通过溶胶-凝胶法,以正硅酸乙酯(TEOS)和十七氟癸基三乙氧基硅烷(PFDTES)为前驱体,在酸性和洁净室条件下制备了十七氟癸基修饰的SiO2膜材料,分别通过动态光散射技术、接触角测量、红外光谱以及热重分析等测试手段对溶胶的粒径分布及膜材料的疏水性能进行了表征,并深入研究了十七氟癸基修饰后膜材料的氢气渗透和分离性能.结果表明,当摩尔比n(PFDTES)/n (TEOS)=0.2时,溶胶的粒径狭窄分布在3.9 nm.十七氟癸基已成功修饰到SiO2膜材料中,十七氟癸基的修饰使得膜材料从亲水性变为疏水性,在上述摩尔比例下,膜材料对水的接触角达到112.0°±0.6°.H2的单组分渗透率随温度的升高而增大,300℃时达到10.00×10-7mol/(m2·s· Pa),H2/CO2的单组分理想分离系数及双组分分离系数分别达到6.10和13.30,均高于其Knudsen扩散分离因子(4.69),H2在膜材料中的输运主要遵循活化扩散机理.
参考文献
[1] | Brunetti A;Caravella A;Barbieri G;Drioli E .Simulation study of water gas shift reaction in a membrane reactor[J].Journal of Membrane Science,2007(1/2):329-340. |
[2] | Petra S;Andrej Z;Francoise M I .Activities on application of nuclear techniques in development and characterization of materials for hydrogen economy[J].Adv Mater Res,2011,324:461-464. |
[3] | Benes N E .Mass transport in thin supported silica membranes[D].Enschede:University of Twente,2000. |
[4] | Nathan W.Ockwig;Tina M.Nenoff .Membranes for Hydrogen Separation[J].Chemical Reviews,2007(10):4078-4110. |
[5] | Baker R W .Research needs in the membrane separation industry:Looking back,looking forward[J].Journal of Membrane Science,2010,362:134-136. |
[6] | 韦奇,李健林,宋春林,刘卫,陈初升.微孔二氧化硅膜的制备、氢气分离以及水热稳定性研究[J].无机材料学报,2004(01):133-139. |
[7] | De Vos R M;Verweij H .High-selectivity,high-flux silica membranes for gas separation[J].SCIENCE,1998,279:1710-1711. |
[8] | Battersby S;Tasaki T;Smart S et al.Performance of cobalt silica membranes in gas mixture separation[J].Journal of Membrane Science,2009,329(02):91-98. |
[9] | Masakoto Kanezashi;Masashi Asaeda .Hydrogen permeation characteristics and stability of Ni-doped silica membranes in steam at high temperature[J].Journal of Membrane Science,2006(1/2):86-93. |
[10] | Gu YF;Hacarlioglu P;Oyama ST .Hydrothermally stable silica-alumina composite membranes for hydrogen separation[J].Journal of Membrane Science,2008(1/2):28-37. |
[11] | Ohta Y;Akamatsu K;Sugawara T;Nakao A;Miyoshi A;Nakao S .Development of pore size-controlled silica membranes for gas separation by chemical vapor deposition[J].Journal of Membrane Science,2008(1/2):93-99. |
[12] | Hegde ND;Rao AV .Organic modification of TEOS based silica aerogels using hexadecyltrimethoxysilane as a hydrophobic reagent[J].Applied Surface Science: A Journal Devoted to the Properties of Interfaces in Relation to the Synthesis and Behaviour of Materials,2006(3):1566-1572. |
[13] | Bhagat SD;Rao AV .Surface chemical modification of TEOS based silica aerogels synthesized by two step (acid-base) sol-gel process[J].Applied Surface Science: A Journal Devoted to the Properties of Interfaces in Relation to the Synthesis and Behaviour of Materials,2006(12):4289-4297. |
[14] | 韦奇,李健林,宋春林,刘卫,陈初升.憎水二氧化硅膜的制备、表征及水热稳定性研究[J].无机材料学报,2004(02):417-423. |
[15] | Castricum HL;Sah A;Kreiter R;Blank DHA;Vente JF;ten Elshof JE .Hybrid ceramic nanosieves: stabilizing nanopores with organic links[J].Chemical communications,2008(9):1103-1105. |
[16] | 段小勇,韦奇,何俊,闫建平,李群艳,聂祚仁.表面修饰的有机-无机杂化微孔SiO2膜的制备及氢气分离性能[J].高等学校化学学报,2011(10):2256-2261. |
[17] | 王学伟,韦奇,洪志发,李群艳,聂祚仁.三氟丙基修饰的有机-无机杂化二氧化硅膜制备、氢气分离及水热稳定性能[J].化学学报,2012(24):2529-2535. |
[18] | 宋霖,韦奇,郝润秋,聂祚仁,李群艳.十七氟癸基修饰的有机-无机杂化二氧化硅膜材料的制备及气体分离性能[J].高等学校化学学报,2012(08):1670-1675. |
[19] | Castricum, HL;Sah, A;Kreiter, R;Blank, DHA;Vente, JF;ten Elshof, JE .Hybrid ceramic nanosieves: stabilizing nanopores with organic links[J].Chemical communications,2008(9):1103-1105. |
[20] | 王学伟 .用于水煤气变换反应的三氟丙基修饰有机—无机杂化SiO2膜材料研究[D].北京工业大学,2013. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%