新型管式炭载体上Silicalite-1型沸石复合膜的制备与性能

无机材料学报

新型管式炭载体上Silicalite-1型沸石复合膜的制备与性能

邹本雪1, 张雄福1, 王同华2, 王金渠1, 刘海鸥3, 王安杰3

大连理工大学化工学院1. 化学工艺系吸附与无机膜研究所; 2. 材料化工系; 3.催化化学与工程催化系和精细化工国家重点实?验室, 大连 116012

收稿日期:2004-12-13 修回日期:2005-01-17 出版日期:2006-01-20 网络出版日期:2006-01-20

Preparation and Properties of Carbon-Zeolite Silicalite-1 Membranes on Novel Tubular Carbon Supports

ZOU Ben-Xue¹, ZHANG Xiong-Fu¹, WANG Tong-Hua², WANG Jin-Qu¹, LIU Hai-Ou³, WANG An-Jie³

1. Department of Chem. and Technol., Dalian University of Technology, Dalian 116012, China; 2. Department of Mater. Sci. and Chem.
Eng., Dalian University of Technology, Dalian 116012, China; 3. Department of Catalytic Chem. and Eng., State Key Laboratory of Fine Chemicals, Dalian
University of Technology, Dalian 116012, China

Received:2004-12-13 Revised:2005-01-17 Published:2006-01-20 Online:2006-01-20

摘要/Abstract

摘要： 以多孔炭管为载体, 采用预涂晶种二次生长法在澄清溶液体系制备了炭基- Silicalite-1沸石复合膜. XRD、SEM及气体渗透性能表明: 合成的炭基-沸石复合膜完整、致密, 在室温下, H₂/C₃H₈
的理想分离因数达到了13.6, 显示出明显的分子筛分性能. 沸石直接在无晶种层的炭表面上不易生长成膜, 而具有晶种层的炭表面可形成连续沸石膜. 用弱极性的乙醇代替常规的水作为
晶种溶剂可有效地将晶种引入到非极性的炭表面而形成连续、均匀的晶种涂层. 在氮气气氛、793K下焙烧, 可以除去复合膜中的有机胺模板剂, 并避免炭载体结构的氧化破坏.

关键词: 沸石膜, 多孔炭材料, 沸石, 无机膜

Abstract: The zeolite silicalite-1 composite membranes on porous carbon tubes were successfully prepared by using a simple seeded synthesis from clear solutions. SEM, XRD and single gas permeation characterization
indicate that the membrane is dense, free-defected and shows good permeation properties. H₂/C₃H₈ ideal selectivity for the membrane is over 15 at room temperature. Zeolite seeds are easily introduced
into the porous carbon surface by a slip-casting technique from seed ethanol solution instead of water solution. The continuous seed layer on the carbon support favors the formation of the perfect membrane. The organic template from the composite membrane can be removed by calcination at 793K under
nitrogen flow. This opens up the route for the preparation of carbon-zeolite films on porous carbon materials and also develops a novel method for tailoring and improving carbon pore structure of porous carbon materials.

Key words: zeolite membrane, porous carbon, zeolite, inorganic membrane

中图分类号:

O614

邹本雪1,张雄福1,王同华2,王金渠1,刘海鸥3,王安杰3. 新型管式炭载体上Silicalite-1型沸石复合膜的制备与性能[J]. 无机材料学报.

ZOU Ben-Xue,ZHANG Xiong-Fu,WANG Tong-Hua,WANG Jin-Qu,LIU Hai-Ou,WANG An-Jie. Preparation and Properties of Carbon-Zeolite Silicalite-1 Membranes on Novel Tubular Carbon Supports[J]. Journal of Inorganic Materials.

参考文献

[1] Tavolaro A , Drioli E. Adv. Mater., 1999, 11: 975-996.
[2] Coronas J, Santamaria J. Topics in Catalysis, 2004, 29(1-2): 29-44.
[3] 纪君美, 项寿鹤, 李赫喧(JI Mei-jun, et al). 无机材料学报 ( Journal of Inorganic Materials), 1995, 10(1): 100-104.
[4] 程志林, 晁自胜, 方维平, 等(CHENG Zhi-lin, et al). 无机材料学报 ( Journal of Inorganic Materials), 2003, 18(6): 1306-1312.
[5] Xu Xiao-chun, Yang Wei-sheng, Liu Jie, et al. Micropor. Mesopor. Mater., 2001, 43(3): 299-311.
[6] Lai Z, Bonilla G, Diaz I, et al. Science, 2003, 300: 456-460.
[7] 张雄福, 刘海鸥, 王金渠, 等. 催化学报. 2004, 25(7): 586-590.
[8] 宋成文, 王同华, 邱介山. 化工进展, 2003, 22(9): 961-964.
[9] Kyotani T. Carbon, 2000, 38: 269-286.
[10] vander Vaart R, Bosch H, Keizer K, et al. Micropor. Mater., 1997, 9: 203-207.
[11] Garcia-Martinez J, Cazorla-Amoros D, Linares-Solano A, et al. Micropor. Mesopor. Mater., 2001, 42: 255-268.
[12] Berenguer-Murcia A, Garcia-Martinez J, Cazorla-Amoros D, et al. Micropor. Mesopor. Mater., 2003, 59: 147-159.
[13] Berenguer-Murcia A, Morallon E, Cazorla-Amoros D, et al. Micropor. Mesopor. Mater., 2003, 66: 331-340.
[14] ZHANG Xiong-fu, WANG Tong-hua, LIU Hai-ou, et al. J. Mater. Sci., , 2004, 39: 5603-5605.
[15] ZHANG Xiong-fu, ZHU Wen-qing, LIU Hai-ou, et al. Mater. Letters., 2004, 58 (17-18): 2223-2226.