：于鑫浩 武军 于巾媛 王德强 何佳艺 胡静 谷俐 曹雪波 YU Xin-hao;WU Jun;YU Jin-yuan;WANG De-qiang;HE Jia-yi;HU Jing;GU Li;CAO Xue-bo(School of Materials Science and Engineering,Changzhou University,Changzhou 213164,China;College of Advanced Materials Engineering,Jiaxing Nanhu University,Jiaxing 314001,China;School of Materials and Textile Engineering,Jiaxing University,Jiaxing 314001,China;School of Biological and Chemical Engineering,Jiaxing University,Jiaxing 314001,China)

机构地区：[1]School of Materials Science and Engineering,Changzhou University,Changzhou 213164,China [2]College of Advanced Materials Engineering,Jiaxing Nanhu University,Jiaxing 314001,China [3]School of Materials and Textile Engineering,Jiaxing University,Jiaxing 314001,China [4]School of Biological and Chemical Engineering,Jiaxing University,Jiaxing 314001,China

出　　处：《Journal of Central South University》2023年第1期35-48,共14页中南大学学报（英文版）

基　　金：Project(2020AD10010) supported by the Public Welfare Research Project of Jiaxing city,China;Project(LQ19B030005) supported by the Natural Science Foundation of Zhejiang Province,China。

摘　　要：近年来,含氮金属碳化物氧还原反应(ORR)催化剂被广泛报道,但受到Fe_(x)N、N_(x)C和Fe纳米颗粒等多种反应活性位点的干扰,Fe_(3)C在催化过程中的具体作用尚不清楚。本文以Fe_(2)O_(3)纳米微球和细菌纤维素(BC)为原料,经热解得到了一种Fe_(3)C/C核壳催化剂。虽然被封装的无氮Fe_(3)C颗粒不接触电解液,但BC碳化后形成石墨层的ORR催化活性得到大幅提升。石墨层保护了内部碳化物,使其在酸性和碱性电解液中均表现出良好的催化活性和稳定性。该催化剂可作为理解此类无杂元素封装型催化剂ORR活性位点的模型系统。本文提出的碳化物催化剂及其作用机理为ORR催化剂的开发提供了新的思路。In recent years, nitrogenous metallic-complex catalysts for oxygen reduction reaction(ORR) have been extensively reported, but the exact role of Fe_(3)C in the catalytic process is not clear due to the interference of reactive sites such as Fe_(x)N, N_(x)C and Fe nanoparticles. In this work, a new type of pyrolysis catalyst Fe_(3)C-core/C-shell(Fe_(3)C/C) was designed using Fe_(2)O_(3) nanospheres and bacterial cellulose(BC) as raw materials. The encased nitrogen-free carbide isolated from the electrolyte, promoting the graphitic layers to form after BC carbonization toward high ORR catalytic activity, and the graphitic layers protected the internal carbide which exhibited excellent ORR activity and stability in both acidic and alkaline media. The catalyst was a model system for understanding the ORR active site of such encapsulated catalysts without other element doping. The carbide-based catalyst and mechanism proposed in this work provided a new idea for the development of ORR catalyst.

关 键 词：碳化铁 非贵金属电极催化剂 纳米结构 细菌纤维素 氧还原反应 

分 类 号：O643.36[理学—物理化学] TB383.1[理学—化学]