摘要
我们通过简单的一步固相纳米铸造热解法,设计并合成了Fe-N双掺杂的有序介孔碳材料氧还原催化剂。我们采用经典的介孔二氧化硅作为硬模板,并首次以氨基酸作为唯一的碳源与氮源,将两种物质与含铁前驱体研磨均匀混合后直接焙烧,接着去除模版,最终得到具有高比表面积(1134 m~2/g)、二维六方介观结构、均一孔径(5.1 nm)、高含氮量(4.9 wt%)、高度石墨化的Fe/N掺杂有序介孔碳材料。在碱性条件下,所合成的催化剂具有很高的电催化氧还原活性,半波电位(-0.07 V vs Ag/AgCl)与极限电流均优于高活性的商业化Pt/C催化剂,并且具有很高的循环稳定性和化学耐受性。
Novel ordered mesoporous nitrogen/iron co-doped carbon(MN/Fe-C) catalysts have been rationally designed and synthesized by a simple solvent-free assembly method. In this facile method, mesoporous silicas were ground with amino acids and iron-containing precursor uniformly, followed by direct pyrolysis. In the resulted carbon materials, the ordered hexagonal mesostructures, high surface area(1134 m~2/g), ordered pore channels, and well-distributed Fe–Nx moieties embedded within the graphitic carbon backbones make them highly efficient for electro-catalyzing oxygen reduction reaction. The half-wave potential(-0.07 V vs Ag/AgCl) and the limited current density are both superior to commercial Pt/C catalysts. Furthermore, their excellent catalytic activity is extremely stable, and methanol-tolerant in alkaline conditions.
引文