Explosion effect directly induced hierarchical carbon nanotube electrocatalyst integrated with Fe/Co dual sites for hydrogen fuel cells

Bolong Yang, Jingkui Hou, Yueyue Mi, Xiaogang Yu, Zhonghua Xiang
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Abstract

Atomically dispersed metal-site catalysts, especially those derived from high temperature calcination of zeolite-based imidazole salt framework (ZIFs), have great potential in catalyzing oxygen reduction reaction (ORR) with slow kinetics owing to their large atomic utilization and tunable coordination environment. However, ZIFs-derived carbon-based catalysts often exhibit octahedral particle morphology and thus complex post-treatment processes were usually required to modulate the pore structure of the membrane electrodes to enhance the utilization of metal-site sites in the cathode ORR of fuel cells. Herein, a highly efficient catalyst with Fe/Co dual metal sites anchored onto N-doped carbon nanotubes (CNTs) was synthesized by one-step calcination based on the explosion effect of ClO4- ion and Fe-Co bimetal coordination interaction, named FeCo-N-CNT. The introduction of ClO4- ions and Fe/Co bimetals gives the catalyst a dense reachable active site and a hierarchical porous structure. It is worth noting that the half-wave potential of the FeCo-N-CNT reached 0.9 V in an alkaline medium and showed good cyclic stability. More impressively, the FeCo-N-CNT also shows excellent ORR catalytic performance in both acid and neutral electrolytes, with a maximum power density 1.2 and 1.4 times higher than Fe-N-PC and Co-N-PC with single-metal sites in hydrogen fuel cells, respectively. This work provides a novel method for adjusting the structure of catalysts and improving the accessibility of metal-sites.

爆炸效应直接诱导的分层碳纳米管电催化剂与铁/钴双位点集成用于氢燃料电池
原子分散的金属基催化剂,尤其是沸石基咪唑盐框架(ZIFs)高温煅烧衍生的催化剂,由于其原子利用率大且配位环境可调,在催化动力学缓慢的氧还原反应(ORR)方面具有巨大潜力。然而,ZIFs 衍生的碳基催化剂通常呈现八面体颗粒形态,因此通常需要复杂的后处理过程来调节膜电极的孔隙结构,以提高燃料电池阴极 ORR 中金属位点的利用率。本文基于 ClO4- 离子和 Fe-Co 双金属配位相互作用的爆炸效应,通过一步煅烧合成了一种锚定在 N 掺杂碳纳米管(CNT)上的具有 Fe/Co 双金属位点的高效催化剂,命名为 FeCo-N-CNT。ClO4- 离子和 Fe/Co 双金属的引入使催化剂具有致密的可触及活性位点和分层多孔结构。值得注意的是,FeCo-N-CNT 在碱性介质中的半波电位达到 0.9 V,并表现出良好的循环稳定性。更令人印象深刻的是,FeCo-N-CNT 在酸性和中性电解质中也表现出优异的 ORR 催化性能,在氢燃料电池中的最大功率密度分别是单金属位点的 Fe-N-PC 和 Co-N-PC 的 1.2 倍和 1.4 倍。这项工作为调整催化剂结构和提高金属位点的可及性提供了一种新方法。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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