【作者】 张怡；

【导师】 苏跃增； 冯新亮；

【作者基本信息】 上海交通大学 ， 航空工程， 2014， 硕士

【摘要】 杂原子掺杂的碳材料，作为一种高燃料选择性、耐CO毒性、长时间工作稳定的新型氧还原电催化剂，吸引了无数研究者的目光。目前通过多种手段如化学气相沉积、水热、高温热解、等离子体处理等已实现杂原子掺杂碳材料的制备。本文主要选用氧化石墨烯、活性炭作为主要碳原材料，通过多种手段将杂原子掺杂进碳骨架中，制备了氮硫共掺杂三维石墨烯气凝胶、硼氮共掺杂二维多孔碳材料、氮掺杂活性炭，并对这些材料进行了相关表征。具体研究内容为：（1）使用硫氰酸铵作为氮源、硫源，利用硫氰酸铵在180℃时会分解产生氨气、硫化氢的特点，在水热过程中将杂原子掺杂到氧化石墨烯碳骨架中。水热过程中，氧化石墨烯被还原。研究结果表明，氮、硫原子被均匀的掺杂到了石墨烯骨架中，所制备的材料具有较高的比表面积，氧还原电催化表征表明材料具有优异的电催化性能。（2）使用氨基苯硼酸半硫酸盐、苯胺、间苯二胺为单体，苯胺功能化的氧化石墨烯为基底，将聚合物包裹在氧化石墨烯外，形成二维多孔聚合物。以此为原料，对材料进行高温热解、二氧化碳活化等热处理，最终获得具有高比表面积的二维石墨烯基硼氮共掺杂碳材料。所得材料经过表征，证明具有出色的氧还原电催化活性。（3）使用活性炭作为碳源，通过氨气活化，在提高比表面积的同时将氮原子引入碳骨架中，获得高比表面积碳掺杂材料。经过表征，所得材料具有超高比表面积和优异的氧还原电催化活性。更多还原

【Abstract】 Doped carbon materials, as a kind materials with high fuel selectivity,anti-CO toxicity, long stability on ORR catalysis application, have drawmany attention. To realize the heteroatom doping, many methods havebeen presented such as chemical vapor deposition, hydrothermal, pyrolysis.In this paper, we prepare the heteratom doped carbon aergoels,2Dnanosheets and high specify surface area activatied carbon by usinghydrothermal, pyrolysis and carbon dioxide activation, respectively. Thedetails are as follows:(1) We apply ammonium thiocyanate as the sulfur&nitrogen source,for the characteristic of the salt that ammonium thiocyanate decomposes toammonia, hydrogen sulfide during hydrothermal process. During thehydrothermal process, doped atoms can be doped into graphene oxideframework sucessfully, and graphene oxide is also reduced. The resultsshow that nitrogen, sulfur atoms are uniformly distributed in the grapheneframwork. The high specific surface area and doped atoms result to anexcellent oxygen reduction electrocatalytic characterization.(2) Two dimensional graphene based polymer have beenmanufactured by using3-Aminobenzeneboronic acid hemisulfate salt,aniline and m-phenylenediamine as monomers, aniline functionalizedgraphene oxide as substrate. The polymer wrapped up the anilinefunctionalized graphene oxide. The product after polymerzation is used asthe raw material of thermal treatment. After pyrolysis and carbon dioxideactivation, we fabricate a kind of new two dimensional graphene basedboron and nitrogen co-doped carbon with a high specific surface area. Theresulting materials have been characterized with ORR test and shown an excellent electrocatalytic activity.(3) In this work, activated carbon is used as raw materials. We useammonia to activate the materials in high temperature. During thepyrolysis process, the specific surface area increase, while nitrogen atomsare doped into carbon framwork. The resulting material shows a ultra-highspecific surface area and excellent electrocatalytic activity for oxygenreduction.更多还原