铜掺杂炭气凝胶的制备及燃油脱硫性能研究

发布时间：2018-09-07 08:27

【摘要】：采用溶胶-凝胶法,以问苯二酚、甲醛为有机相前驱体,无水碳酸钠作为催化剂,经过溶胶凝胶化、老化、溶剂置换、干燥和炭化的步骤制备出炭气凝胶,并对其进行改性。采用的改性方法有水蒸气活化、等体积浸渍法负载乙二胺四乙酸铜(EDTA-Cu)、研磨热分散的方法负载氯化亚铜。同时在制备炭气凝胶的过程中用无水碳酸钠和醋酸铜为催化剂,制备出原位负载铜的炭气凝胶。对所制备出来的样品通过静态吸附脱硫和动态吸附脱硫两种方式来考察其对模拟燃油中的噻吩类硫化物二苯并噻吩(DBT)脱除性能。研究结果表明,在炭气凝胶的制备过程中,间苯二酚和甲醛的摩尔比对炭气凝胶的密度影响较大。炭气凝胶经水蒸气活化后其比表面积比原来提高了一倍,达到了1141m2.g-1,微孔孔容也有了较大的提高,变为0.3317 cm3.g-1。吸附硫容和吸附速率也得到了提高。负载EDTA-Cu后样品中的铜主要以CuO和单质Cu的晶粒的形式存在,样品的硫容有所降低,主要可能是因为CuO和单质Cu堵孔导致的,但是样品的选择性则随着铜含量的增多而提高。负载氯化亚铜的样品,随着负载量的增多样品中除了有CuO和单质Cu的晶粒外,还发现CuCl晶体,当Cu负载量为5wt.%的样品在非竞争和有苯竞争条件下的硫容最大。用醋酸铜和无水碳酸钠作为催化剂制备出的原位载铜炭气凝胶所含的微孔比较丰富。将样品的硫容与样品的微孔孔容进行关联,结果得到了较好的线性关系,并且样品的选择性也是随着铜含量的增加而提高。
[Abstract]:Carbon aerogel was prepared by sol-gel method with Phenechol formaldehyde as organic precursor and anhydrous sodium carbonate as catalyst through sol-gel aging solvent replacement drying and carbonization. The modified methods include steam activation, equivolumic impregnation with copper ethylenediamine tetraacetate (EDTA-Cu) and grinding heat dispersion with cuprous chloride. At the same time, carbon aerogels loaded with copper in situ were prepared using anhydrous sodium carbonate and copper acetate as catalysts during the preparation of carbon aerogels. The (DBT) removal of thiophene sulfides from simulated fuel was investigated by static adsorption desulfurization and dynamic adsorption desulfurization. The results show that the molar ratio of resorcinol and formaldehyde has a great influence on the density of carbon aerogel during the preparation of carbon aerogel. The specific surface area of carbon aerogel was doubled to 1141 m2.g-1 after steam activation, and the pore volume of carbon aerogel was increased to 0.3317 cm3.g-1.. The adsorption capacity and adsorption rate of sulfur were also increased. After loading EDTA-Cu, the copper in the sample mainly exists in the form of CuO and Cu grains, and the sulfur capacity of the sample decreases, which may be due to the blocking of pores by CuO and Cu, but the selectivity of the sample increases with the increase of copper content. The samples loaded with cuprous chloride also found CuCl crystals in addition to the grains of CuO and Cu with the increase of loading amount. When the loading amount of Cu was 5wt.%, the sulfur capacity of the samples with 5 wt.% Cu loading was the largest in non-competitive and benzene competitive conditions. The in-situ copper-loaded carbon aerogels prepared with copper acetate and anhydrous sodium carbonate as catalysts are rich in micropores. By correlating the sulfur capacity of the sample with the pore volume of the sample, a good linear relationship was obtained, and the selectivity of the sample increased with the increase of copper content.
【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】：TQ427.26;TE624.55

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