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Sustainable Hydrothermal Carbonization Synthesis of Iron/Nitrogen-Doped Carbon Nanofiber Aerogels as Electrocatalysts for Oxygen Reduction

机译:铁/氮掺杂碳纳米纤维气凝胶作为氧还原电催化剂的可持续水热碳化合成

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摘要

It is urgent to develop new kinds of low-cost and high-performance nonprecious metal (NPM) catalysts as alternatives to Pt-based catalysts for oxygen reduction reaction (ORR) in fuel cells and metal-air batteries, which have been proved to be efficient to meet the challenge of increase of global energy demand and CO2 emissions. Here, an economical and sustainable method is developed for the synthesis of Fe, N codoped carbon nanofibers (Fe-N/CNFs) aerogels as efficient NPM catalysts for ORR via a mild template-directed hydrothermal carbonization (HTC) process, where costeffective biomass-derived d(+)-glucosamine hydrochloride and ferrous gluconate are used as precursors and recyclable ultrathin tellurium nanowires are used as templates. The prepared Fe/N-CNFs catalysts display outstanding ORR activity, i.e., onset potential of 0.88 V and half-wave potential of 0.78 V versus reversible hydrogen electrode in an alkaline medium, which is highly comparable to that of commercial Pt/C (20 wt% Pt) catalyst. Furthermore, the Fe/N-CNFs catalysts exhibit superior long-term stability and better tolerance to the methanol crossover effect than the Pt/C catalyst in both alkaline and acidic electrolytes. This work suggests the great promise of developing new families of NPM ORR catalysts by the economical and sustainable HTC process.
机译:迫切需要开发出新型的低成本高性能非贵金属(NPM)催化剂,以替代用于燃料电池和金属空气电池中氧还原反应(ORR)的Pt基催化剂。高效应对全球能源需求和二氧化碳排放量增加的挑战。在这里,通过一种温和的模板导向水热碳化(HTC)工艺,开发了一种经济,可持续的方法来合成Fe,N共掺杂的碳纳米纤维(Fe-N / CNFs)气凝胶,作为ORR的有效NPM催化剂,在该工艺中,具有成本效益的生物质衍生的d(+)-氨基葡萄糖盐酸盐和葡萄糖酸亚铁用作前体,而可回收的超薄碲纳米线用作模板。制备的Fe / N-CNFs催化剂显示出出色的ORR活性,即在碱性介质中相对于可逆氢电极的起始电势为0.88 V,半波电势为0.78 V,与商业化的Pt / C相当(20 wt%Pt)催化剂。此外,在碱性和酸性电解质中,Fe / N-CNFs催化剂均比Pt / C催化剂表现出优异的长期稳定性和对甲醇穿越效果的更好耐受性。这项工作表明通过经济且可持续的HTC工艺开发新的NPM ORR催化剂系列的巨大前景。

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