Ultra-small Fe2N nanocrystals embedded into mesoporous nitrogen-doped graphitic carbon spheres as a highly active, stable, and methanol-tolerant electrocatalyst for the oxygen reduction reaction

电催化剂 甲醇 材料科学 介孔材料 催化作用 化学工程 比表面积 纳米晶 无机化学 打赌理论 电化学 纳米技术 化学 有机化学 电极 物理化学 工程类
作者
Junwu Xiao,Yangyang Xu,Yating Xia,Jiangbo Xi,Shuai Wang
出处
期刊:Nano Energy [Elsevier]
卷期号:24: 121-129 被引量:139
标识
DOI:10.1016/j.nanoen.2016.04.026
摘要

Abstract A low-cost, highly active, stable, and methanol tolerant electrocatalyst towards the oxygen reduction reaction (ORR) is extremely desirable for promoting the commercialization of fuel cells. Herein, we reported a facile two-step pyrolysis and acid leaching process to synthesize a high performance ORR electrocatalyst, where ultra-small Fe2N nanocrystals were incorporated into mesoporous nitrogen-doped graphitic carbon spheres (MNGCS). The Fe2N/MNGCS electrocatalysts with difference Fe2N contents and BET surface areas were obtained via altering the acid leaching time, and all exhibited the apparent electrocatalytic activity. The optimized ORR activity was achieved over (Fe2N/MNGCS)4 with the positive half-wave potentials (0.881 V vs RHE), high selectivity (4 e− process), excellent long-term stability (95.2% of the initial current remaining after 60,000 s of continuous operation) and good tolerance against methanol-crossover effect (94.9% of the current retained prior to 4.0 M methanol injection) in alkaline media, which even was more superior to that of commercial Pt/C catalyst. The remarkable ORR activity was originated from the cooperative effect of ultra-small Fe2N nanocrystals and MNGCS, where the balance of catalytic active site density, mesoporous structure, BET specific surface area, and electron conductivity played a key role in determining the ORR performance.
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