Synthesis and ORR performance of nitrogen-doped ordered microporous carbon by CVD of acetonitrile vapor using silanized zeolite as template
Synthesis and ORR performance of nitrogen-doped ordered microporous carbon by CVD of acetonitrile vapor using silanized zeolite as template
复制标题
硅烷化沸石为模板乙腈蒸气CVD合成氮掺杂有序微孔碳及其ORR性能
DOI：
10.1016/j.apsusc.2019.144438
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发表时间：
2020
影响因子：
6.7
通讯作者：
An Baigang
中科院分区：
文献类型：
--
作者：
Zhao Hongwei;Li Lixiang;Liu Yuanyuan;Geng Xin;Yang Haiming;Sun Chengguo;An Baigang
采用简单的乙腈蒸汽一步气相沉积法制备了氮掺杂有序微孔碳，通过对沸石模板进行硅化处理，提高了碳在沸石孔壁上沉积的活性，利用气相沉积时间调节了分子筛的微观结构和含氮种类。采用XRD、n2吸附等温线、SEM、TEM和XPS表征了氮掺杂沸石模板碳（n- ztc）的组成、微观结构、比表面积(SSA)/孔分布和化学状态。通过电化学试验分析了样品作为ORR催化剂的性能。结果表明，在750 ℃、4 h的CVD条件下制备的N-ZTC （N-ZTC-4h）微孔有序，SSA大，含氮官能团丰富。作为无金属催化剂，N-ZTC-4h具有较高的ORR电流密度、良好的耐久性和优异的甲醇耐受性。N-ZTC-4h具有良好的ORR催化性能是由于其含有大量的含氮物质，具有较高的吡啶- n和季铵盐- n活性，且其微孔在三维空间上分布有序，便于质量传递。n - ztc制备工艺简单，孔隙结构和含氮种类控制方法简便，在开发氮掺杂碳基ORR催化剂方面具有很大的潜力。
A simple one-step CVD of acetonitrile vapor was successfully used to prepare nitrogen-doped ordered microporous carbon, where zeolite template was silanized to improve activity of carbon deposition into pore walls of the zeolite, CVD time was used to adjust microstructure and nitrogen containing species. XRD, N2adsorption isotherms, SEM, TEM and XPS were used to characterize the composition, microstructure, specific surface area (SSA)/pore distribution and chemical state of nitrogen-doped zeolite-templated carbons (N-ZTCs). Electrochemical tests were carried out to analyze the performance of samples as ORR catalyst. The results show that the N-ZTC as prepared at 750 °C with CVD time of 4 h (N-ZTC-4h) owns ordered micropores, large SSA and abundant nitrogen containing functional groups. As metal free catalyst, N-ZTC-4h exhibits high current density of ORR, good durability and excellent methanol tolerance. Good catalytic ORR performance of N-ZTC-4h is owed to a large quantity of nitrogen containing species with a high ratio of pyridinic-N and quaternary-N owning activity of ORR and the ordered microporous distribution in three-dimensions for mass transport. Easy preparation process and control method of pore structure and nitrogen containing species of N-ZTCs makes it have a big potential in developing nitrogen doped carbon based catalysts of ORR.