芳烃官能化有机硅膜的制备及丙烯/丙烷分离性能

doi:10.16085/j.issn.1000-6613.2023-0443

化工进展 ›› 2024, Vol. 43 ›› Issue (3): 1428-1435.DOI: 10.16085/j.issn.1000-6613.2023-0443

• 材料科学与技术 • 上一篇

芳烃官能化有机硅膜的制备及丙烯/丙烷分离性能

钱俊明¹(), 郭猛¹(), 任秀秀¹, 余亮², 钟璟¹, 徐荣¹()

^1.常州大学石油化工学院，常州大学精细石油化工江苏省重点实验室，江苏常州 213164
^2.北京理工大学前沿交叉科学研究院，北京 100081

收稿日期:2023-03-22 修回日期:2023-06-30 出版日期:2024-03-10 发布日期:2024-04-11
通讯作者: 郭猛,徐荣
作者简介:钱俊明（1997—），男，硕士研究生，研究方向为功能膜材料。E-mail：2429144792@qq.com。
基金资助:
江苏省自然科学基金青年基金(BK20210855);江苏省高校自然科学研究重大项目(22KJA530001);江苏省精细石油化工重点实验室开放课题(KF2105);常州市科技计划(CJ20220140)

Fabrication of aromatic functionalized organosilica membranes and gas separation performance

QIAN Junming¹(), GUO Meng¹(), REN Xiuxiu¹, YU Liang², ZHONG Jing¹, XU Rong¹()

^1.School of Petrochemical Engineering, Jiangsu Province Key Laboratory of Fine Petrochemical Engineering, Changzhou University, Changzhou 213164, Jiangsu, China
^2.Frontier Cross Science Research Institute, Beijing University of Technology, Beijing 100081, China

Received:2023-03-22 Revised:2023-06-30 Online:2024-03-10 Published:2024-04-11
Contact: GUO Meng, XU Rong

摘要/Abstract

摘要：

利用具有单苯和联苯桥联结构的有机硅前体1,4-二(三乙氧基硅基)苯（BTESB）和4,4'-二(三乙氧基硅基)联苯（BTESBPh），通过溶胶-凝胶法制备成有机硅膜并应用于丙烯/丙烷分离。在25℃时，BTESB膜的C₃H₆渗透速率为3.4×10^-9mol/(m²·s·Pa)，C₃H₆/C₃H₈选择性为9.6；BTESBPh膜的C₃H₆渗透速率为1.7×10^-8mol/(m²·s·Pa)，C₃H₆/C₃H₈选择性为10.5。具有联苯桥联结构的BTESBPh膜网络结构更为疏松，可获得更高的气体渗透速率。苯环中大π键与待分离组分C₃H₆中的碳碳双键产生π-π相互作用，有利于C₃H₆组分的优先吸附和渗透。而BTESBPh中联苯结构增强了这一过程，表现为低温测试条件下，BTESBPh膜的C₃H₆/C₃H₈选择性略高于BTESB膜。本研究可为高性能丙烯/丙烷气体分离膜的开发提供参考。

关键词: 有机硅膜, 孔径, 丙烯/丙烷分离, 溶胶-凝胶法, 分子筛分

Abstract:

Two organosilica presursors, 1,4-bis (triethoxysilyl) benzene (BTESB) with benzene bridges and 4,4'-bis (triethoxysilyl) biphenyl (BTESBPh) with biphenyl bridges were utilized for the fabrication of organosilica membranes via the sol-gel strategy. The two membranes were applied to the gas separation. At 25℃, BTESB membrane displayed a C₃H₆ permeance of 3.4×10^-9mol/(m²·s·Pa)and C₃H₆/C₃H₈ selectivity of 9.6. Nevertheless, BTESBPh membrane showed a C₃H₆permeance of 1.7×10^-8mol/(m²·s·Pa) and a comparable C₃H₆/C₃H₈ selectivity of 10.5. BTESBPh membrane networks with biphenyl bridged structures were much looser and could achieve higher gas permeance. The π-π interactions occurred between the big π bond in the benzene ring and the C $̿$ C bond in the C₃H₆ molecules, which was beneficial for the preferential adsorption and permeation of the C₃H₆ molecules. The biphenyl bridges in BTESBPh membranes enhanced the adsorption and permeation process, as evidenced by the increased C₃H₆/C₃H₈ selectivity of the BTESBPh membrane under low testing temperatures. This study could provide a reference for the development of high-performance propylene/propane separation membranes.

Key words: organosilica membranes, pore size, C₃H₆/C₃H₈ separation, sol-gel method, molecular sieving

中图分类号:

O611.4

钱俊明, 郭猛, 任秀秀, 余亮, 钟璟, 徐荣. 芳烃官能化有机硅膜的制备及丙烯/丙烷分离性能[J]. 化工进展, 2024, 43(3): 1428-1435.

QIAN Junming, GUO Meng, REN Xiuxiu, YU Liang, ZHONG Jing, XU Rong. Fabrication of aromatic functionalized organosilica membranes and gas separation performance[J]. Chemical Industry and Engineering Progress, 2024, 43(3): 1428-1435.

图/表 11

图1 BTESBPh与BTESB结构式与溶胶水解聚合后的网络结构示意图

图2 气体性能测试装置示意图

图3 BTESB和BTESBPh溶胶粒径分析

图4 BTESB膜和BTESBPh凝胶粉末热处理后的FTIR图分析

图5 BTESB和BTESBPh凝胶粉末的BET相关数据

图6 BTESB、BTESBPh膜及支撑体截面SEM图

图7 200℃时的BTESB膜和BTESBPh膜的单气体渗透性能

图8 BTESB膜、BTESBPh膜在200～25℃时的温度依存性

图9 BTESB膜和BTESBPh膜的部分气体活化能数据

图10 本工作与其他类型膜的C3H6/C3H8分离性能对比

图11 C3H6/C3H8选择性渗透示意图

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芳烃官能化有机硅膜的制备及丙烯/丙烷分离性能

Fabrication of aromatic functionalized organosilica membranes and gas separation performance

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