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Hollow-structured conjugated porous polymer derived Iron/Nitrogen-codoped hierarchical porous carbons as highly efficient electrocatalysts

机译:中空结构缀合多孔聚合物衍生铁/氮编码的等级多孔碳作为高效电催化剂

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摘要

Iron and nitrogen (Fe/N) co-doped porous carbons have already shown great potential as electrocatalysts for oxygen reduction reaction in alkaline media. However, it still remains a great challenge to finely integrate a hierarchical porous structure and Fe/N co-doping effect into one material at the same time. In this work, a rational design toward Fe/N-codoped hierarchical porous carbon spheres was developed by the formation of an iron-porphyrin-containing conjugated microporous polymer sphere with hollow structure (HCMP) through a silica sphere template directed condensation of pyrrole and 1,4-phthalaldehyde, then etched with NaOH, and treated with FeCl2. The resulting HCMP-Fe polymer was readily converted to a series of Fe/N co-doped hierarchical porous carbons (HPC-Fe/N-X, X = 700-900) upon pyrolysis at different temperatures and etching treatment. These porous carbons exhibit the high specific surface areas up to 518 m(2) g(-1) and the contents of N and Fe up to 3.28 at.% and 0.85 wt.%, respectively. Benefiting from the high surface area, Fe/N co-doping character, HPC-Fe/N-700 exhibited excellent electrochemical catalytic performance for oxygen reduction reaction under alkaline condition (0.1 M KOH) with a low half-wave potential (0.84 V), a dominant four-electron transfer mechanism (n = 3.89 at 0.65 V), as well as a high diffusion limiting current density (J(L) = 5.19 mA cm(-2)), comparable to those porous carbon-based ORR catalysts with excellent electrochemical performance. (C) 2017 Elsevier Inc. All rights reserved.
机译:铁和氮(铁/ N)共掺杂的多孔碳已经显示出巨大的潜力作为电催化剂用于在碱性介质中的氧还原反应。但是,它仍然在同一时间的分级多孔结构和Fe / N共掺杂效果精细地整合到一种材料的巨大挑战。在这项工作中,朝向的Fe /一个合理设计的N-共掺杂的分级多孔碳球通过吡咯和1的二氧化硅球模板定向缩合通过用中空结构(HCMP)含铁的卟啉的共轭微孔聚合物球的形成被开发,4-苯二醛,然后用NaOH刻蚀,用氯化亚铁处理。将所得HCMP - 铁聚合物容易转换成一系列的Fe / N共掺杂分级多孔碳的(HPC-的Fe / N-X,X = 700-900)后在不同温度下热解和蚀刻处理。这些多孔碳表现出高的比表面积达518米(2)克(-1)以及N和Fe至多3.28原子%和0.85%(重量),分别的内容。从高表面积受益,铁/ N共掺杂字符,HPC-的Fe / N-700表现出对具有低半波电势碱性条件(0.1M KOH)下的氧还原反应优异的电化学催化能力(0.84 V) ,显性四电子转移机制(N = 3.89 0.65 V),以及高的扩散极限电流密度(j(L)=5.19毫安厘米(-2)),与那些基于多孔碳的ORR催化剂具有优良的电化学性能。 (c)2017年Elsevier Inc.保留所有权利。

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  • 作者单位

    Shanghai Jiao Tong Univ Sch Chem &

    Chem Engn State Key Lab Met Matrix Composites Shanghai Key Lab Elect Insulat &

    Thermal Ageing Dongchuan Rd 800 Shanghai 200240 Peoples R China;

    Shanghai Jiao Tong Univ Sch Chem &

    Chem Engn State Key Lab Met Matrix Composites Shanghai Key Lab Elect Insulat &

    Thermal Ageing Dongchuan Rd 800 Shanghai 200240 Peoples R China;

    ShanghaiTech Univ iHuman Inst 100 Haike Rd Shanghai 201210 Peoples R China;

    Shanghai Jiao Tong Univ Sch Chem &

    Chem Engn State Key Lab Met Matrix Composites Shanghai Key Lab Elect Insulat &

    Thermal Ageing Dongchuan Rd 800 Shanghai 200240 Peoples R China;

    Shanghai Jiao Tong Univ Sch Chem &

    Chem Engn State Key Lab Met Matrix Composites Shanghai Key Lab Elect Insulat &

    Thermal Ageing Dongchuan Rd 800 Shanghai 200240 Peoples R China;

    East China Univ Sci &

    Technol Inst Appl Chem Key Lab Adv Mat 130 Meilong Rd Shanghai 200237 Peoples R China;

    East China Normal Univ Phys Dept North Zhongshan Rd 3663 Shanghai 200062 Peoples R China;

    Shanghai Jiao Tong Univ Sch Chem &

    Chem Engn State Key Lab Met Matrix Composites Shanghai Key Lab Elect Insulat &

    Thermal Ageing Dongchuan Rd 800 Shanghai 200240 Peoples R China;

    Shanghai Jiao Tong Univ Sch Chem &

    Chem Engn State Key Lab Met Matrix Composites Shanghai Key Lab Elect Insulat &

    Thermal Ageing Dongchuan Rd 800 Shanghai 200240 Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 表面现象的物理化学;胶体化学(分散体系的物理化学);
  • 关键词

    Conjugated microporous polymer; Hollow sphere; Fe/N-doping; Hierarchical porous carbon; Oxygen reduction reaction;

    机译:共轭微孔聚合物;中空球;Fe / N-掺杂;分层多孔碳;氧还原反应;

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