Engineered Zeolite Membranes
(January 1997 - present)
Publications and Presentations
A new synthesis technique has been developed for the preparation of zeolite membranes with engineered structure and tailored chemistry [1,10,11,15]. Mesoporous layers of colloidal zeolite seeds are deposited onto the support material and the intercrystalline voids between seed particles are regrown under hydrothermal condition to yield a well-intergrown zeolite film. In the traditional seed and regrow method (i.e., ex situ synthesis), the zeolite crystallizes outward from the surface of the seed layer. The resulting membrane consists of two distinct layers of seed and polycrystalline zeolite film, while the new synthesis technique yields one continuos zeolite membrane layer resulting in more stable membrane that has better separation performance. Submicron (i.e., 0.2 mm) to 40-mm thick zeolite membranes have been successfully grown onto porous glass, alumina and stainless steel supports [2-9]. The membrane morphology [5], grain size and shape [5,7], as well as film orientation [6] have been successfully engineered to produce membranes with the desired gas permeation properties. Membranes with different Al, B, Ti and V frame work metal ions (i.e., ZSM-5, BZSM-5, TS-1 and VS-1, respectively) have been prepared and tested [8,9,23,25]. The new technique also enables the preparation of zeolite membranes with non-uniform distribution of framework metal ions [15]. The spatial concentration and location of the metal ions along the width of the zeolite membrane can be precisely controlled.
The project addresses the fundamental issues of zeolite membrane synthesis, i.e., investigating the relationship between synthesis variables and the membrane's structural, chemical and separation properties. The research also explores the potential applications of zeolite membrane technology for industry. This project is sponsored by both Hong Kong government research grant council (HK-RGC) and by international companies (i.e., ExxonMobil and Vivendi).
1. DAG96/97.EG33 Zeolite Technology for a Cleaner Environment: Synthesis Methodology.
PRINCIPAL INVESTIGATOR: King Lun Yeung
STATUS: Completed
SUMMARY: The funding supported a systematic study of zeolite membrane synthesis onto porous support materials. The effects of synthesis variables on membrane formation and growth have been investigated, and the role of the support material in zeolite deposition has been elucidated. A comparison of various synthesis methodologies for zeolite membranes was also conducted to determine the best synthesis strategy.
2. HKUST6118/97P Membrane technology for a cleaner environment: Synthesis and application of zeolite membranes.
PRINCIPAL INVESTIGATOR: King Lun Yeung
STATUS: Completed
SUMMARY: A novel synthesis technique for "Engineered Zeolite Membranes" has been developed which allows the precise control of the structural, chemical, separation and catalytic properties of the zeolite membranes. The synthesis methodology is general and can be applied to other inorganic membrane systems. The technology has potential for revolutionizing the preparation of zeolite membranes. A membrane pervaporation unit has also been designed and constructed for testing the zeolite membrane performance in solvent recovery and reuse from industrial wastewater.
3. HKUST6072/99P Separation Properties of Engineered Zeolite Membranes.
PRINCIPAL INVESTIGATOR: King Lun Yeung
STATUS: On-going (September, 1999 - present)
SUMMARY: Engineered zeolite membranes with controlled thickness, microstructure and orientations were prepared using a novel synthesis technique developed by the author. The technique also provides a precise method for tailoring the chemical nature of the zeolite membranes. The aim of the research is to develop a model for the transport properties of gases across the zeolite membrane as a function of the physical and chemical properties of the membrane material. Work is in progress to evaluate the permeation properties of different permanent gases and hydrocarbons across the zeolite membrane.
4. DAG99/00.EG19 Separation properties of zeolite membranes with engineered structure and tailored chemistry.
PRINCIPAL INVESTIGATOR: King Lun Yeung
STATUS: On-going (December, 1999 - present)
SUMMARY: Engineering of zeolite membrane structure through zeolite thin film technology and microfabircation methods developed in our laboratory. The new fabrication methods enabled the precise incorporation of zeolite catalysts and membranes within the architecture of the microreactors and membrane microseparators.
5. Exxon001.99/00 Fundamental study of the mechanical properties of supported silicalite-1 films in relation to their transport characteristics.
PRINCIPAL INVESTIGATOR: King Lun Yeung
STATUS: Completed
SUMMARY: Investigated the effects of zeolite membrane microstructure on its thermomechanical properties during high temperature separation.
6. PDF99/00 Fundamental transport mechanism across zeolite membrane: Effects of structure and chemistry on the membrane separation properties.
PRINCIPAL INVESTIGATOR: King Lun Yeung
STATUS: On-going (May 2001 - present)
SUMMARY: The objective is to study the permeation and separation properties of gases and hydrocarbons across small- (NaA), medium- (ZSM-5) and large- (NaX) pore zeolite membranes with well-defined structure and chemistry.
7. HKUST-Anjou Recherche JRC Catalytically activated membrane for industrial wastewater treatment.
PRINCIPAL INVESTIGATOR: King Lun Yeung
STATUS: On-going (October 2000 - present)
SUMMARY: The objective of the study is to develop membrane assisted catalytic process for effective wastewater treatment.
8. HKUST6009 02P Engineered zeolite micromembranes.
PRINCIPAL INVESTIGATOR: King Lun Yeung
STATUS: On-going (December 2002 - present)
SUMMARY: This project investigates the fundamental issues in zeolite micromembrane synthesis, in particular their incorporation and growth within the confined environment of a microsystem, and to establish the relationship between synthesis parameters and the physicochemical, thermomechanical and transport properties of the zeolite micromembranes.
9. HKUST-Veolia Water-Anjou Recherches A membrane process for water and wastewater applications
PRINCIPAL INVESTIGATOR: King Lun Yeung
STATUS: On-going (October 2003 - present)
SUMMARY: The objective of the study is to develop membrane-assisted technology for the treatment and remediation of wastewater and production of clean water.
Students: (3 post-doctoral researchers, 3 Ph. D., 4 M. Phil., 3 UG students, 2 Research Assistants)
Mr. Wan Cheong Wong (M. Phil. student, September, 1997 - January, 2000)
Mr. Joseph L. H. Chau (M. Sc. student, January-December, 1997; Ph. D. student, January, 1998 - August, 2001)
Dr. Juan Baranda (Research Associate, May, 1998 - November, 1999)
Ms. Louisa T. Y. Au (part time Jr. R.A., January, 1998 - May, 1998; M. Phil. student, September, 1998 - February, 2001)
Ms. Pui Hang Chung (UG student (CENG 298), May-August, 1998; part time Jr. R.A., September-December, 1998)
Dr. Carlos A. Tellez (Research Associate, March 1999 - March 2000)
Ms. Prudence P. S. Lau (part time Jr. R.A., January - May, 1999; M. Phil. student, September 1999 - August 2002)
Ms. Emily S. M. Lai (UG student (CENG 298), May-August, 1999)
Mr. Etienne Brois (Research Assistant, October 2000 - January 2002)
Mr. Adrian L.Y. Leung (UG student (CENG 398), May-August, 2000; M. Phil. student, September 2001 - present)
Mr. Wai Yin Mui (UG student (CENG 398), May-August, 2000)
Dr. Xiongfu Zhang (Research Associate, May 2001 - May 2003)
Mr. Samuel Heng (Research Assistant, February 2002 - August 2003; Ph. D. student, September 2003 - present)
Mr. Michael KWAN, Siu Ming (Ph. D. student, September 2003 - present)
Publications and Presentations:(12 peer-reviewed journal manuscripts, 27 presentations)
1. L.H. Chau, W.C. Wong and K.L. Yeung, "New synthesis method for thin supported zeolite membranes: Membrane orientation and nonuniform distribution of framework ions," Proceedings of the 5th ICIM (1998) 432.
2. J.L.H. Chau, C. Tellez, K.L. Yeung and N.K. Ho, "The role of surface chemistry on zeolite membrane formation," J. Membr. Sci., 164 (2000) 257-275. PDF file
3. L.T.Y., Au, J.L.H. Chau, C. Tellez and K.L. Yeung, "Preparation of supported Sil-1, TS-1 and VS-1 membranes: Effects of Ti and V metal ions on the membrane synthesis and permeation properties," J. Membr. Sci., 183 (2001) 269-291. PDF file
4. W.C. Wong, L.T.Y., Au, C. Tellez and K.L. Yeung, "Effects of synthesis parameters on the zeolite membrane growth," J. Membr. Sci., 191 (2001) 143-163. PDF file
5. W.C. Wong, L.T.Y. Au, P.S. Lau, C. Tellez and K.L. Yeung, "Effects of synthesis parameters on the zeolite membrane morphology," J. Membr. Sci., 193 (2001) 141-161. PDF file
6. L.T.Y. Au and K.L. Yeung, "An investigation of the relationship between microstructure and permeation properties of ZSM-5 membranes," J. Membr. Sci., 194 (2001) 33-55. PDF file
7. L.T.Y. Au, W.Y. Mui, P.S. Lau, C. Tellez and K.L. Yeung, "Engineering the shape of zeolite crystal grain in MFI membrane and their effects on the gas permeation properties," Microporous and Mesoporous Mater., 47 (2001) 203-216. PDF file
8. E.S.M. Lai, L.T.Y. Au and K.L. Yeung, "Influence of synthesis conditions and growth environment on MFI zeolite film orientation," Microporous and Mesoporous Mater., 54 (2002) 63-77. PDF file
9. X.F. Zhang, J.Q. Wnag, H.O. Liu, C.H. Liu and K.L. Yeung, "Factors affecting the synthesis of hetero-atom zeolite Fe-ZSM-5 membrane," Sep. and Puri. Technol., 32 (2003) 151-158.
10. J.L.H. Chau, A.Y.L. Leung, M.B. Shing, K.L. Yeung and C.M. Chan, “Hydrogen and proton transport properties of nanoporous zeolite micromembranes,” in Z. Tang and P. Sheng (Eds), Nano Science and Technology: Novel Structure and Phenomena, Taylor and Francis, London, 2003, pp228-232.
11. J.L.H. Chau, A.Y.L. Leung and K.L. Yeung, Zeolite micromembranes,
Lab-on-a-Chip 3 (2003) 53-55. PDF file
12. S. Heng, P.S. Lau, K.L. Yeung, M. Djafer and J.-C. Schrotter,
"Low-temperature ozone treatment for organic template removal from zeolite membrane," J. Membr. Sci., 243 (2004) 69-78. PDF file
13. X.F. Zhang and K.L. Yeung, “Influence of seed size on the growth and microstructure of NaA membrane,” J. Microporous and Mesoporous Mater. (in review).
14. X.F. Zhang, S.M. Lai, R. Martin-Aranda and K.L. Yeung, " An investigation of knoevenagel condensation reaction in microreactors using new zeolite catalysts," Appl. Catal. A, (in review).
15. P.S. Lau, L.T.Y. Au and K.L. Yeung, "Influence of support material on MFI zeolite membrane permeation properties: ZSM-5/a-Al2O3 and ZSM-5/g-Al2O3," J. Membr. Sci., (in review).
16. P.S. Lau and K.L. Yeung, "Effects of cations on the permeation and separation properties of ZSM-5 membrane," J. Membr. Sci., (in review).
Conferences and Invited Talks:
1. L.H. Chau, W.C. Wong and K.L. Yeung, "Zeolite membranes with engineered structure and tailored chemistry," 1998 Catalysis and Zeolite Workshop, Hsinchu, Taiwan, ROC, July 28, 1998.
2. W.C. Wong, L.H. Chau and K.L. Yeung, "New synthesis method for thin supported zeolite membranes: Membrane orientations and nonuniform distribution of framework ions," 5th International Conference on Inorganic Membranes at Nagoya, Japan, June 22-26, 1998.
3. K. L. Yeung, "Inorganic Membranes: State of the Art and Future Developments," Invited Lecture at the Mitsubishi Chemical Corp., Mizushima Plant, Okayama, Kurashiki, Japan, July 3, 1998.
4. K. L. Yeung, "Zeolite Membranes with Engineered Structure and Tailored Chemistry," Invited Lecture at 1998 Catalysis and Zeolite Workshop, Hsinchu, Taiwan, ROC, July 28, 1998.
5. K. L. Yeung, "Inorganic Membranes: Synthesis, Characterization and Application," Invited Lecture at the Department of Chemistry, National Tsinghua University, Hsinchu, Taiwan, ROC, July 29, 1998.
6. L.H. Chau, W.C. Wong and K.L. Yeung, "Synthesis of MFI-type zeolite membranes with nonuniform distribution of Al and Ti framework ions," 15th International Symposium on Chemical Reaction Engineering (ISCRE-15) at Newport Beach, CA, USA, September 13-16, 1998.
7. K. L. Yeung, "Membrane Materials with Engineered Structure and Tailored Chemistry," Invited Lecture at the Department of Chemical Engineering, University of Colorado at Boulder, Boulder, CO, USA, September 17, 1998.
8. K. L. Yeung, "New Synthesis Strategy for Engineered Zeolite Membranes," Invited Lecture at the Exxon Research and Engineering Co., Clinton, NJ, USA, September 22, 1998.
9. W.C. Wong, L.H. Chau and K.L. Yeung, "Zeolite membranes with engineered structure and tailored chemistry," 1998 Regional Symposium on Chemical Engineering at Manila, Philippines, October 14-16, 1998.
10. K. L. Yeung, "Zeolite Membranes with Engineered Structure and Tailored Chemistry," Invited Lecture at the University College, London, United Kingdom, January 5, 1999.
11. K. L. Yeung, "Structural and Chemical Designs of Engineered Membranes," Invited Lecture at the Institute of Catalysis and Petrochemistry, Madrid, Spain, January 12, 1999.
12. K. L. Yeung, "Engineered Zeolite Membranes," Invited Lecture at Exxon Chemical Europe Inc., Machelen, Belgium, January 13, 1999.
13. J.L.H. Chau, C. Tellez, K.L. Yeung, N.K. Ho and P.L. Wong, "The Role of Surface Chemistry on Zeolite Membrane Formation," The 8th Asia Chemical Congress at Taipei, Taiwan, November 21-24, 1999.
14. L.T.Y., Au, J.L.H. Chau, C. Tellez and K.L. Yeung, "Aluminum, Titanium and Vanadium Silicalite-1 Membranes Preparation, Characterization and Permeation Measurements," The 8th Asia Chemical Congress at Taipei, Taiwan, November 21-24, 1999.
15. L.T.Y. Au, W.C. Wong and K.L. Yeung, "Growth Behavior and Permeation Properties of Silicalite-1 Membranes on Seeded Porous Support," North American Membrane Society 2000: 11th Annual Conference at Boulder, Colorado, U.S.A., May 23-27, 2000.
16. L.T.Y. Au and K.L. Yeung, "Effects of Al content on the permeation properties of ZSM-5 membranes," Sixth International Conference on Inorganic Membranes at Montpellier, France, June 26-30, 2000.
17. W.C. Wong, L.T.Y. Au and K.L. Yeung, "Growth behavior and permeation properties of Si-rich MFI membranes on seeded porous support," Sixth International Conference on Inorganic Membranes at Montpellier, France, June 26-30, 2000.
18. J.L.H. Chau, C. Tellez, K.L. Yeung and N.K. Ho, "The role of surface chemistry on the formation of supported Sil-1 membrane," Sixth International Conference on Inorganic Membranes at Montpellier, France, June 26-30, 2000.
19. W.C. Wong, L.T.Y. Au, M.A. Banares, E. Sastre, J.L. Fierro and K.L. Yeung, "Preparation, characterization and reaction performances of engineered zeolite membranes with tailored chemistry," 4th International Conference on Catalysis in Membrane Reactors at Zaragoza, Spain, July 3-5, 2000.
20. P.S. Lau and K. L. Yeung, "Influence of concentration and spatial distribution of framework ions on the permeation properties of ZSM-5 membranes, "Seventh International Conference on Inorganic Membranes at Dalian, China, June 23-26, 2002.
21. X.F. Zhang and K.L. Yeung, “Preparation and characterization of NaA zeolite membranes, ”Seventh International Conference on Inorganic Membranes at Dalian, China, June 23-26, 2002.
22. X.F. Zhang, B.M. Li, J.Q. Wang, H. Liu and K.L. Yeung, “Factors affecting the synthesis of ZSM-5 and Fe-ZSM-5 membranes, ”Seventh International Conference on Inorganic Membranes at Dalian, China, June 23-26, 2002.
23. K.F. Lam, S.M. Lai and K.L. Yeung, "Biological applications of structural and chemical micropatterns based on zeolite materials," AIChE 2003 at San Francisco, USA, November 16-21, 2003.
24. A.Y.L. Leung and K.L. Yeung, "Microfabricated zeoite micromembranes," IZC-14 at Cape Town, South Africa, April 25-30, 2004.
25. A.Y.L. Leung, K.L. Yeung and M.B. Shing, "Properties of free standing ZSM-5 micromembrane with different Si/Al ratio," ICIM-8 at Cincinnati, Ohio, USA, July 18-22, 2004.
26. K.F. Lam and K.L. Yeung, "Fabrication of miniature zeolite membrane microstructure for chemical storage and delivery," ICIM-8 at Cincinnati, Ohio, USA, July 18-22, 2004.
27. P.S. Lau, and K.L. Yeung, "Low temperature activation of MFI zeolite membrane as a tool for membrane characterization," ICIM-8 at Cincinnati, Ohio, USA, July 18-22, 2004.
