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硫、痕量氮和铁共掺杂的分级多孔碳泡沫作为协同氧还原反应的催化剂。

Sulfur, trace nitrogen and iron codoped hierarchically porous carbon foams as synergistic catalysts for oxygen reduction reaction.

机构信息

Key Laboratory of Bio-inspired Smart Interfacial Science and Technology of Ministry of Education, School of Chemistry and Environment, Beihang University , Beijing 100191, People's Republic of China.

出版信息

ACS Appl Mater Interfaces. 2014 Dec 10;6(23):21454-60. doi: 10.1021/am506459f. Epub 2014 Nov 25.

Abstract

Sulfur, trace nitrogen and iron codoped, hierarchically porous carbon foams (HPCFs) were fabricated by directly pyrolyzing sulfur-enriched conductive polymer, poly(3,4-ethylenedioxythiphene)-polystyrenesulfonic acid (PEDOT-PSS) aerogels under argon atmosphere. This simple pyrolysis treatment results in the molecular rearrangement of heteroatom sulfur, adjacent carbons and trace nitrogen/iron from oxidants to form active catalytic sites of HPCFs. At the same time, the high porosity of HPCFs provides the large surface area for the uniform distribution of active sites, and allows rapid oxygen transport and diffusion. As a result, these HPCFs exhibit the enhanced catalytic performances for oxygen reduction reaction (ORR) via a direct four-electron reduction pathway in alkaline electrolyte. Besides, they also display a higher stability and better methanol/CO tolerance than the commercial Pt/C catalyst, which makes them promising low cost, non-precious-metal ORR catalysts for practical application in fuel cells and metal-air batteries.

摘要

硫、痕量氮和铁共掺杂的分级多孔碳泡沫(HPCF)是通过在氩气气氛下直接热解富硫导电聚合物聚(3,4-亚乙基二氧噻吩)-聚苯乙烯磺酸(PEDOT-PSS)水凝胶制备的。这种简单的热解处理导致杂原子硫、相邻碳和痕量氮/铁与氧化剂的分子重排,形成 HPCF 的活性催化位点。同时,HPCF 的高孔隙率为活性位点的均匀分布提供了大的表面积,并允许快速的氧气传输和扩散。结果,这些 HPCF 在碱性电解质中通过直接的四电子还原途径表现出增强的氧还原反应(ORR)催化性能。此外,它们还表现出比商业 Pt/C 催化剂更高的稳定性和更好的甲醇/CO 耐受性,这使得它们成为用于燃料电池和金属-空气电池的低成本、非贵金属 ORR 催化剂的有前途的候选材料。

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