BERNA TOPUZ, Aylin ÖNDER SAKA, HALİL KALIPÇILAR

MFI Tipi Zeolit Membranların Yüksek Sıcaklıkta Geri Döngülü Akış Sisteminde Sentezi

Bu çalışmada, MFI tipi zeolit membranlar makro gözenekli destekler üzerinde yüksek sıcaklık ve basınç altında geri döngülü akış sisteminde sentezlenmiş ve MFI tipi zeolit membranların özellikleri üzerine membran sentez sıcaklığının etkisi incelenmiştir. Membranların sentezi 140-160oC aralığında iç tarafı nano boyutta MFI tohum kristalleri ile kaplanmış alümina tüpler üzerinde yapılmıştır. Membranlar ve sentez sırasında eş zamanlı olarak oluşan toz malzemeler X-ışını kırınımı, taramalı elektron mikroskobu, ve tanecik boyut dağılımı ölçümleri ile karakterize edilmiştir. Elde edilen membranlarda n-C4H10/isoC4H10 ile yapılan seçicilik testlerinde ideal seçicilik değerinin 20’ye ulaşması uygulanan sentez tekniğinin yüksek kalitede membran üretimine olanak sağlayacağını göstermektedir.

Synthesis of MFI Membranes through Recirculated Flow at Elevated Temperatures

In this study, MFI type zeolite membranes were synthesised in a recirculating flow system at elevated temperatures. MFI membranes were prepared on the inner surface of the seeded tubular alumina supports in the 140-160oC temperature range. MFI membranes were characterized by scanning electron microscopy, X-ray diffraction and single gas permeation experiments. The best membrane had a n-C4H10 single gas permeance of 3.6x10-8 mol/m2-s-Pa and n-C4H10/iso-C4H10 ideal selectivity of 20 at 25oC. The results showed that it is possible to produce high quality MFI membranes by a recirculating flow system operating at elevated temperature.

PDF

___

Kresge CT, Dhingra S.S. 2004. Molecular Sieves, Kirk Othmer Encyclopedia of Chemical Technology.
Breck D.W. 1974. Zeolite Molecular Sieves: Structure, Chemistry, and Use, New York: Wiley
Szostak R. 1984. Handbook of Molecular Sieves, New York: Van Nostrand Reinhold..
Funke HH, Kovalchick MG, Falconer JL, Noble RD. 1996. Separation of Hydrocarbon Isomer Vapors with Silicalite Zeolite Membranes, Industrial and Engineering Chemistry Research, Cilt 35, s.1575-1582. DOI: 10.1021/ie950495e
Hedlund J, Sterte J, Anthonis M, Bons A, Crastensen B, Corcorand N, Cox D, Deckman H, De Gijnst W, de Moor P, Lai F, McHenry J, Mortier W, Reinoso J, Peters J. 2002. High-flux MFI Membranes, Microporous and Mesoporous Materials, Cilt 52, s.179-189.DOI: 10.1016/S1387-1811(02)003165
Noack M, Kölsch P, Schafer R, Toussiant P, Caro J. 2002. Molecular Sieve Membranes for Industrial Application: Problems, Progress, Solutions, Chemical Engineering and Technology, Cilt 25, No 3, s.221-230.
Coronas J, Santamaria J. 1999. Separations Using Zeolite Membranes, Separation and Purification Methods, Cilt 28, No 2, s.127-177.DOI: 10.1080/03602549909351646
Pina MP, Arruebo M, Felipe M, Fleta F, Bernal MP, Coronas J, Menendez M, Santamaria J. 2004. A Semi-Continuous Method for the Synthesis of NaA Zeolite Membranes on Tubular Supports, Journal of Membrane Science, Cilt 244, s.141-150.DOI: 10.1016/j.memsci.2004.06.049
Aguado S, Gascon J, Jansen JC, Kapteijn F. 2009. Continuous Synthesis of NaA Zeolite Membranes, Microporous and Mesoporous Materials, Cilt 120, s.170-176.DOI: 10.1016/j.micromeso.2008.08.06 2
Çulfaz PZ, Çulfaz A, Kalıpçılar H. 2006. Preparation of MFI Type Zeolite Membranes in a Flow System with Circulation of the Synthesis Solution. Microporous and Mesoporous Materials, Cilt 92, s.134-144. DOI: 10.1016/j.micromeso.2006.01.00 4 [
Pera-Titus M., Mallada R., Llorens J., Cunill Fidel, Santamaria J. 2006. Preparation of Inner-side Tubular NaA Membranes in a Semi-Continuous Synthesis System, Journal of Membrane Science, Cilt 278, No 1–2, s.401-409. DOI: 10.1016/j.memsci.2005.11.026
Richter H, Voight I, Fischer P, Puhlfürβ P. 2003. Preparation of Zeolite Membranes on the Inner Surface of Ceramic Tubes and Capillaries, Separation and Purification Technology, Cilt 32, s.133-138. DOI: 10.1016/S13835866(03)00025-X
Dede Ö. 2007. Pervaporation of Organic/Water Mixture by MFI Type Zeolite Membranes Synthesized in a Flow System, Orta Doğu Teknik Üniversitesi, Fen Bilimleri Enstitüsü, Y. Lisans Tezi, Ankara.
Topuz B., Önder A., Bowen T., Kalıpçılar H., 2017. Synthesis of ZSM-5 and SAPO-34 Membranes in a High Temperature-Pressure Recirculating Flow System, Chemical Engineering Research and Design, Cilt 117, s.746-755. DOI: 10.1016/j.cherd.2016.11.035
Li Y, Zhang X, Wang J, 2001. Preparation for ZSM-5 Membranes by a Two-stage Varying-Temperature Synthesis, Separation and Purification Technology, Cilt 25, s. 459466.DOI: 10.1016/S13835866(01)00075-2
Hedlund J, Noack M, Kölsch P, Creaser D, Caro J, Sterte J. 1999. ZSM-5 Membranes Synthesized without Organic Templates Using A Seeding Technique, Journal of Membrane Science, Cilt 159, s.263-273. DOI: 10.1016/S0376-7388(99)000691
Noack M, Kölsch P, Seefeld V, Toussaint P, Georgi G, Caro J. 2005. Influence of the Si/Al-Ratio on the Permeation Properties of MFI-Membranes, Microporous and Mesoporous Materials, Cilt 79, s.329-337. DOI: 10.1016/j.micromeso.2005.01.00 4
Tuan VA, Falconer JL, Noble RD. 1999. Alkali-Free ZSM-5 Membranes: Preparation Conditions and Separation Performance, Industrial and Engineering Chemistry Research, Cilt 35, s.3635-3646. DOI: 10.1021/ie980808g
Au LTY, Yeung KL. 1999. An Investigation of the Relationship Between Microstructure and Permeation Properties of ZSM-5 Membranes, Journal of Membrane Science, Cilt 194, s.33-55. DOI: 10.1016/S03767388(01)00489-6