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通过盐再结晶实现形态固定:将纳米结构聚合物转化为碳纳米材料的形态控制方法,作为氧还原反应的高效催化剂。

Shape Fixing via Salt Recrystallization: A Morphology-Controlled Approach To Convert Nanostructured Polymer to Carbon Nanomaterial as a Highly Active Catalyst for Oxygen Reduction Reaction.

机构信息

Chongqing Key Laboratory of Chemical Process for Clean Energy and Resource Utilization, School of Chemistry and Chemical Engineering, Chongqing University, Shazhengjie 174, Chongqing 400044, China.

出版信息

J Am Chem Soc. 2015 Apr 29;137(16):5414-20. doi: 10.1021/jacs.5b00292. Epub 2015 Apr 21.

Abstract

Herein, we report a "shape fixing via salt recrystallization" method to efficiently synthesize nitrogen-doped carbon material with a large number of active sites exposed to the three-phase zones, for use as an ORR catalyst. Self-assembled polyaniline with a 3D network structure was fixed and fully sealed inside NaCl via recrystallization of NaCl solution. During pyrolysis, the NaCl crystal functions as a fully sealed nanoreactor, which facilitates nitrogen incorporation and graphitization. The gasification in such a closed nanoreactor creates a large number of pores in the resultant samples. The 3D network structure, which is conducive to mass transport and high utilization of active sites, was found to have been accurately transferred to the final N-doped carbon materials, after dissolution of the NaCl. Use of the invented cathode catalyst in a proton exchange membrane fuel cell produces a peak power of 600 mW cm(-2), making this among the best nonprecious metal catalysts for the ORR reported so far. Furthermore, N-doped carbon materials with a nanotube or nanoshell morphology can be realized by the invented method.

摘要

本文报道了一种“通过盐再结晶固定形状”的方法,可有效地合成暴露于三相区的大量活性位的氮掺杂碳材料,用作 ORR 催化剂。通过 NaCl 溶液的再结晶,将具有 3D 网络结构的自组装聚苯胺固定并完全密封在 NaCl 内。在热解过程中,NaCl 晶体充当完全密封的纳米反应器,有利于氮的掺入和石墨化。在这样的封闭纳米反应器中气化会在所得样品中产生大量的孔。在溶解 NaCl 后,发现有利于传质和高利用活性位的 3D 网络结构被准确地转移到最终的氮掺杂碳材料中。在质子交换膜燃料电池中使用发明的阴极催化剂可产生 600 mW cm(-2) 的峰值功率,使其成为迄今为止报道的最佳非贵金属 ORR 催化剂之一。此外,通过该方法可以实现具有纳米管或纳米壳形态的氮掺杂碳材料。

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