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

doi:10.15541/jim20150411

Abstract

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

CLC Number:

TQ028

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.

Figures/Tables 7

Fig.1 Thermal analysis curves of precursors

Fig. 2 Infrared spectra of samples

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

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

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	--

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

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

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