Synthesis of High-performance AlPO4-14 Zeolite Membranes for Gas Separation †

doi:10.7503/cjcu20190255

Abstract

Abstract:

The AlPO₄-14 molecular sieve membrane with high separation performance was prepared. Firstly, the uniform AlPO₄-14 zeolite with the size of 15—18 mm was obtained by controlling the amount of water and template in the reaction sols of zeolite. Then, the AlPO₄-14 zeolite size was further regulated through a seed method by adding the AlPO₄-14 zeolite seeds into the reaction sols, through which not only the zeolite size was reduced from 15—18 mm to 2—3 mm with uniform plate-like morphology, but also the synthesis time was effectively shortened. Lastly, AlPO₄-14 zeolite membranes were fabricated on mullite supports via a secondary growth method, and two different sizes of zeolite seeds(large size: 15—18 mm, small size: 2—3 mm) were used to explore the effect of seeds size on membrane morphology and separation performance. Results revealed that the separation layers of the resulting membranes prepared from large-sized seeds showed many defects, while the membranes prepared from small-sized seeds were more uniform and defect-free. Besides, the AlPO₄-14 zeolite membranes kept its own crystal structure after template removal at 425 ℃, indicating that the se-condary growth method promoted the growth of AlPO₄-14 crystals in the membrane and endowed membrane with high crystallinity and thermal stability. The best AlPO₄-14 zeolite membrane displayed H₂ permeance of 6.3×10 ^-7 mol·(m ²·s·Pa) ^-1 and CO₂ permeance of 9×10 ^-7 mol·(m ²·s·Pa) ^-1 with ideal selectivities of 28, 40 and 1047 for H₂/CH₄, CO₂/CH₄ and H₂/CF₄, respectively; for the equimolar CO₂/CH₄ mixture separation, the selectivity was as high as 81.5 with CO₂ permeance of 8.8×10 ^-7 mol·(m ²·s·Pa) ^-1 at 25 ℃ and 100 kPa pressure drop.

Key words: Aluminophosphate molecular sieve, AlPO₄-14 zeolite membrane, Seed method, Secondary growth method, CO₂/CH₄ separation

CLC Number:

O611

TrendMD:

SHAO Guoquan,ZHU Hui,MA Wei,YAN Pan,MA Jilong. Synthesis of High-performance AlPO₄-14 Zeolite Membranes for Gas Separation ^†[J]. Chem. J. Chinese Universities, 2019, 40(11): 2265.

Figures/Tables 11

Scheme 1 Schematic illustration of the synthesis of AlPO4-14 zeolite membranes

Fig.1 Schematic diagram of gas permeation setup 1. Stop valve; 2. mass flow controller; 3. pressure gauge; 4. oven; 5. membrane cell; 6. rubber O-ring; 7. membrane; 8. back pressure valve; 9. bubble film meter; 10. gas sampler; 11. gas chromatograph.

Sample	n(Al₂O₃)/mol	n(P₂O₅)/mol	n(C₃H₉N)/mol	n(H₂O)/mol
S1	1	1	1	45
S2	1	1	1.5	45
S3	1	1	1	70
S4	1	1	1	100

Fig.2 SEM images of AlPO4-14 zeolite prepared from different sols (A) S1; (B) S2; (C) S3; (D) S4.

Sample^*	n(Al₂O₃)/mol	n(P₂O₅)/mol	n(C₃H₉N)/mol	n(H₂O)/mol
SS2	1	1	1.5	45
SS3	1	1	1	70
S3-24 h	1	1	1	70

Fig.3 SEM images of AlPO4-14 zeolite prepared by the secondary growth (A),(B) SS2; (C) SS3; (D) S3-24 h.

Fig.4 XRD patterns of AlPO4-14 powders and membranes a. as-synthesized AlPO4-14 powders SS2; b. as-synthesized AlPO4-14 membrane M-SS2; c. calcined AlPO4-14 membrane M-SS2.

Fig.5 SEM images of calcined AlPO4-14 membranes (A) Surface section of M-S2;(B) cross section of M-S2;(C) surface section of M-SS2;(D) cross section of M-SS2.

Fig.6 Single-gas permeances of different gases through AlPO4-14 membrane M-SS2 at 25 ℃ The inset shows the ideal selectivities for H2 and CO2 over other gases.

Fig.7 Temperature dependence of selectivity and permeance through the AlPO4-14 membrane M-SS2 in an equimolar CO2/CH4 mixture The solid symbols represent the data in mixtures and the open ones represent the data in single gas.

Fig.8 Comparison of AlPO4-14 membrane with other membranes Present upper bound for polymeric membranes from Robeson plot(2008)[23], zeolite T[24], DDR[25], AlPO-18[5,6,26] and SAPO-34[27,28], 1 Barrer=3.348×10-16 mol·(m·Pa·S)-1.

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Synthesis of High-performance AlPO₄-14 Zeolite Membranes for Gas Separation ^†

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