本文關(guān)鍵詞：多層結(jié)構(gòu)鈦硅（TS-1）分子篩膜的制備　出處：《青島科技大學(xué)》2017年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： TS-1 周期性二次生長 雙層結(jié)構(gòu) 多級孔結(jié)構(gòu) 溶解-再結(jié)晶機(jī)制

【摘要】：TS-1分子篩具有MFI拓?fù)浣Y(jié)構(gòu),因其在溫和條件下優(yōu)越的擇形氧化性能而被人們所熟知。盡管TS-1分子篩在許多有機(jī)化合物的氧化反應(yīng)中表現(xiàn)出良好的活性,但其微孔孔徑大小只有約為0.5 nm。因此,較大分子尺寸的基質(zhì)不能進(jìn)入通道,它們只能與分子篩表面活性中心接觸反應(yīng)。因而,本文旨在改善TS-1分子篩及TS-1分子篩膜的孔道結(jié)構(gòu),進(jìn)而改善其性能。具體研究內(nèi)容如下:(1)通過堿處理制得具有豐富次生孔隙的多級孔TS-1分子篩。脫除模板劑后的TS-1分子篩通過TPAOH后處理可形成多級孔TS-1分子篩。催化加氫裂化法和焙燒法都能脫除TS-1分子篩中的模板劑,但前者對應(yīng)的多級孔TS-1分子篩具有更高的比表面積和孔容。此外,TPAOH濃度也影響多級孔TS-1分子篩的形成。隨著堿濃度的增加,溶蝕-再結(jié)晶過程加劇,空心孔隙體積增加。在分子篩/TPAOH/H2O質(zhì)量比為1/3/5時,BET比表面積和孔容可達(dá)460 cm2/g和0.61 cm3/g。(2)傳統(tǒng)的二次生長法只能制備單層的TS-1分子篩膜。基于傳統(tǒng)的二次生長法,我們提出了周期性二次生長法用來制備雙層TS-1分子篩膜,周期性二次生長法可以制得雙層結(jié)構(gòu)的TS-1分子篩膜。這種新型的周期性二次生長法包含兩到幾個周期(多個周期),每個周期包含三步,首先升溫到特定溫度,然后保溫一段時間,最后降溫到室溫。通過SEM,EDS,氣體滲透和脫鹽測試可知,雙層TS-1分子篩膜具有較好的完備性和疏水性能。由此說明通過周期性二次生長法能夠合成具有更優(yōu)越性能的TS-1分子篩膜。(3)通過溶解-再結(jié)晶機(jī)制在堿性懸浮液中對TS-1分子篩膜進(jìn)行處理,成功制得了多級孔結(jié)構(gòu)TS-1分子篩膜。通過XRD,SEM和EDS測試分析了制得的HTS-1分子篩膜的結(jié)構(gòu)和組成�？梢杂^察到HTS-1分子篩膜中存在一定量的孔洞,懸浮液中的TS-1分子篩顆粒,TPAOH模板劑和水對孔洞的形成有一定的影響。氣體滲透性能和脫鹽測試結(jié)果表明,具有多級孔結(jié)構(gòu)的TS-1分子篩膜比傳統(tǒng)的TS-1分子篩膜具有更好的氣體/水滲透性。這對于提高膜通量的工作提供了新的見解。
[Abstract]:TS-1 molecular sieve has MFI topology. TS-1 molecular sieves are well known for their superior shape selective oxidation properties under mild conditions, although TS-1 molecular sieves exhibit good activity in the oxidation of many organic compounds. But its pore size is only about 0.5 nm. Therefore, the larger molecular size of the matrix can not enter the channel, they can only contact with the molecular sieve surface active center reaction. The purpose of this paper is to improve the pore structure of TS-1 molecular sieve and TS-1 molecular sieve membrane. Then improve its performance. The specific research contents are as follows: 1). The multiporous TS-1 molecular sieve with abundant secondary pores was prepared by alkali treatment. The TS-1 molecular sieve after removing the template was treated with TPAOH to form the multiporous TS-1 molecular sieve. The catalytic hydrogenation cracking was carried out. The template of TS-1 molecular sieve can be removed by both chemical method and roasting method. However, the former has higher specific surface area and higher pore volume. In addition, the concentration of TPAOH also affects the formation of multiporous TS-1 molecular sieve. When the mass ratio of molecular sieve / TPAOH / H _ 2O is 1 / 3 / 5, the volume of hollow pore increases. The specific surface area and pore volume of BET can reach 460 cm2/g and 0.61 cm 3 / g 路m2). The traditional secondary growth method can only produce monolayer TS-1 molecular sieve membranes, based on the traditional secondary growth method. A periodic secondary growth method was proposed to prepare bilayer TS-1 molecular sieve membranes. Double layer TS-1 molecular sieve membranes can be prepared by periodic quadratic growth method, which consists of two or several cycles (multiple cycles, each cycle consists of three steps). First to a specific temperature, then to hold it for a period of time, finally to the room temperature. Through SEMN EDS, gas permeation and desalination tests know. The bilayer TS-1 molecular sieve membrane has good completeness and hydrophobicity, which shows that the TS-1 molecular sieve membrane with better performance can be synthesized by periodic secondary growth method. TS-1 molecular sieve membranes were treated in alkaline suspensions by solution-recrystallization mechanism. TS-1 molecular sieve membrane with multilevel pore structure was successfully prepared by XRD. The structure and composition of the HTS-1 molecular sieve membrane were analyzed by SEM and EDS. A certain number of pores and TS-1 particles in the suspension of HTS-1 molecular sieve membrane were observed. TPAOH template and water have a certain effect on the formation of pores. The gas permeability and desalination test results show that. The gas / water permeability of the TS-1 molecular sieve membrane with multilevel pore structure is better than that of the traditional TS-1 molecular sieve membrane, which provides a new insight for improving the membrane flux.
【學(xué)位授予單位】：青島科技大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：X78

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