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Urea-assisted synthesis of a Fe nanoparticle modified N-doped three-dimensional porous carbon framework for a highly efficient oxygen reduction reaction
New Journal of Chemistry ( IF 2.7 ) Pub Date : 2020-04-06 , DOI: 10.1039/c9nj06289k
Hui Peng 1, 2, 3, 4, 5 , Xuan Xie 1, 2, 3, 4, 5 , Kanjun Sun 5, 6, 7, 8 , Miaoran Zhang 1, 2, 3, 4, 5 , Rui Zhao 1, 2, 3, 4, 5 , Guofu Ma 1, 2, 3, 4, 5 , Ziqiang Lei 1, 2, 3, 4, 5
Affiliation  

Transition metals and heteroatom doped porous carbon materials have become sone of the most promising catalyst candidates to replace noble metal catalysts for high efficiency oxygen reduction reactions (ORR). Currently, however, the widely used hard templating method for preparing such materials is often complicated and expensive. Here, we develop a rapid gas foaming process to prepare a novel Fe nanoparticle modified N-doped three-dimensional porous carbon framework (Fe/3DNC) catalyst with a controllable microscopic morphology and catalytic efficiency by regulating the amount of urea. It is found that the optimized Fe/3DNC-2 catalyst has a high specific surface area (438 m2 g−1), hierarchically porous structure and homogeneous distribution of active sites (pyridinic N, graphitic N and FeNX). Thanks to the unique 3D framework architecture, the Fe/3DNC-2 catalyst exhibits a remarkable activity and long-term durability towards the ORR, such as a half-wave potential (E1/2 = 0.874 V vs. RHE) and onset potential (EOnset = 0.995 V vs. RHE) which is more positive than that of a commercial noble metal catalyst (20% Pt/C, E1/2 = 0.848 V, EOnset = 0.973 V) in an alkaline medium, and a half-wave potential with only a slight negative shift of approximately 7 mV after 5000 cycles.

中文翻译:

尿素辅助合成Fe纳米粒子修饰的N掺杂的三维多孔碳骨架,可实现高效的氧还原反应

过渡金属和杂原子掺杂的多孔碳材料已成为最有前途的候选催化剂,可以代替贵金属催化剂进行高效氧还原反应(ORR)。然而,目前,用于制备这种材料的广泛使用的硬模板方法通常是复杂且昂贵的。在这里,我们开发了一种快速的气体发泡工艺,通过调节尿素的量来制备具有可控的微观形态和催化效率的新型Fe纳米粒子修饰的N掺杂的N掺杂三维多孔碳骨架(Fe / 3DNC)催化剂。发现优化的Fe / 3DNC-2催化剂具有高的比表面积(438 m 2 g -1),层次结构的多孔结构和均匀分布的活性位点(吡啶氮,石墨氮和FeN X)。由于独特的3D框架结构,Fe / 3DNC-2催化剂对ORR具有出色的活性和长期耐久性,例如半波电势(E 1/2 = 0.874 V vs. RHE)和启动电势(E起始= 0.995 V相对于RHE )在碱性介质中比市售贵金属催化剂(20%Pt / C,E 1/2 = 0.848 V,E起始= 0.973 V)更具正性,并且半波电势,在5000次循环后仅出现约7 mV的轻微负移。
更新日期:2020-04-24
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