摘要
石墨烯是一种新发现的碳纳米材料,比表面大,制备工艺简单,具有独特的物理和化学性能,已经成为纳米研究领域的一个新热点,尤其是在水处理方面有着巨大的潜力。
本文通过氧化还原法制备石墨烯并以氧化石墨为起点制备石墨烯负载金属(Graphene-Pt,Graphene-Cu)和金属氧化物(Graphene-Fe_3O_4,Graphene-MnO_2)纳米材料,并分别以它们为催化剂,对选定的内分泌干扰物2,4-二氯苯酚进行催化臭氧化降解性能研究。
以氧化石墨为基础,依据不同负载前驱体的特性,分别制备了不同金属和金属氧化物负载的石墨烯-铂、石墨烯-铜、石墨烯-Fe_3O_4和石墨烯-MnO2材料。采用X射线粉末衍射、拉曼光谱、X射线光电子能谱、热重分析、原子力显微镜、透射电镜等多种现代化测试仪器和方法对样品进行了结构和形貌表征。
催化降解性能研究表明,6.4wt%石墨烯-铂材料和石墨烯-Fe_3O_4做催化剂的催化臭氧化能力较强且高于石墨烯,说明石墨烯与金属铂或Fe_3O_4相结合对臭氧分解具有一定的催化协同作用。降解性能测试表明在相同条件下,不同的初始浓度降解率不同,浓度越低去除的越快。不同的pH条件对去除率也有影响,中性条件下的去除效果最好。石墨烯负载铜之后对2,4-二氯苯酚的去除率与石墨烯作催化剂的去除效果大体基本相同。石墨烯-多孔MnO2材料的催化臭氧化能力比石墨烯差,具有负催化效应。
Graphene, which have been one of the new hot spot in the nanomaterial field because of its large surface area, simple preparation methods, unique physical and chemical properties, is a newly discovered carbon nanomaterial, and especially it has great potential in water treatment.
The method of oxiding and reducing graphite is adopted to prepare graphene in this paper, and graphite oxide as the starting point of preparation of garaphene-metal (Graphene-Pt, Graphene-Cu) and graphene-metal oxides (Graphene-Fe_3O_4, Graphene-MnO_2) nanomaterials, and each of them as a catalyst on selected endocrine disrupting chemicals 2,4-dichlorophenol catalytic ozonation performance.
According to different charasteristics of precursors, the graphene with different metals and metal oxides load as graphene-platinum, graphene-copper, graphene-Fe_3O_4, graphene-MnO_2 were prepared by taking graphite oxide as the foundation. X-ray diffraction and Raman spectroscopy, X-ray photoelectron spectroscopy and thermal gravimetric analysis, atomic force microscopy, transmission electron microscopy and other modern test instruments and methods were characterized on the structure and the appearance attribute to the sample. Catalytic degradation experiment suggest that the abilities of the catalytic ozonation of 6.4wt% graphene-Pt and graphene-Fe_3O_4 catalytic material performance stronger and higher than the capacity of graphene, showing synergy in
catalytic decomposition of ozone after the combination of Fe_3O_4 or platinum. Degradati- on performance tests show that under the same conditions, different initial concentrations have the different degradation rates, the lower the faster the removal. Different pH conditions also affect the removal, removal under neutral conditions the best. Graphene after load of copper as a catalyst on the 2, 4–dichlorophenol removal behave the same as graphene. The Capability of catalytic ozonation of graphene– porous MnO_2 material is worse than graphene.
引文
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