Synthesis of least defect NaY membranes: Defining optimum heating and cooling rate of hydrothermal treatment (HT) and application of zeta potential measurement via different seeding methods


  • Muhammad Aimen Isa PETRONAS Research Sdn. Bhd
  • Muhammad Hanif Halim PETRONAS Research Sdn. Bhd



NaY, zeolite membrane, zeta potential, dip-coating, spin coating, vacuum coating, seeding, cracks, pinholes



Zeolite membrane is one type of microporous inorganic membrane which has gained so much interests among researchers as an alternative especially for gas separation. Among major challenges to produce high quality zeolite membranes with less defects are to have a good seeding and hydrothermal treatment (HT) method. On this matter, a study on the colloidal stability of the zeolite NaY seeds in the seeds solution in order to obtain homogenous seeds layer on top of the alumina support via several seeding methods and pHs of the seeds solutions were investigated. Then, the seeded samples were taken into HT process in order to form zeolite NaY membranes. During this stage, heating and cooling rates (oC/hr) were varied in order to study their effects towards formation of zeolite membrane with least defects. Characterizations were performed by using X-Ray Diffraction (XRD) in order to identify degree of crystallization and amount of impurities while Scanning Electron Microscopy (SEM) was used in order to study surface morphology of the samples. From this study, it was found that densification effect from different seeding methods played important factor in forming zeolite membranes with least defects. Accordingly, suitable heating and cooling rates were required in order to optimize the growths of zeolite NaY seeds to form zeolite layer on top of the alumina support. In this case, due to thermal mismatch between the substrate and zeolite material, it could form some cracks on top of the alumina support. Thus, by implementing optimum heating/cooling rate, a zeolite NaY membrane with least amount of defects i.e. cracks and pinholes could be achieved with less degree of impurities i.e. zeolite NaP during HT process.

Author Biographies

Muhammad Aimen Isa, PETRONAS Research Sdn. Bhd

Gas Sustainability Technology R&D Department

Muhammad Hanif Halim, PETRONAS Research Sdn. Bhd

Gas Sustainability Technology R&D Department


Aziz, S. A. A. Amirnordin, S. H., Rahman, H. A., and Abdullah, H. Z. 2013. Effect of zeta potential of stanum oxide (SnO2) on electrophoretic deposition (EPD) on porous alumina. Advanced Materials Research, 795, pp.334–337.

Algieri, C., Bernardo, P., Barbieri, G., and Drioli, E. 2009. A novel seeding procedure for preparing tubular NaY zeolite membranes. Microporous and Mesoporous Materials, 119(1–3), pp.129–136.

Aoki, K., Tuan, V. A., Falconer, J. L., and Noble, R. D. 2000. Gas permeation properties of ion-exchanged ZSM-5 zeolite membranes. Microporous and Mesoporous Materials, 39(3), pp.485–492.

Asghari, M., Mohammadia, T., Aziznia, A., Danayi, M. R. , Moosavi, S. H.,. Alamdari, R. F., and Agan, F. 2008. Preparation and characterization of a thin continuous faujasite membrane on tubular porous mullite support. Desalination, 220(1–3), pp.65–71.

Caro, J., and Noack, M. 2008. Zeolite membranes - Recent developments and progress. Microporous and Mesoporous Materials, 115(3), pp. 215–233.

Chaves, T.F., Pastore, H.O. and Cardoso, D. 2016. Synthesis and properties of zeolite FAU with nanocrystals. Microporous and Mesoporous Materials, 161(February), pp. 67–75.

Cheng, Z., Gao, E., Wan, H. and Processes, C. 2004. Novel synthesis of FAU-type zeolite membrane with high performance †. Chemical Communications, (c), pp.1718–1719.

Cheng, Z. and Han, S. 2015. Synthesis and separation performance of Y-type zeolite membranes by pre-seeding using electrophoresis deposition method. China Petroleum Processing & Petrochemical Technology, 17(4), pp.62–70.

Chew, T. L., Ahmad, A. L. and Bhatia, S. 2011. Ba-SAPO-34 membrane synthesized from microwave heating and its performance for CO2/CH4 gas separation. Chemical Engineering Journal, 171(3), pp.1053–1059.

Das, J. K., Das, N. and Bandyopadhyay, S. 2012. Effect of PVP intermediate layer on the properties of SAPO 34 membrane. Advances in Materials Science and Engineering, 2012, article ID 650127.

Das, N., Kundu, D. and Chatterjee, M. 2010. The effect of intermediate layer on synthesis and gas permeation properties of NaA zeolite membrane. Journal of Coatings Technology and Research, 7(3), pp.383–390.

Dey, K. P., Kundu, D., Chatterjee, M. and Naskar, M. K. 2013. Preparation of NaA zeolite membranes using poly(ethyleneimine) as buffer layer, and study of their permeation behavior. Journal of the American Ceramic Society, 96(1), pp.68–72.

Feng, C., Khulbe, K. C., Matsuur, T., Farnood, R. and Ismail, A. F. 2015. Recent progress in zeolite/zeotype membranes. Journal of Membrane Science and Research, 1(2), pp.49–72.

Fu, X.-L., Zeng, M., Zhou, J.-B. and Xu, C. 2017. A novel cellulose–silicalite-1 membrane with excellent gas separation property. RSC Advances, 7, pp.41070–41076.

Gu, X., Dong, J. and Nenoff, T. M. 2005. Synthesis of defect-free FAU-Type zeolite membranes and separation for dry and moist CO 2 / N 2 mixtures. Industrial & Engineering Chemistry Research, 44(4), pp.937–944.

Gualtieri, M. 2006. Synthesis and characterization of zeolite films and membranes (Unpublished PhD thesis). Luleå University of Technology, Luleå, Sweden.

Hasegawa, Y., Tanaka, T., Watanabe, K., Jeong, B.-H., Kusakabe, K. and Morooka, S. 2002. Separation of CO2-CH4 and CO2-N2 systems using ion-exchanged FAU-type zeolite membranes with different Si/Al ratios. Korean Journal of Chemical Engineering, 19(2), pp.309–313.

Hasegawa, Y., Watanabe, K., Kusakabe, K. and Morooka, S., 2002. Influence of alkali cations on permeation properties of Y-type zeolite membranes. Journal of Membrane Science, 208(1–2), pp.415–418.

Hong, M., Li, S., Funke, H. F., Falconer, J. L. and Noble, R. D. 2007. Ion-exchanged SAPO-34 membranes for light gas separations. Microporous and Mesoporous Materials, 106(1–3), pp.140–146.

Huang, A., Lin, Y. S. and Yang, W. 2004. Synthesis and properties of A-type zeolite membranes by secondary growth method with vacuum seeding. Journal of Membrane Science, 245(1–2), pp.41–51.

Huang, A., Wang, N. and Caro, J., 2012a. Seeding-free synthesis of dense zeolite FAU membranes on 3-aminopropyltriethoxysilane-functionalized alumina supports. Journal of Membrane Science, 389, pp.272–279.

Huang, A., Wang, N. and Caro, J., 2012b. Synthesis of multi-layer zeolite LTA membranes with enhanced gas separation performance by using 3-aminopropyltriethoxysilane as interlayer. Microporous and Mesoporous Materials, 164, pp.294–301.

Kita, H., Fuchida, K., Horita, T., Asamura, H., and Okamoto, K. 2001. Preparation of Faujasite membranes and their permeation properties. Separation and Purification Technology, 25(1–3), pp.261–268.

Kosinov, N., Gascon, J., Kapteijn, F. and Hensen, E. J. M., 2016. Recent developments in zeolite membranes for gas separation. Journal of Membrane Science, 499, pp.65–79.

Kuzniatsova, T., Kim, Y., Shqau, K., Dutta, P. K. and Verweij, H. 2007. Zeta potential measurements of zeolite Y: Application in homogeneous deposition of particle coatings. Microporous and Mesoporous Materials, 103(1–3), pp.102–107.

Lang, W. Z., Ouyang, J. X., Guo, Y. J. and Chu, L. F., 2011. Synthesis of tubular faujasite X-type membranes with mullite supports and their gas permeances for N2/CO2 mixtures. Separation Science and Technology, 46(11), pp.1716–1725.

Li, H., Wang, J., Xu, J., Meng, X., Xu, B., Yang, J., Li, S., Lu, J., Zhang, Y., He, X., and Yin, D. 2013. Synthesis of zeolite NaA membranes with high performance and high reproducibility on coarse macroporous supports. Journal of Membrane Science, 444, pp.513–522.

Li, Q., Creaser, D. and Sterte, J., 2002. An investigation of the nucleation/crystallization kinetics of nanosized colloidal faujasite zeolites. Chemistry of Materials, 14(3), pp.1319–1324.

Liu, Y., Yang, Z., Yu, C., Gu, X., and State, N. X. 2011. Effect of seeding methods on growth of NaA zeolite membranes. Microporous and Mesoporous Materials, 143(2–3), pp.348–356.

Liu, Z., Shi, C., Wu, D., He, S., and School, B. R. 2016. A simple method of preparation of high silica zeolite Y and its performance in the catalytic cracking of cumene. Journal of Nanotechnology, 2016, Article ID 1486107.

Ma, J., Shao, J., Wang, Z. and Yan, Y. 2014. Preparation of zeolite NaA membranes on macroporous alumina supports by secondary growth of gel layers. Industrial and Engineering Chemistry Research, 53(14), pp.6121–6130.

Mason, G., 2012. The development of online learning designs for patients with type 2 diabetes. Studies in Health Technology and Informatics, 2012, pp. 130–135.

Mastropietro, T. F., Brunetti, A., Zito, P., Poerio, T., Richter, H., Weyd, M., Wöhner, S., Driolia, E., and Barbieri, G. 2015. Study of the separation properties of FAU membranes constituted by hierarchically assembled nanozeolites. Separation and Purification Technology, 156(part 2), pp.321–327.

Motazedi, K., Mahinpey, N. and Karami, D., 2016. Preparation and application of faujasite-type Y zeolite-based catalysts for coal pyrolysis using sodium silicate solution and colloidal silica as silicon source. Chemical Engineering Communications, 203(3), pp.300–317.

O’Brien-Abraham, J. and Lin, J. Y. S., 2010. Zeolite membrane separations. In S. Kulpathripanja (ed.) Zeolites in Industrial Separation and Catalysis (pp.307–327). Retrieved from

Peng, Y., Zhan, Z., Shan, L., Li, X., Wang, Z., and Yan, Y. 2013. Preparation of zeolite MFI membranes on defective macroporous alumina supports by a novel wetting-rubbing seeding method: Role of wetting agent. Journal of Membrane Science, 444, pp.60–69.

Sato, K., Sugimoto, K., Sekine, Y., Takada, M., Matsukata, M., and Nakane, T. 2007. Application of FAU-type zeolite membranes to vapor/gas separation under high pressure and high temperature up to 5 MPa and 180°C. Microporous and Mesoporous Materials, 101(1-2 SPEC. ISS.), pp.312–318.

Sato, K., Sugimoto, K. and Nakane, T. 2008a. Mass-production of tubular NaY zeolite membranes for industrial purpose and their application to ethanol dehydration by vapor permeation. Journal of Membrane Science, 319(1–2), pp.244–255.

Sato, K., Sugimoto, K. and Nakane, T. 2008b. Synthesis of industrial scale NaY zeolite membranes and ethanol permeating performance in pervaporation and vapor permeation up to 130°C and 570 kPa. Journal of Membrane Science, 310(1–2), pp.161–173.

Severance, M. A., 2014. Nanocrystalline zeolites: Synthesis, mechanism, and applications (Unpublished PhD dissertation). The Ohio State University, Ohio, United States.

Shah, M. and Muzyyan, N. 2009. A novel approach for the synthesis of tungsten trioxide nanostructures. Journal of King Abdulaziz University-Science, 21(1), pp.109–115.

Sun, G., Liu, Y., Yang, J., and Wang, J. 2011. Seeded synthesis of small polycrystalline NaY zeolite membrane using zeolite structure-directing agent and its pervaporation performance. Journal of Porous Materials, 18(4), pp.465–473.

Wang, B., Ho, W. S. W., Figueroa, J. D. and Dutta, P. K., 2015. Bendable zeolite membranes: synthesis and improved gas separation performance. Langmuir, 31(24), pp.6894–6901.

Wang, P. and Keller, A. A., 2009. Natural and engineered nano and colloidal transport: Role of zeta potential in prediction of particle deposition. Langmuir, 25(12), pp.6856–6862.

Wang, Z., Ge, Q., Gao, J., Shao, J., Liu, C., and Yan, Y. 2011. High-performance zeolite membranes on inexpensive large-pore supports: Highly reproducible synthesis using a seed paste. ChemSusChem, 4(11), pp.1570–1573.

Wang, Z., Kumakiri, I., Tanaka, K., Chen, X., and Kita, H. 2013. NaY zeolite membranes with high performance prepared by a variable-temperature synthesis q. Microporous and Mesoporous Materials, 182, pp.250–258.

Wee, L. H., Tosheva, L., Itani, L., Valtchev, V., and Doyle, A. M. 2008. Steam-assisted synthesis of zeolite films from spin-coated zeolite precursor coatings. Journal of Materials Chemistry, 18(30), pp.3563–3567.

Wong, W. C., Au, L. T. Y., Ariso, C. T. and Yeung, K. L. 2001. Effects of synthesis parameters on the zeolite membrane growth. Journal of Membrane Science, 191(1–2), pp.143–163.

Xu, G., Zhang, J. and Song, G. 2003. Effect of complexation on the zeta potential of silica powder. Powder Technology, 134(3), pp.218–222.

Xu, K., Jin, H., Wang, L., Liu, Y., Zhou, C., Caro, J., and To, A. H. 2018. Seeding-free synthesis of oriented zeolite LTA membrane on PDI-modified support for dehydration of alcohols. Separation Science and Technology (Philadelphia), 53(11), pp.1741–1751.

Zhu, G., Qiu, S., Yu, J., Sakamoto, Y., Xiao, F., Xu, R., and Terasaki, O. 1998. Synthesis and characterization of high-quality zeolite LTA and FAU single nanocrystals. Chemical Materials, 4756(18), pp.1483–1486.