高氢渗透分离性的沸石杂化支撑炭膜的制备

doi:10.15541/jim20150411

无机材料学报 ›› 2016, Vol. 31 ›› Issue (3): 257-262.DOI: 10.15541/jim20150411 CSTR: 32189.14.10.15541/jim20150411

高氢渗透分离性的沸石杂化支撑炭膜的制备

张兵¹(), 江园¹, 吴永红¹, 鲁云华²(), 赵丹丹¹, 王同华³()

1.沈阳工业大学石油化工学院, 辽阳 111003
2.辽宁科技大学功能材料省级重点实验室, 鞍山 114051
3.大连理工大学精细化工国家重点实验室, 大连 116024

收稿日期:2015-08-31 修回日期:2015-10-10 出版日期:2016-03-20 网络出版日期:2016-02-24
作者简介:
张兵(1977-), 男, 博士, 教授. E-mail: zhangbing@sut.edu.cn
基金资助:
国家自然科学基金(20906063, 21376037, 21436009, 21406102);国家863项目(2012AA03A611);辽宁省自然科学基金(20102170);辽宁省高等学校杰出青年学者基金(LJQ2012010);辽宁省功能材料重点实验室开放课题(USTLKFSY201507)

Fabrication of Zeolite Hybrid Supported Carbon Membranes with High Hydrogen Permselective Performance

ZHANG Bing¹(), JIANG Yuan¹, WU Yong-Hong¹, LU Yun-Hua²(), ZHAO Dan-Dan¹, WANG Tong-Hua³()

1. School of Petrochemical Engineering, Shenyang University of Technology, Liaoyang 111003, China
2. Provincial Key Laboratory of Functional Materials, University of Science and Technology Liaoning, Anshan 114051, China
3. State Key Laboratory of Fine Chemical Engineering, Dalian University of Technology, Dalian 116024, China

Received:2015-08-31 Revised:2015-10-10 Published:2016-03-20 Online:2016-02-24
Supported by:
National Natural Science Foundation of China (20906063, 21376037, 21436009, 21406102);863 High-Tech Project of China (2012AA03A611);Liaoning Natural Science Foundation of China (20102170);Program for Liaoning Excellent Talents in University (LJQ2012010);Liaoning Key Laboratory of Functional Materials (USTLKFSY201507)

摘要/Abstract

摘要：

以ZSM-5沸石掺杂改性的1, 4-双(4-氨基-2-三氟甲基-苯氧基)苯-1, 2, 3, 4-环丁烷四甲酸二酐型聚酰亚胺为前驱体, 通过旋涂成膜和热解过程制备了平板状支撑炭膜。采用热失重、红外光谱、X射线衍射、扫描电镜及气体渗透技术分别研究了前驱体热稳定性、膜表面官能团、微结构, 微观形貌及分离性能。考察了ZSM-5掺杂量及热解温度对炭膜结构和气体分离性的影响。结果表明: 经ZSM-5改性后前驱体热稳定性与残炭量降低, 炭膜微观结构变致密; 加入沸石显著提高了炭膜的渗透性, 且随ZSM-5掺杂量增加, 气体渗透性先减小后增大; 随着热解温度升高, 炭膜的渗透性与选择性皆减小。经650℃热解制得杂化炭膜对H₂/N₂体系的分离性能均远超过Robeson上界限。

关键词: 聚酰亚胺, 沸石, 炭膜, 分离性能

Abstract:

Plate supported carbon membranes were prepared by precursor of 1, 4-bis(4-amino-2-trifluoromethylphenoxy) benzene-1, 2, 3, 4-cyclobutanetetracar-boxylic dianhydride type polyimide modified with zeolite ZSM-5, through the processes of spin-coating and pyrolysis. Thermal stability of precursor, surface functional groups, microstructure, morphology, and separation performance of membranes were characterized by the techniques of thermogravimetric analysis, infrared spectroscopy, X-ray diffraction, scanning electron microscope, and gas permeation, respectively. Effects of incorporating amount of ZSM-5 and pyrolysis temperature on structure and gas separation performance of carbon membranes were investigated. Results show that thermal stability and carbon residue of precursor are reduced by ZSM-5 modification. Simultaneously, the microstructure of carbon membranes becomes more compact. Incorporation of zeolite remarkably increases the gas permeability of carbon membranes. In addition, the gas permeability first decreases then increases with increased incorporation of ZSM-5. As the pyrolysis temperature elevating, both permeability and selectivity of as-obtained carbon membranes decrease. The separation performance of hybrid carbon membranes prepared at pyrolysis temperature of 650℃ is by far the Robeson's upper bound for H₂/N₂ system.

Key words: polyimide, zeolite, carbon membranes, separation performance

中图分类号:

TQ028

张兵, 江园, 吴永红, 鲁云华, 赵丹丹, 王同华. 高氢渗透分离性的沸石杂化支撑炭膜的制备[J]. 无机材料学报, 2016, 31(3): 257-262.

ZHANG Bing, JIANG Yuan, WU Yong-Hong, LU Yun-Hua, ZHAO Dan-Dan, WANG Tong-Hua. Fabrication of Zeolite Hybrid Supported Carbon Membranes with High Hydrogen Permselective Performance[J]. Journal of Inorganic Materials, 2016, 31(3): 257-262.

图/表 7

图1 前驱体膜热分析曲线

Fig.1 Thermal analysis curves of precursors

图2 样品的红外光谱图

Fig. 2 Infrared spectra of samples

图3 不同膜样品的XRD图谱

Fig. 3 XRD patterns of different samples(a) Precursor membranes; (b) Hybrid carbon membranes; (c) Influence of pyrolysis temperature

图4 炭膜的SEM照片

Fig. 4 SEM images of carbon membranes(a) CMZ-0-650; (b) CMZ-0.1wt%-650; (c) CMZ-0.3wt%-650; (d) CMZ-0.5wt%-650

表1 炭膜的气体分离性能数据

Table 1 Data of gas separation performance of carbon membranes

Sample codes	Permeability /Barrer ^a			Selectivity
Sample codes	H₂	CO₂	N₂	H₂/N₂	H₂/CO₂
CMZ-0-650	47.2	41.9	3.6	13.1	1.1
CMZ-0.1wt%-650	1474.6	324.6	15.7	93.9	4.6
CMZ-0.1wt%-750	119.4	48.2	4.1	29.1	2.5
CMZ-0.1wt%-850	51.8	37.9	2.7	19.1	1.4
CMZ-0.3wt%-650	776.6	96.5	11.0	70.5	8.0
CMZ-0.5wt%-650	1029.1	102.3	15.3	67.2	10.0
[22]	628.0	302.0	38.6	16.2	2.1
[23]	298.1	106.8	48.9	6.1	2.8
[22]	308.0	--	--	2.0	--

图5 沸石含量对杂化炭膜渗透性影响示意图

Fig. 5 Schematic of the effect of zeolite content on the permeability for hybrid carbon membranes(a) Low content; (b) Moderate content; (c) High content

图6 炭膜H2/N2分离性的Robeson图

Fig. 6 Robeson's plot of carbon membranes for the separation performance of H2/N2

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高氢渗透分离性的沸石杂化支撑炭膜的制备

Fabrication of Zeolite Hybrid Supported Carbon Membranes with High Hydrogen Permselective Performance

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