金属改性有序杂化介孔碳材料的制备及其对燃油吸附脱硫性能的研究

发布时间：2018-05-28 14:03

本文选题：金属改性 + 有序杂化介孔碳　；参考：《上海应用技术学院》2015年硕士论文

【摘要】：燃油中硫化物在燃烧过程中会转化为SOx,除了形成酸雨,还会导致尾气转化催化剂中毒。另外,作为清洁能源的质子交换膜燃料电池和固态氧化物燃料电池也需要低硫含量(分别小于lppm和10ppm)的液体燃料作为原料。因此,燃油的超深度脱硫已经成为一项重要研究课题。本文制备了铜改性的有序杂化介孔碳材料,考察了铜负载方式、基体组成及孔结构、基体表面酸性等对模拟燃油中二苯并噻吩(DBT)常温常压吸附性能的影响。1.采用等体积浸渍法制备了铜改性的有序介孔碳硅复合材料(MCS),与铜改性的纯硅(SBA-15)和纯碳(CMK-3)相比,其对含苯的模拟燃油中DBT的吸附具有高的选择性。这主要是由于金属铜在MCS表面较高的分散性以及铜与炭组分对DBT的协同作用,而铜的高分散得益于硅和碳组分相互贯穿所形成的杂化孔表面。2.采用等体积浸渍法制备了铜改性的有序介孔碳硅铝材料(MCSA)和有序介孔碳铝材料(MCA),基体表面B酸量越多,铜的分散程度越高,相比于纯基体DBT吸附量提高的程度越大。另外,纯基体材料对DBT的吸附容量与表面酸量成正比,而与微孔孔容相关性不大。3.采用原位载铜法制备了铜改性的MCS材料,其硫容量相比纯基体提高了49%(高于后负载法),可能是由于铜颗粒呈半裸露状嵌在孔壁上使其分散程度提高所致。
[Abstract]:The sulfides in fuel oil can be converted into so _ x during combustion, which, in addition to forming acid rain, can lead to poisoning of tail gas conversion catalyst. In addition, proton exchange membrane fuel cells (PEMFC) and solid oxide fuel cells (SOFC), which are clean energy sources, also need liquid fuel with low sulfur content (less than lppm and 10 ppm respectively) as feedstock. Therefore, ultra-deep desulfurization of fuel has become an important research topic. In this paper, the ordered hybrid mesoporous carbon materials modified by copper were prepared. The effects of copper loading mode, matrix composition and pore structure, surface acidity of matrix on the adsorption properties of dibenzothiophene dithiophene (DBT) in simulated fuel at room temperature and atmospheric pressure were investigated. Copper modified ordered mesoporous carbon silicon composites (MCSs) were prepared by equal volume impregnation method. Compared with copper modified pure silicon SBA-15 and pure carbon CMK-3, the adsorption of DBT in benzene-containing simulated fuel oil has high selectivity. This is mainly due to the high dispersion of copper on the surface of MCS and the synergistic effect of copper and carbon on DBT, while the high dispersion of copper is due to the interpenetration of silicon and carbon on the surface of hybrid pore. The copper-modified ordered mesoporous carbon silica-aluminum (DBT) and ordered mesoporous carbon aluminum (MCA) were prepared by the same volume impregnation method. The higher the amount of B acid on the surface of the matrix, the higher the dispersion degree of copper, and the greater the adsorption capacity of copper was compared with that of pure matrix. In addition, the adsorption capacity of DBT on pure matrix material is directly proportional to the amount of acid on the surface, but has little correlation with the micropore volume. Copper modified MCS materials were prepared by in-situ copper loading method. The sulfur capacity of copper modified MCS was increased by 49% compared with pure matrix (higher than that by post-loading method), which may be due to the increase of dispersion degree of copper particles embedded in the pore wall in semi-bare form.
【学位授予单位】：上海应用技术学院
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：TQ127.11;TB383.4

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