發(fā)布時間：2018-04-22 01:32

  本文選題：微介孔Y分子篩 + 離子液體��； 參考：《東南大學》2016年碩士論文

【摘要】：微孔Y型分子篩由于具有較大的比表面積、較強的酸性、良好的水熱穩(wěn)定性,被廣泛地用在催化、吸附和分離等領域。但其狹窄的的孔徑(～0.74nm)阻礙了反應物和產物的擴散與分離,從而限制了其在大分子反應中的應用。與微孔分子篩相比,介孔材料具有較大的孔徑,能夠加快擴散速度。易于反應物通過介孔到達反應活性位,相應地,反應產物能夠快速地從催化劑孔道內部擴散出來。但是介孔材料的水熱穩(wěn)定性和耐酸性均較差。因此將介孔引入到Y型分子篩中,可以有效地避免二者的缺點,優(yōu)勢互補,協同作用。這種新型的微介孔Y型分子篩既具有傳統(tǒng)的沸石分子篩的性能,又能夠降低擴散阻力,極其有利于含有大分子的催化反應。二芳基乙烷(PXE)是生產壓敏復寫紙顯色劑的優(yōu)良溶劑,主要通過鄰二甲苯和苯乙烯的烷基化反應獲得。本論文以離子液體1-甲基-3-(3-三甲氧基硅基丙基)咪唑氯摀(MTPI)為介孔模板劑,硅酸鈉為硅源,偏鋁酸鈉、十八水硫酸鋁為鋁源,制備了一種新型的微介孔Y型分子篩。將制備的Na型Y分子篩進行離子交換得到H型微介孔Y型分子篩,并考察其在鄰二甲苯和苯乙烯制備二芳基乙烷(PXE)的烷基化反應中的催化性能。采用離子液體MTPI為介孔模板劑,在不加入任何助劑的條件下,一步水熱法制備了結晶度較好的微介孔NaY型分子篩�？疾炝穗x子液體MTPI與溶液中Na2O的摩爾比(n)、晶化溫度(x)對分子篩NaY-nMTPI-x的影響。研究表明：當x為100℃、n為0.15時,制備的NaY-0.15MTPI分子篩樣品的比表面積最大,達到690 m2/g(其中介孔比表面占76 m2/g)；孔體積為0.39 cm3/g(其中介孔孔體積為0.11 cm3/g)。通過離子交換法制備系列的微介孔HY-nMTPI分子篩作為烷基化催化劑。對比發(fā)現,所有的微介孔HY-nMTPI分子篩都比微孔分子篩HY的催化性能好。其中HY-0.15 MTPI由于具有較多的介孔結構和最多的酸量,在PXE產率和催化劑循環(huán)使用方面均表現出良好的催化性能。以離子液體MTPI為介孔模板劑,硅酸鈉為硅源,偏鋁酸鈉、十八水硫酸鋁為鋁源,通過不同的方法制備了微介孔NaY分子篩�？疾炝藗鹘y(tǒng)的水熱晶化法和超聲微波協同輔助法對微介孔材料NaY(C)和NaY(UMSS)形成的影響。結果表明：在超聲微波的輻射下,雖然合成微介孔分子篩NaY(UMSS)的晶化時間大大地縮短,但是其具有較大的比表面積與孔容、較好的結晶度、較多的介孔結構、較小的晶粒和較好的分散性。因此經過離子交換后,樣品HY(UMSS)在PXE產率和催化劑壽命方面表現出最佳的催化性能。當晶化溫度為100℃, n(MTPI):n(Na2O)為0.15時,進一步考察了不同的硅鋁比(z)對分子篩z NaY結構的影響。研究表明：隨著硅鋁比的逐漸增大,所得分子篩樣品的結晶度、比表面積和孔容均呈現先增大后減小的趨勢；總酸量和酸位也隨著鋁源加入量的不同有很大的變化。在烷基化反應中,當z≤10.5時,所有的高鋁含量的微介孔分子篩z HY都顯示出較好的催化活性。而且分子篩9.5HY由于具有較高的比表面積,較多的介孔孔容和最多的酸量,在烷基化反應中表現出最好的催化性能。PXE的產率高達91.73%,表明了較多的介孔和酸量有利于烷基化反應的進行。綜上所述,采用離子液體為模板劑制備的微介孔Y分子篩具有較高的比表面積、較大的孔徑、較多的酸量,而且這些優(yōu)點均有益于微介孔Y分子篩作為催化劑應用于鄰二甲苯和苯乙烯制備PXE的烷基化反應中。
[Abstract]:Microporous Y molecular sieves are widely used in the fields of catalysis, adsorption and separation because of their large specific surface area, strong acidity and good hydrothermal stability. But the narrow pore size (~ 0.74nm) hinders the diffusion and separation of reactants and products, thus limiting its application in large molecular reactions. The mesoporous material has a larger aperture and can accelerate the diffusion speed. The reactant can reach the reactive potential through the mesopore. Accordingly, the reaction products can quickly spread out of the catalyst channel. However, the hydrothermal stability and acid resistance of the mesoporous materials are poor. Therefore, the introduction of mesoporous materials to the Y type molecular sieve can effectively avoid it. The new type of micro mesoporous Y type molecular sieves not only have the properties of the traditional zeolite molecular sieves, but also reduce the diffusion resistance, and are extremely beneficial to the catalytic reaction with large molecules. Two aryl ethane (PXE) is a good solvent for the production of pressure-sensitive compound paper chromogenic agent, mainly through the xylene and benzene. The alkylation of ethylene was obtained. In this paper, a new type of micro mesoporous Y molecular sieve was prepared by using the ionic liquid 1- methyl -3- (3- trimethoxy silicon propyl) imidazolium (MTPI) as a mesoporous template, sodium silicate as the silicon source, sodium aluminate, and eighteen water aluminum sulfate as the aluminum source. The prepared Na type Y molecular sieve was exchanged for H micromedium by ion exchange. The catalytic properties of pore Y molecular sieves were investigated in the alkylation of two aryl ethane (PXE) prepared by o-xylene and styrene. Using ionic liquid MTPI as a mesoporous template, the micro mesoporous NaY zeolite with better crystallinity was prepared by one step hydrothermal method without any additives. The MTPI and solution of ionic liquid were investigated. The effect of crystallization temperature (x) on the molecular sieve NaY-nMTPI-x of medium Na2O (n) shows that when x is 100 and N is 0.15, the specific surface area of the prepared NaY-0.15MTPI molecular sieve is the largest, reaching 690 m2/g (which the mesoporous surface is 76 m2/g), and the pore volume of 0.39 cm3/g (including the mesoporous pore volume of 0.11 cm3/g). A series of micro mesoporous HY-nMTPI molecular sieves were prepared as a catalyst for alkylation. It was found that all microporous HY-nMTPI molecular sieves have better catalytic properties than microporous molecular sieves. Among them, HY-0.15 MTPI has a good catalytic performance in the yield of PXE and the use of catalytic agents because of the more mesoporous structure and the most acid content. Properties. Using ionic liquid MTPI as a mesoporous template, sodium silicate as a silicon source, sodium aluminate, eighteen water aluminum sulfate as the aluminum source, micro mesoporous NaY zeolite was prepared by different methods. The influence of the traditional hydrothermal crystallization method and ultrasonic microwave co assisted method on the formation of NaY (C) and NaY (UMSS) of micro mesoporous materials was investigated. The crystallization time of the synthetic mesoporous molecular sieve NaY (UMSS) is greatly shortened, but it has a larger specific surface area and pore volume, better crystallinity, more mesoporous structure, smaller grain size and better dispersibility. Therefore, after ion exchange, the sample HY (UMSS) shows the PXE yield and the life of the catalyst. The optimum catalytic performance. When the crystallization temperature is 100, n (MTPI) and n (Na2O) is 0.15, the effect of different Si / Al ratio (z) on the structure of Z NaY is further investigated. In alkylation, all the microporous mesoporous molecular sieves Z HY with high aluminum content showed good catalytic activity in the alkylation reaction, and the molecular sieve 9.5HY showed a high specific surface area, more mesoporous Kong Kong volume and the most acid content in alkylation. The best catalytic performance of.PXE is up to 91.73%, indicating that more mesoporous and acid content is beneficial to alkylation. To sum up, the micro mesoporous Y zeolite prepared by ionic liquid as a template has higher specific surface area, larger aperture and more acid content, and these advantages are beneficial to micro mesoporous Y molecular sieves. Alkylation of PXE with o-xylene and styrene was used as catalyst.

【學位授予單位】：東南大學
【學位級別】：碩士
【學位授予年份】：2016
【分類號】：O643.36;O645.1

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本文編號：1785025