Journal of Inorganic Materials ›› 2021, Vol. 36 ›› Issue (6): 579-591.DOI: 10.15541/jim20200555
Special Issue: 【虚拟专辑】分离膜,复相陶瓷(2020~2021)
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LI Ziyi1(), ZHANG Jiajia1, ZOU Xiaoqin2, ZUO Jiayu1, LI Jun1, LIU Yingshu1(), PUI David Youhong3,4
Received:
2020-09-22
Revised:
2020-10-27
Published:
2021-06-20
Online:
2020-12-10
Contact:
LIU Yingshu, professor. E-mail: ysliu@ustb.edu.cn
About author:
LI Ziyi(1990-), male, associate professor. E-mail: ziyili@ustb.edu.cn
Supported by:
CLC Number:
LI Ziyi, ZHANG Jiajia, ZOU Xiaoqin, ZUO Jiayu, LI Jun, LIU Yingshu, PUI David Youhong. Synthesis and Gas Separation of Chabazite Zeolite Membranes[J]. Journal of Inorganic Materials, 2021, 36(6): 579-591.
Method | Advantage | Disadvantage | Status of use |
---|---|---|---|
In-situ synthesis | ① Simple production equipment ② Easy to use | ① Low success rate ② Long synthesis time ③ Difficult to control | Less research, basically used for the synthesis of SAPO-34 membrane |
Secondary growth | ① Simple production equipment ② High success rate ③ Short synthesis time | ① Tedious steps | More research, conducive to large-scale mass production |
Microwave heating | ① High success rate ② Short synthesis time | ① Tedious steps ② High equipment cost ③ High energy consumption | New method, still in basic research stage |
Table 1 Comparison of CHA zeolite membrane synthesis methods
Method | Advantage | Disadvantage | Status of use |
---|---|---|---|
In-situ synthesis | ① Simple production equipment ② Easy to use | ① Low success rate ② Long synthesis time ③ Difficult to control | Less research, basically used for the synthesis of SAPO-34 membrane |
Secondary growth | ① Simple production equipment ② High success rate ③ Short synthesis time | ① Tedious steps | More research, conducive to large-scale mass production |
Microwave heating | ① High success rate ② Short synthesis time | ① Tedious steps ② High equipment cost ③ High energy consumption | New method, still in basic research stage |
Influencing factors | SSZ-13 | SAPO-34 | |
---|---|---|---|
Seed conditions | Support | α-Al2O3, mullite | α-Al2O3 |
Seed crystal | Ball milled nano seeds | Flake nano seeds | |
Seeding method | Dip coating | Wipe, electrophoretic deposition | |
Hydrothermal synthesis conditions | Formula (structure directing agent, Si/Al, water content, cationic species) | Non-pure silica: 1SiO2 : (5-100)Al2O3 : (0.1-0.2)NaOH : (0-0.06)KOH(Oriented growth regulation) : (0.05-0.6)TMAdaOH : (0-0.05)TEAOH : (40-120)H2O Pure silica : 1SiO2 : (0.5-1.4)TMAdaOH : (0.5-1.4)HF : (3-6)H2O | 1Al2O3 : (1-2)P2O5 : (0.3-0.6)SiO2 : (1-4)TEAOH : (0-1.6)DPA : (55-400)H2O |
Temperature | 160-170 ℃ | 180-230 ℃ | |
Time | 24-72 h | 6-30 h | |
Calcination conditions | Conventional calcination | 400-550 ℃ (6-12 h), temperature rise and fall rate (0.2-1) ℃/min | 400-480 ℃ (4-10 h), temperature rise and fall rate (0.5- 2) ℃/min |
Rapid heat treatment | 700-1000 ℃ (0.5-2 min)+conventional calcination | 700 ℃ (1-5 min)+ conventional calcination |
Table 2 Summary table of preferred conditions for secondary synthesis of SSZ-13 membrane and SAPO-34 membrane
Influencing factors | SSZ-13 | SAPO-34 | |
---|---|---|---|
Seed conditions | Support | α-Al2O3, mullite | α-Al2O3 |
Seed crystal | Ball milled nano seeds | Flake nano seeds | |
Seeding method | Dip coating | Wipe, electrophoretic deposition | |
Hydrothermal synthesis conditions | Formula (structure directing agent, Si/Al, water content, cationic species) | Non-pure silica: 1SiO2 : (5-100)Al2O3 : (0.1-0.2)NaOH : (0-0.06)KOH(Oriented growth regulation) : (0.05-0.6)TMAdaOH : (0-0.05)TEAOH : (40-120)H2O Pure silica : 1SiO2 : (0.5-1.4)TMAdaOH : (0.5-1.4)HF : (3-6)H2O | 1Al2O3 : (1-2)P2O5 : (0.3-0.6)SiO2 : (1-4)TEAOH : (0-1.6)DPA : (55-400)H2O |
Temperature | 160-170 ℃ | 180-230 ℃ | |
Time | 24-72 h | 6-30 h | |
Calcination conditions | Conventional calcination | 400-550 ℃ (6-12 h), temperature rise and fall rate (0.2-1) ℃/min | 400-480 ℃ (4-10 h), temperature rise and fall rate (0.5- 2) ℃/min |
Rapid heat treatment | 700-1000 ℃ (0.5-2 min)+conventional calcination | 700 ℃ (1-5 min)+ conventional calcination |
Fig. 4 Schematic diagram of gas separation mechanisms on CHA zeolite membrane before (left) and after (right) the modulation of membrane surface chemistry[24,36,49,83,87] (a) Si/Al regulation; (b) Cation exchange; (c) Heteroatom replacement; (d) Amino functionalization
Serial number | Ref. | Thickness/μm | Temperature/℃ | Pressure/MPa | Gas separation, X/Y | X permeance/ (×10-8, mol·m-2·s-1·Pa-1) | Separation selectivity, X/Y |
---|---|---|---|---|---|---|---|
1 | Kalipcilar[ | 10-40 | 25 | - | H2/n-C4H10 | 14 | 8.7 |
2 | Zheng[ | 10 | 30 | 0.2 | C2H4/C2H6 | 0.29 | 11 |
3 | Feng[ | 4.3 | 20 | 0.138 | Kr/Xe | 12 | 35 |
4 | Yang[ | 3.7 | 22 | - | H2/C3H8 | 8.4 | 810 |
Table 3 Separation performances of H2, hydrocarbon and noble gases on CHA zeolite membranes
Serial number | Ref. | Thickness/μm | Temperature/℃ | Pressure/MPa | Gas separation, X/Y | X permeance/ (×10-8, mol·m-2·s-1·Pa-1) | Separation selectivity, X/Y |
---|---|---|---|---|---|---|---|
1 | Kalipcilar[ | 10-40 | 25 | - | H2/n-C4H10 | 14 | 8.7 |
2 | Zheng[ | 10 | 30 | 0.2 | C2H4/C2H6 | 0.29 | 11 |
3 | Feng[ | 4.3 | 20 | 0.138 | Kr/Xe | 12 | 35 |
4 | Yang[ | 3.7 | 22 | - | H2/C3H8 | 8.4 | 810 |
Serial number | Ref. | Thickness/μm | Temperature/℃ | Pressure/MPa | Gas separation, X/Y | X permeance/ (×10-7, mol·m-2·s-1·Pa-1) | Separation selectivity, X/Y |
---|---|---|---|---|---|---|---|
1 | Kosinov[ | 4-6 | 20 | 0.6 | CO2/CH4 | 2.5 | 42 |
20 | 0.6 | CO2/N2 | 2.5 | 12 | |||
2 | Wu[ | 6-8 | 20 | 0.27 | CO2/CH4 | 2.1 | 178 |
20 | 0.27 | N2/CH4 | 0.18 | 9 | |||
3 | Song[ | 6 | 25 | 0.2 | CO2/CH4 | 5.6 | 56.5 |
25 | 0.2 | N2/CH4 | 0.89 | 10 | |||
4 | Li[ | 2 | 25 | 0.2 | CO2/CH4 | 1.16 | 213 |
25 | 0.2 | N2/CH4 | 1.07 | 13 | |||
5 | Yu[ | 1.5 | -24 | 0.9 | CO2/CH4 | 79 | 76 |
6 | Karakiliç[ | 2-4 | 22 | 0.2 | CO2/CH4 | 2.6 | 176 |
7 | Qiu[ | 0.44 | 20 | 0.14 | CO2/CH4 | 48 | 153 |
8 | Kida[ | - | 40 | 0.1 | CO2/CH4 | 17 | 54 |
40 | 0.1 | H2/CH4 | 11 | 34 | |||
9 | Tang[ | 10 | 20 | 0.2 | CO2/CH4 | 9.3 | 208 |
10 | Kida[ | 5 | 25 | 0.1 | CO2/CH4 | 40 | 130 |
11 | Imasaka[ | 3 | 40 | 0.3 | CO2/CH4 | 15 | 115 |
12 | Maghsoudi[ | 20 | 30 | 0.1 | CO2/CH4 | 0.34 | 21.6 |
13 | Yu[ | 1.3 | 3 | 0.9 | CO2/CH4 | 84 | 47 |
14 | Li[ | 5 | 80 | 0.14 | CO2/CH4 | 2.0 | 270 |
15 | Li[ | - | 24 | 0.138 | CO2/CH4 | 1.6 | 67 |
16 | Carreon[ | - | 22 | 0.138 | CO2/CH4 | 3.8 | 170 |
17 | Venna[ | - | 22 | 0.138 | CO2/CH4 | 5.0 | 245 |
22 | 0.138 | CO2/N2 | 2.1 | 39 | |||
18 | Huang[ | 2 | 22 | 0.074 | N2/CH4 | 4.93 | 11.3 |
19 | Chen[ | 2-3 | 25 | 0.1 | CO2/CH4 | 1.18 | 160 |
20 | Chang[ | - | - | 4 | CO2/CH4 | 6.1 | 88 |
21 | Liu[ | 3 | 30 | 0.1 | CO2/CH4 | 12 | 95 |
22 | Rehman[ | - | 80 | 0.4 | CO2/CH4 | 47.3 | 65 |
23 | Liu[ | 7-15 | 25 | 0.1 | CO2/N2 | 18.5 | 29.8 |
24 | Li[ | 4-6 | 22 | 7 | CO2/CH4 | 0.4 | 100 |
25 | Zhang[ | - | 20 | 4.6 | CO2/CH4 | 8.2 | 55 |
26 | Noble[ | - | 22 | 0.14 | CO2/CH4 | 1.2 | 170 |
27 | Shi[ | 2-4 | 22 | 0.14 | CO2/CH4 | 23.2 | 186 |
28 | Shi[ | 4-5 | 22 | 0.14 | CO2/CH4 | 16.8 | 256 |
29 | Li[ | 3 | - | 4 | CO2/CH4 | 13.2 | 62 |
30 | Bai[ | 0.8 | - | 0.2 | CO2/CH4 | 25.3 | 70 |
Table 4 Separation performances of CO2/CH4, CO2/N2, N2/CH4, H2/CH4 on CHA zeolite membranes
Serial number | Ref. | Thickness/μm | Temperature/℃ | Pressure/MPa | Gas separation, X/Y | X permeance/ (×10-7, mol·m-2·s-1·Pa-1) | Separation selectivity, X/Y |
---|---|---|---|---|---|---|---|
1 | Kosinov[ | 4-6 | 20 | 0.6 | CO2/CH4 | 2.5 | 42 |
20 | 0.6 | CO2/N2 | 2.5 | 12 | |||
2 | Wu[ | 6-8 | 20 | 0.27 | CO2/CH4 | 2.1 | 178 |
20 | 0.27 | N2/CH4 | 0.18 | 9 | |||
3 | Song[ | 6 | 25 | 0.2 | CO2/CH4 | 5.6 | 56.5 |
25 | 0.2 | N2/CH4 | 0.89 | 10 | |||
4 | Li[ | 2 | 25 | 0.2 | CO2/CH4 | 1.16 | 213 |
25 | 0.2 | N2/CH4 | 1.07 | 13 | |||
5 | Yu[ | 1.5 | -24 | 0.9 | CO2/CH4 | 79 | 76 |
6 | Karakiliç[ | 2-4 | 22 | 0.2 | CO2/CH4 | 2.6 | 176 |
7 | Qiu[ | 0.44 | 20 | 0.14 | CO2/CH4 | 48 | 153 |
8 | Kida[ | - | 40 | 0.1 | CO2/CH4 | 17 | 54 |
40 | 0.1 | H2/CH4 | 11 | 34 | |||
9 | Tang[ | 10 | 20 | 0.2 | CO2/CH4 | 9.3 | 208 |
10 | Kida[ | 5 | 25 | 0.1 | CO2/CH4 | 40 | 130 |
11 | Imasaka[ | 3 | 40 | 0.3 | CO2/CH4 | 15 | 115 |
12 | Maghsoudi[ | 20 | 30 | 0.1 | CO2/CH4 | 0.34 | 21.6 |
13 | Yu[ | 1.3 | 3 | 0.9 | CO2/CH4 | 84 | 47 |
14 | Li[ | 5 | 80 | 0.14 | CO2/CH4 | 2.0 | 270 |
15 | Li[ | - | 24 | 0.138 | CO2/CH4 | 1.6 | 67 |
16 | Carreon[ | - | 22 | 0.138 | CO2/CH4 | 3.8 | 170 |
17 | Venna[ | - | 22 | 0.138 | CO2/CH4 | 5.0 | 245 |
22 | 0.138 | CO2/N2 | 2.1 | 39 | |||
18 | Huang[ | 2 | 22 | 0.074 | N2/CH4 | 4.93 | 11.3 |
19 | Chen[ | 2-3 | 25 | 0.1 | CO2/CH4 | 1.18 | 160 |
20 | Chang[ | - | - | 4 | CO2/CH4 | 6.1 | 88 |
21 | Liu[ | 3 | 30 | 0.1 | CO2/CH4 | 12 | 95 |
22 | Rehman[ | - | 80 | 0.4 | CO2/CH4 | 47.3 | 65 |
23 | Liu[ | 7-15 | 25 | 0.1 | CO2/N2 | 18.5 | 29.8 |
24 | Li[ | 4-6 | 22 | 7 | CO2/CH4 | 0.4 | 100 |
25 | Zhang[ | - | 20 | 4.6 | CO2/CH4 | 8.2 | 55 |
26 | Noble[ | - | 22 | 0.14 | CO2/CH4 | 1.2 | 170 |
27 | Shi[ | 2-4 | 22 | 0.14 | CO2/CH4 | 23.2 | 186 |
28 | Shi[ | 4-5 | 22 | 0.14 | CO2/CH4 | 16.8 | 256 |
29 | Li[ | 3 | - | 4 | CO2/CH4 | 13.2 | 62 |
30 | Bai[ | 0.8 | - | 0.2 | CO2/CH4 | 25.3 | 70 |
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