本文選題：二甘醇 + 叔丁胺　； 參考：《吉林大學(xué)》2017年碩士論文

【摘要】：天然氣中通常含有CO_2、H_2S和有機(jī)硫化合物,這三者又通稱為酸性氣體。其中H_2S在運(yùn)輸和存儲的過程當(dāng)中會使存儲設(shè)備和運(yùn)輸管道發(fā)生腐蝕,而且H_2S燃燒之后產(chǎn)生的氣體會嚴(yán)重污染空氣環(huán)境。叔丁氨基乙氧基乙醇(TBEE)具有空間位阻的效應(yīng),這種效應(yīng)可以讓氨基表現(xiàn)出更高的化學(xué)活性,是一種非常有效的選擇性脫硫溶劑。被廣泛應(yīng)用在石油、油田伴生氣、天然氣以及合成氣等氣體的選擇性脫硫。現(xiàn)在有關(guān)其合成工藝的報(bào)道很少,其合成方法和相應(yīng)的催化劑體系需進(jìn)行深入研究。本論文選擇通過二甘醇和叔丁胺胺化反應(yīng)合成TBEE,針對該反應(yīng)的特點(diǎn)設(shè)計(jì)制備了一系列Ni基催化劑,在間歇釜式反應(yīng)體系中考察了催化劑在二甘醇和叔丁胺胺化反應(yīng)中的催化性能,并優(yōu)化了反應(yīng)條件。同時(shí)結(jié)合反應(yīng)結(jié)果和多種表征手段,研究了催化劑的結(jié)構(gòu)、活性組分以及酸堿性等在催化劑反應(yīng)體系中所起的作用。還考察了催化劑的制備條件對催化性能的影響。論文的主要工作如下:(1)針對二甘醇和叔丁胺的胺化反應(yīng),對催化劑的活性組分進(jìn)行了篩選,并考察了反應(yīng)溫度、壓強(qiáng)、溶劑、轉(zhuǎn)速等反應(yīng)條件對催化劑催化反應(yīng)性能的影響。結(jié)果表明,以Ni為催化劑的主要組分,反應(yīng)溫度為200℃,轉(zhuǎn)速為400r/min,H_2壓強(qiáng)為0.5MPa,原料摩爾比TBA:DEG為2:1,無溶劑時(shí),催化劑有較好的催化性能。(2)采用共沉淀法制備了一系列的Ni-Al_2O_3催化劑,考察了Ni/Al、焙燒溫度和還原溫度對二甘醇和叔丁胺胺化反應(yīng)合成TBEE的影響。結(jié)果表明,共沉淀法制備的Ni-Al_2O_3催化劑,Ni/Al為1:1,在450℃焙燒和550℃還原時(shí),催化劑表現(xiàn)出較高的活性和選擇性。結(jié)合相關(guān)表征和催化性能結(jié)果,金屬Ni顆粒(Ni0)是反應(yīng)的活性中心,并且催化劑的酸-堿中心在提高催化劑的活性和選擇性方面發(fā)揮著協(xié)同作用。(3)對Ni-Al_2O_3催化劑的制備條件(如Ni含量、沉淀劑、合成溫度和沉淀方法)進(jìn)行了進(jìn)一步優(yōu)化,并考察了合成條件以及反應(yīng)時(shí)間對催化劑的胺化反應(yīng)性能的影響。結(jié)果表明,催化劑制備條件對催化劑的結(jié)構(gòu)性質(zhì)及催化反應(yīng)性能有較大影響。最適宜的制備條件為,Ni含量為20%,以Na2CO3為沉淀劑,合成溫度為80℃,在最佳的反應(yīng)條件下反應(yīng)6h,催化劑有較好的反應(yīng)性能。
[Abstract]:Natural gas usually contains CO _ 2H _ 2S and organic sulfur compounds, which are also known as acid gases. In the process of transportation and storage of H2S, the storage equipment and transportation pipeline will be corroded, and the gas produced after the combustion of H2S will pollute the air environment seriously. Tert-butylamino ethoxy ethanol (TBEE) has the effect of steric hindrance which can make amino show higher chemical activity and is a very effective solvent for selective desulfurization. It is widely used in selective desulfurization of petroleum, oil field associated gas, natural gas and syngas. At present, there are few reports about the synthesis process, and the synthesis method and the corresponding catalyst system need to be deeply studied. In this paper, a series of Ni-based catalysts were designed and prepared by the reaction of diethylene glycol and tert-butylamination to synthesize TBEE. in accordance with the characteristics of the reaction, a series of Ni based catalysts were prepared. The catalytic performance of the catalyst in diethylene glycol and tert-butylamination was investigated in the batch reactor system, and the reaction conditions were optimized. At the same time, combined with the reaction results and various characterization methods, the role of catalyst structure, active components, acid and basic in the catalyst reaction system was studied. The effect of preparation conditions on the catalytic performance was also investigated. The main work of this paper is as follows: (1) for the amination of diethylene glycol and tert-butylamine, the active components of the catalyst were screened, and the effects of reaction temperature, pressure, solvent and rotational speed on the catalytic performance of the catalyst were investigated. The results showed that a series of Ni-Al_2O_3 catalysts were prepared by coprecipitation method with Ni as the main component, reaction temperature at 200 鈩，

本文編號：1920158