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氮掺杂有序介孔碳-Ni纳米复合材料的制备及电化学性能
引用本文:潘旭晨,汤静,薛海荣,郭虎,范晓莉,朱泽涛,何建平. 氮掺杂有序介孔碳-Ni纳米复合材料的制备及电化学性能[J]. 无机化学学报, 2013, 29(18)
作者姓名:潘旭晨  汤静  薛海荣  郭虎  范晓莉  朱泽涛  何建平
作者单位:南京航空航天大学材料科学与技术学院, 南京 210016;南京航空航天大学材料科学与技术学院, 南京 210016;南京航空航天大学材料科学与技术学院, 南京 210016;南京航空航天大学材料科学与技术学院, 南京 210016;南京航空航天大学材料科学与技术学院, 南京 210016;南京航空航天大学材料科学与技术学院, 南京 210016;南京航空航天大学材料科学与技术学院, 南京 210016
基金项目:国家自然科学基金(No.51372115)资助项目.
摘    要:以F127为模板剂,NiCl2为镍源,尿素为氮源,间苯二酚甲醛原位聚合树脂为碳源,分别采用均相法和两相法制备Ni-N-OMC-1,Ni-N-OMC-2纳米复合材料.X射线衍射(XRD)、激光拉曼以及透射电子显微镜(TEM)等测试结果表明,复合材料具有有序介孔结构,Ni以金属微粒形式嵌于碳骨架中,提高了有序介孔碳的石墨化程度.X射线光电子能谱测试(XPS)表明尿素热解后以4种形式存在:sp3杂化与C结合的N原子,吡啶N原子,sp2杂化与C结合的N原子以及quaternary-N原子.Ni-N的共改性改变了碳载体的理化性质,有利于Pt纳米粒子的负载与分散.均相法制备的Ni-N-OMC-1复合材料微波负载Pt后,氧还原极限电流密度为5.32mA·cm-2,氢氧化电化学活性面积高达138.53m2·g-1,电化学催化活性优于商业20%Pt/C材料(4.49mA·cm-2,96.98m2·g-1).

关 键 词:均相法  两相法  有序介孔碳  N-Ni复合掺杂  电催化活性

Synthesis and Electrocatalytic Performance of N-Doped Ordered Mesoporous Carbon-Ni Nanocomposite
PAN Xu-Chen,TANG Jing,XUE Hai-Rong,GUO Hu,FAN Xiao-Li,ZHU Ze-Tao and HE Jian-Ping. Synthesis and Electrocatalytic Performance of N-Doped Ordered Mesoporous Carbon-Ni Nanocomposite[J]. Chinese Journal of Inorganic Chemistry, 2013, 29(18)
Authors:PAN Xu-Chen  TANG Jing  XUE Hai-Rong  GUO Hu  FAN Xiao-Li  ZHU Ze-Tao  HE Jian-Ping
Affiliation:College of Material Science and Engineering, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China;College of Material Science and Engineering, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China;College of Material Science and Engineering, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China;College of Material Science and Engineering, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China;College of Material Science and Engineering, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China;College of Material Science and Engineering, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China;College of Material Science and Engineering, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China
Abstract:Highly ordered mesoporous carbon co-modified with Ni-Ncan be prepared via homogeneous phase route as well as dual-phase route, named as Ni-N-OMC-1 and Ni-N-OMC-2 respectively. Triblock copolymer Pluronic F127 were employed as the template agent, urea as the Nprecursor, NiCl2 as the Ni source and resorcinol-formaldehyde resin as the carbon precursor. X-ray diffraction (XRD), Raman, and transmission electron microscope (TEM) showed that nickel particles dispersed in the carbon matrix in forms of metal nickel, in situ catalyzing the graphitization of amorphous carbon. X-ray photoelectron spectroscopy (XPS) revealed that urea existed in four different Nspecies after heat treatment: sp3 nitrogen atoms bonded to carbon atoms, pyridine-like N, sp2 nitrogen atoms bonded to carbon atoms and quaternary-Natoms. The co-modification of nitrogen and nickel changed the physicochemical properties of carbon matrix, thus making for the loading and dispersing of Pt. Pt nanoparticles deposited on Ni-N-OMC-1 nanocompsite showed excellent electrocatalytic activity. The electrochemical active surface area of hydrogen oxidation was 138.53 m2·g-1 and the limiting current density in ORRwas 5.32 mA·cm-2, which indicated higher electrocatalytic ability than that of the commercial 20% Pt/Ccatalysts (4.49 mA·cm-2, 96.98 m2·g-1).
Keywords:homogeneous phase route  dual-phase route  ordered mesoporous carbon  co-modified with Ni-N  electrocatalytic activity
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