【摘要】：采用普通浸漬法、超聲浸漬法和溶膠凝膠法三種方式制備高溫煤氣脫硫劑,通過(guò)ICP、SEM、XRD、氮吸附等手段對(duì)脫硫劑進(jìn)行表征,并在一立式固定床上進(jìn)行活性評(píng)價(jià)。得出結(jié)論如下： (1)采用超聲浸漬法和普通浸漬法制備鐵、錳、銅、鋅、鈰、鈣六種物系脫硫劑,ICP-AES結(jié)果表明超聲浸漬不僅縮短了浸漬時(shí)間,還促進(jìn)了活性成分的負(fù)載。BET分析結(jié)果和粒徑分布曲線表明,超聲浸漬豐富了脫硫劑的孔隙結(jié)構(gòu),增加了比表面積和孔容,并具有細(xì)化顆粒的效果。SEM結(jié)果顯示,超聲浸漬制備得到的脫硫劑顆粒較小而且分布均勻,燒結(jié)程度較輕。XRD分析表明超聲浸漬對(duì)脫硫劑的晶粒分布狀態(tài)有影響。在固定床上對(duì)所有脫硫劑進(jìn)行活性評(píng)價(jià),結(jié)果表明超聲波浸漬法制備得到的脫硫劑的穿透硫容有顯著提高。6種物系的脫硫穿透硫容比較結(jié)果為：MnFeCuCeCaZn,但超聲波處理后Fe的穿透硫容提高最為明顯。 (2)采用超聲浸漬法分別制備Mn/SiO2、Mn/TiO2、Mn/γ-Al2O3三種高溫煤氣脫硫劑,研究載體對(duì)于脫硫劑活性的影響。三種載體的比較研究表明,Mn/γ-Al2O3比表面積大,脫硫活性大,能滿(mǎn)足IGCC中硫化氫的凈化要求,是一種較好的高溫煤氣脫硫劑。而Mn/SiO2不能較長(zhǎng)時(shí)間維持硫化氫在低濃度,Mn/TiO2高溫穩(wěn)定性差。 (3)采用溶膠凝膠法和超聲浸漬法分別制備相同負(fù)載的錳系脫硫劑,并對(duì)其進(jìn)行表征和活性評(píng)價(jià),得出結(jié)論：溶膠凝膠法制備得到的脫硫劑孔隙更為豐富,具有良好的微觀結(jié)構(gòu),XRD測(cè)試結(jié)果顯示其活性成分在載體上的分布更為均勻,能夠更好的進(jìn)行脫硫反應(yīng)。溶膠凝膠法制備得到的脫硫劑活性比相同負(fù)載下的超聲浸漬法制得的脫硫劑來(lái)得高。溫度越大,脫硫劑活性增大,但是漲幅并不大�？傮w上講,溶膠法具有較為優(yōu)良的性能,各種參數(shù)比超聲浸漬來(lái)得好；但是,由于其制備工藝較為復(fù)雜,費(fèi)用高,目前難以在工業(yè)化推廣應(yīng)用。
[Abstract]:High temperature gas desulphurizer was prepared by ordinary impregnation method, ultrasonic impregnation method and sol-gel method. The desulphurizer was characterized by ICP,SEM,XRD, nitrogen adsorption and evaluated in a vertical fixed bed. The conclusions are as follows: (1) six kinds of desulphurizing agents, iron, manganese, copper, zinc, cerium and calcium, were prepared by ultrasonic impregnation and ordinary impregnation. ICP-AES results show that ultrasonic impregnation not only shortens the impregnation time. The results of BET analysis and particle size distribution show that ultrasonic impregnation enriches the pore structure of desulphurizer, increases the specific surface area and pore volume, and has the effect of refining particles. SEM results show that the ultrasonic impregnation enriches the pore structure of desulphurizer, increases the specific surface area and pore volume, and has the effect of refining particles. The particles of desulphurizer prepared by ultrasonic impregnation are small and uniform, and the sintering degree is light. XRD analysis shows that ultrasonic impregnation has an effect on the grain distribution of desulphurizer. The activity of all desulphurizers was evaluated in a fixed bed. The results showed that the penetrating sulfur capacity of the desulphurizers prepared by ultrasonic impregnation method was significantly improved. The comparison of desulphurization penetrating sulfur capacity of six kinds of compounds was as follows: MnFeCuCeCaZn, However, the penetrating sulfur capacity of Fe increased most obviously after ultrasonic treatment. (2) three kinds of high temperature gas desulphurizer Mn/SiO2,Mn/TiO2,Mn/ 緯-Al2O3 were prepared by ultrasonic immersion method, and the effect of carrier on the activity of desulphurizer was studied. The comparative study of the three carriers shows that Mn/ 緯-Al2O3 has large specific surface area and high desulphurization activity, which can meet the purification requirements of hydrogen sulfide in IGCC and is a good high temperature gas desulphurizer. However, Mn/SiO2 can not maintain hydrogen sulfide at low concentration for a long time, and the high temperature stability of Mn/TiO2 is poor. (3) Manganese desulphurizer with the same load was prepared by sol-gel method and ultrasonic impregnation method, and its characterization and activity evaluation were carried out respectively. it was concluded that the pores of desulphurizer prepared by sol-gel method were more abundant. The results of XRD test show that the distribution of active components on the carrier is more uniform and the desulphurization reaction can be carried out better. The activity of desulphurizer prepared by sol-gel method is higher than that prepared by ultrasonic impregnation under the same load. The higher the temperature, the higher the activity of desulphurizer, but the increase is not great. Generally speaking, the sol method has excellent properties and various parameters are better than those of ultrasonic impregnation. However, because of its complex preparation process and high cost, it is difficult to be popularized and applied in industrialization at present.
【學(xué)位授予單位】：浙江大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2010
【分類(lèi)號(hào)】：X701.3

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