【摘要】：采用溶膠-凝膠法,以問苯二酚、甲醛為有機相前驅(qū)體,無水碳酸鈉作為催化劑,經(jīng)過溶膠凝膠化、老化、溶劑置換、干燥和炭化的步驟制備出炭氣凝膠,并對其進行改性。采用的改性方法有水蒸氣活化、等體積浸漬法負載乙二胺四乙酸銅(EDTA-Cu)、研磨熱分散的方法負載氯化亞銅。同時在制備炭氣凝膠的過程中用無水碳酸鈉和醋酸銅為催化劑,制備出原位負載銅的炭氣凝膠。對所制備出來的樣品通過靜態(tài)吸附脫硫和動態(tài)吸附脫硫兩種方式來考察其對模擬燃油中的噻吩類硫化物二苯并噻吩(DBT)脫除性能。研究結(jié)果表明,在炭氣凝膠的制備過程中,間苯二酚和甲醛的摩爾比對炭氣凝膠的密度影響較大。炭氣凝膠經(jīng)水蒸氣活化后其比表面積比原來提高了一倍,達到了1141m2.g-1,微孔孔容也有了較大的提高,變?yōu)?.3317 cm3.g-1。吸附硫容和吸附速率也得到了提高。負載EDTA-Cu后樣品中的銅主要以CuO和單質(zhì)Cu的晶粒的形式存在,樣品的硫容有所降低,主要可能是因為CuO和單質(zhì)Cu堵孔導(dǎo)致的,但是樣品的選擇性則隨著銅含量的增多而提高。負載氯化亞銅的樣品,隨著負載量的增多樣品中除了有CuO和單質(zhì)Cu的晶粒外,還發(fā)現(xiàn)CuCl晶體,當(dāng)Cu負載量為5wt.%的樣品在非競爭和有苯競爭條件下的硫容最大。用醋酸銅和無水碳酸鈉作為催化劑制備出的原位載銅炭氣凝膠所含的微孔比較豐富。將樣品的硫容與樣品的微孔孔容進行關(guān)聯(lián),結(jié)果得到了較好的線性關(guān)系,并且樣品的選擇性也是隨著銅含量的增加而提高。
[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.
【學(xué)位授予單位】：上海應(yīng)用技術(shù)學(xué)院
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：TQ427.26;TE624.55

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