High Performance a&b Oriented T Zeolite Membrane by a Two-stage Crystallization Synthesis

doi:10.15541/jim20190469

Abstract

Abstract:

A thin and dense high-performance T-type zeolite membrane was successfully prepared by a two-step seed crystal induction plus two-step temperature-varied hydrothermal synthesis on inexpensive and macroporous α-Al₂O₃ support. This method can fully perform nucleation of seed crystal, regulate the epitaxial growth and crystal growth direction by changing the hydrothermal crystallization temperature and time during the two-stage. Finally a continuous and defect-free a&b oriented zeolite T membrane was obtained. Effects of crystallization temperature and crystallization time of the first-stage and crystallization temperature of the second-stage on the surface structure and properties of zeolite membranes were investigated. The T-type zeolite membrane prepared under the optimal two-step crystallization condition displayed high pervaporation performance with flux over 3.84 kg·m ^-2·h ^-1 and separation factor higher than 10000 for separation of 90wt% isopropanol/water at 75 ℃.

Key words: T zeolite membrane, two-stage crystallization, a&b orientation, pervaporation

CLC Number:

TQ174

ZHANG Bo,ZHANG Ning,YANG Jianhua,LAN Jiancheng,WANG Jinqu. High Performance a&b Oriented T Zeolite Membrane by a Two-stage Crystallization Synthesis[J]. Journal of Inorganic Materials, 2020, 35(8): 939-946.

Figures/Tables 12

Fig. 1 SEM images of α-Al2O3 support photographed from surface (a) and cross section (b), large seeds (c), small seeds (d), modified by large seeds photographed from surface (e) and cross section (f), and the small seed layer photographed from surface (g) and cross section (h)

Fig. 2 XRD patterns of large seeds (a) and small seeds (b)

Fig. 3 SEM images of T-type zeolite membranes after first-step crystallization prepared at different first-step crystallization temperatures (a, b) M1-1, 110 ℃; (c, d) M2-1, 120 ℃; (e, f) M3-1, 130 ℃; (g, h) M4-1, 135 ℃; (i, j) M5-1, 150 ℃

Fig. 4 SEM images of T-type zeolite membranes after two-step crystallizations prepared at different first-step crystallization temperature (a, b) M1, 110 ℃; (c, d) M2, 120 ℃; (e, f) M3, 130 ℃; (g, h) M4, 135 ℃; (i, j) M5, 150 ℃

Fig. 5 XRD patterns of zeolite T membrane M4 (a) and small zeolite T seeds (b)

Table 1 Pervaporation performance of T zeolite membranes prepared under different first-step crystallization temperatures

No.	First-step crystallization		Second-step crystallization		J/ (kg·m^-2·h^-1)	α
No.	Temp./℃	Time/h	Temp./℃	Time/h	J/ (kg·m^-2·h^-1)	α
M1	110	4	110	6	-	-
M2	120	4	110	6	4.19	968
M3	130	4	110	6	3.87	5219
M4	135	4	110	6	3.84	>10000
M5	150	4	110	6	3.53	2918

Fig. 6 SEM images of T-type zeolite membranes after first-step crystallization prepared with varying first-step crystallization time (a, b) M6-1, 2 h; (c, d) M7-1, 3 h; (e, f) M8-1, 5 h; (g, h) M9-1, 6 h

Fig. 7 SEM images of T-type zeolite membranes after two-step crystallizations prepared with different first-step crystallization time (a, b) M6, 2 h; (c, d) M7, 3 h; (e, f) M8, 5 h; (g, h) M9, 6 h

Table 2 Pervaporation performance of T zeolite membranes prepared with different first-step crystallization time

No.	First-step crystallization		Second-step crystallization		J/ (kg ·m^-2·h^-1)	α
No.	Temp./℃	Time/h	Temp./℃	Time/h	J/ (kg ·m^-2·h^-1)	α
M6	135	2	110	6	-	-
M7	135	3	110	6	4.04	915
M4	135	4	110	6	3.84	>10000
M8	135	5	110	6	4.2	2371
M9	135	6	110	6	4.97	697

Fig. 8 SEM images of T-type zeolite membranes after two-step crystallizations prepared at different second-step crystallization temperatures (a, b) M10, 90 ℃; (c, d) M11, 100 ℃; (e, f) M12, 120 ℃; (g, h) M13, 130 ℃

Table 3 Pervaporation performance of T zeolite membranes prepared under different second-step crystallization temperatures

No	First-step crystallization		Second-step crystallization		J/ (kg·m^-2·h^-1)	α
No	Temp./℃	Time/h	Temp./℃	Time/h	J/ (kg·m^-2·h^-1)	α
M10	135	4	90	6	-	-
M11	135	4	100	6	3.94	2646
M4	135	4	110	6	3.84	>10000
M12	135	4	120	6	3.97	5867
M13	135	4	130	6	3.41	5594

Table 4 Pervaporation performance of zeolite T membranes for 90wt% isopropanol/water mixture at 75 ℃

Support	Temp./ ℃	Time/ h	J/ (kg·m^-2·h^-1)	α	Ref.
α-Al₂O₃ disc	120	24	2.24	10000	[29]
α-Al₂O₃ tube	100	30	2.52	10000	[21]
α-Al₂O₃ tube	120	16	2.96	6400	[23]
α-Al₂O₃ tube	100+140^a	8+1^a	2.15	10000	[19]
α-Al₂O₃ tube	150+120^b	4+8^b	2.04	2874	[30]
α-Al₂O₃ tube	135+110^c	4+6^c	3.84	>10000	This work

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