Sains Malaysiana 47(2)(2018): 337-345

http://dx.doi.org/10.17576/jsm-2018-4702-16

 

Nanocrystalline K-F Zeolite from Rice Husk Silica as an Eco-friendly Solid Base Catalyst for the Synthesis of Jasminaldehyde under Microwave Irradiation

(Nanohablur K-F Zeolit daripada Silika Sekam Padi sebagai Mangkin Bes Pepejal  Mesra Alam untuk Sintesis Jasminaldehid di bawah Sinaran Gelombang Mikro)

 

SIEW-FAN WONG1, KRITTANUN DEEKAMWONG2, JATUPORN WITTAKAYUN2*, TAU CHUAN LING3, OKI MUZARA4, HOOI LING LEE1, FAROOK ADAM1, ENG-POH NG1*

 

1School of Chemical Sciences, Universiti Sains Malaysia, 11800 USM, Pulau Pinang, Malaysia

2School of Chemistry, Institute of Science, Suranaree University of Technology, Nakhon Ratchasima, 30000, Thailand

3Institute of Biological Sciences, Faculty of Science, University of Malaya, 50603 Kuala Lumpur, Federal Territory, Malaysia

4Center of Research Excellence in Nanotechnology and Chemical Engineering Department, King Fahd University of Petroleum & Minerals, Dhahran 31261, Saudi Arabia

  Diserahkan: 21 April 2017/Diterima: 17 Ogos 2017

 

ABSTRACT

Nanocrystalline aluminosilicate F-type zeolite (K-F, EDI-type structure) was synthesized in an organic template-free system using rice husk ash (RHA) silica source and microwave energy. The morphology, crystallite size, chemical composition, crystallographic and basicity properties of the nanocrystals were studied by using various characterization techniques. The results showed that fully crystalline K-F zeolite (Si/Al ratio = 1.26) with flattened cuboid-like shaped could be obtained within 2 min of crystallization which was considerably very fast. In addition, K-F zeolite nanocrystals was also tested as a solid base catalyst in the microwave-enhanced Aldol condensation reaction of heptanal with benzaldehyde and the six catalytic parameters were studied and optimized. The nanosized K-F zeolite crystals showed good catalytic performance in the studied reaction with 77.1% heptanal conversion and 69.5% jasminaldehyde selectivity under optimum reaction condition. The nanocatalyst was reusable and no significant loss in its catalytic reactivity was observed even after five consecutive reaction cycles.

 

Keywords: Aldol condensation; K-F; nanozeolite; microwave synthesis; organotemplate free

 

ABSTRAK

 

Nanohablur aluminosilikat jenis F zeolite (K-F, jenis struktur EDI) telah disintesis dalam sistem bebas templat organik menggunakan sumber silika sekam padi (RHA) dan tenaga gelombang mikro. Morfologi, saiz hablur, komposisi kimia, sifat hablurgrafi dan sifat dasar nanohablur dikaji dengan menggunakan pelbagai teknik pencirian. Keputusan menunjukkan bahawa zeolit ​​K-F menghablur sepenuhnya (nisbah Si / Al = 1.26) dengan bentuk membentuk kuboid rata diperolehi dalam masa 2 minit penghabluran. Selain itu, nanohablur zeolit K-F juga diuji sebagai pemangkin asas pepejal dalam tindak balas pemeluwapan Aldol yang dipertingkatkan oleh gelombang mikro heptanal dengan benzaldeid dan enam ukuran pemangkin dikaji dan dioptimumkan. Zeolit ​​K-F nanohablur menunjukkan prestasi pemangkin yang baik dalam tindak balas yang dikaji dengan penukaran 77.1% heptanal dan jasminaldehid memilih 69.5% di bawah keadaan tindak balas optimum. Nanopemangkin boleh digunakan semula dan tiada kehilangan ketara dalam tindakbalas pemangkinnya selepas lima kitaran reaksi berturut-turut.

 

Kata kunci: K-F; kodensasi aldol; sintesis gelombang mikro; templat organo bebas; zeolit hablur

 

RUJUKAN

 

Abbaspurrad, A.R. & Moradi, O. 2011. The study of catalytic activities of SiO2-Al2O3 for Aldol condensation. Journal of Applied Chemical Research 16: 28-43.

Arbuznikov, A., Vasilyev, V. & Goursot, A. 1998. Relationships between the structure of a zeolite and its adsorption properties. Surface Science 397: 395-405.

Azizi, S.N. & Yousefpour, M. 2010. Synthesis of zeolite NaA and analcime using rice husk ash as silica source without using organic template. Journal of Materials Science 45: 5692-5697.

Bein, T. & Mintova, S. 2005. Title of Article. In Zeolites and Ordered Mesoporous Materials, Progress and Prospects, edited by Cejka, J. & Van Bekkum, H. Amsterdam: Elsevier.

Bouizi, Y., Diaz, I., Rouleau, L. & Valtchev, V.P. 2005. Core-shell zeolite microcomposites. Advanced Functional Materials 15: 1955-1960.

Byrappa, K. & Kumar, B.V.S. 2007. Characterization of zeolites by infrared spectroscopy. Asian Journal of Chemistry 19: 4933-4935.

Climent, M.J., Corma, A., Garcia, H., Guil-Lopez, R., Iborra, S. & Fornes, V. 2001. Acid-base bifunctional catalysts for the preparation of fine chemicals: Synthesis of jasminaldehyde. Journal of Catalysis 197: 385-393.

Dalai, A.K., Rao, M.S. & Gokhale, K.V.G.K. 1985. Synthesis of NaX zeolite using silica from rice husk ash. Industrial & Engineering Chemistry Product Research and Development 24: 465-468.

Dey, K.P., Ghosh, S. & Naskar, M.K. 2012. A facile synthesis of ZSM-11 zeolite particles using rice husk ash as silica source. Materials Letters 87: 189-196.

Ghasemi, Z. & Younesi, H. 2012. Preparation of free-template nanometer-sized Na-A and –X zeolites from rice husk ash. Waste Biomass Valorization 3: 61-74.

Ghasemi, Z., Younesi, H. & Kazemian, H. 2011. Synthesis of nanozeolite sodalite from rice husk ash without organic additives. The Canadian Journal of Chemical Engineering 89: 601-608.

Hamza, A. & Nagaraju, N. 2015. Amorphous metal-aluminophosphate catalysts for aldol condensation of n-heptanal and benzaldehyde to jasminaldehyde. Chinese Journal of Catalysis 36: 209-215.

Hardie, S.M.L., Garnett, M.H., Fallick, A.E., Rowland, A.P. & Ostle, N.J. 2005. Carbon dioxide capture using a zeolite molecular sieve sampling system for isotopic studies (13C and 14C) of respiration. Radiocarbon 47: 441-451.

Haynes, W.M. 2014. Handbook of Chemistry and Physics. 95th ed. New York: CRC Press.

Jaccula, V.S., Williams, C.D., Hocking, T.J. & Fullen, M.A. 2006. High selectivity and affinity of linde type F towards NH4+ on application as a soil amendment for maize growth. Microporous and Mesoporous Materials 88: 101-104.

Jaroonvechatam, N., Sansuksom, P., Worothanakul, P. & Kongkac, P. 2013. SUZ-4 zeolite synthesis derived from rice husk ash. Chiang Mai Journal of Science 40: 109-116.

Khoo, D.Y.Y., Kok, W.M., Mukti, R.R., Mintova, S. & Ng, E.P. 2013. Ionothermal approach for synthesizing AlPO-5 hexagonal thin plate influenced by various parameters at ambient pressure. Solid State Sciences 25: 63-69.

Kordatos, K., Gavela, S., Ntziouni, A., Pistiolas, K.N., Kyritsi, A. & Kasselouri-Rigopoulou, V. 2008. Synthesis of highly siliceous ZSM-5 zeolite using silica from rice husk ash. Microporous and Mesoporous Materials 115: 189-196.

Majano, G., Ng, E.P., Lakiss, L. & Mintova, S. 2011. Nanosized molecular sieves utilized as an environmentally friendly alternative to antioxidants for lubricant oils. Green Chemistry 13: 2435-2440.

Ng, E.P., Awala, H., Ghoy, J.P., Vincente, A., Ling, T.C., Ng, Y.H. & Mintova, S. 2015a. Effects of ultrasonic irradiation on crystallization and structural properties of EMT-type zeolite nanocrystals. Materials Chemistry and Physics 159: 38-45.

Ng, E.P., Awala, H., Tan, K.H., Adam, F., Retoux, R. & Mintova, S. 2015b. EMT-type zeolite nanocrystals synthesized from rice husk. Microporous and Mesoporous Materials 204: 204-209.

Ng, E.P., Lim, G.K., Khoo, G.L., Tan, K.H., Ooi, B.S., Adam, F. & Wong, K.L. 2015c. Synthesis of colloidal stable linde type J (LTJ) zeolite nanocrystals from rice husk silica and their catalytic performance in knoevenagel reaction. Materials Chemistry and Physics 155: 30-35.

Ng, E.P., Delmotte, L. & Mintova, S. 2009. Selective capture of water using microporous adsorbents to increase the lifetime of lubricants. ChemSusChem 2: 255-260.

Ng, E.P. & Mintova, S. 2011. Quantitative moisture measurements in lubricating oils by FT-IR spectroscopy combined with solvent extraction approach. Microchemical Journal 98: 177-185.

Ng, E.P., Ng, D.T.L., Awala, H., Wong, K.L. & Mintova, S. 2014. Microwave synthesis of colloidal stable AlPO-5 nanocrystals with high hydrophilicity and unique morphology. Materials Letters 132: 126-129.

Novembre, D., Pace, C. & Gimeno, D. 2014. Syntheses and characterization of zeolites K-F and W type using a diatomite precursor. Mineralogical Magazine 78: 1209-1225.

Prasetyoko, D., Ramli, Z., Endud, S., Hamdan, H. & Sulikowski, B. 2006. Conversion of rice husk ash to zeolite beta. Waste Management 26: 1173-1179.

Rahimi, M., Ng, E.P., Bakhtiari, K., Vinciguerra, M., Ahmad, H.A., Awala, H., Mintova, S., Daghighi, M., Rostami, F.B., de Vries, M., Motazacker, M.M., Peppelenbosch, M.P., Mahmoudi, M. & Rezaee, F. 2015. Zeolite nanoparticles for selective sorption of plasma proteins. Scientific Reports 5: 17259.

Shan, W., Yu, T., Wang, B., Hu, J., Zhang, Y., Wang, X. & Tang, Y. 2006. Magnetically separable nanozeolites: Promising candidates for bio-applications. Chemistry of Materials 18: 3169-3172.

Sharma, S.K., Parikh, P.A. & Jasra, R.V. 2008. Eco-friendly synthesis of jasminaldehyde by condensation of 1-heptanal with benzaldehyde using hydrotalcite as a solid base catalyst. Journal of Molecular Catalysis A 286: 55-62.

Sherman, J.D. 1991. Synthesis zeolites and other microporous oxide molecular sieves. Proceedings of the National Academy of Sciences of the United States of America 96: 3471-3478.

Tosheva, L., Ng, E.P., Mintova, S., Hölzl, M., Metzger, T.H. & Doyle, A.M. 2008. AlPO-18 seed layers and films by secondary growth. Chemistry of Materials 20: 5721-5726.

Vrbkova, E., Vyskocilova, E., Krupka, J. & Cerveny, L. 2016. Aldol condensation of benzaldehyde with heptanal using solid-supported caesium and potassium catalysts. Progress in Reaction Kinetics and Mechanism 41: 289-300.

Wang, H.P., Lin, K.S., Huang, Y.J. & Tsaur, L.K. 1998. Synthesis of zeolite ZSM-48 from rice husk ash. Journal of Hazardous Materials 58: 147-152.

Wong, J.T., Ng, E.P. & Adam, F. 2012. Microscopic investigation of nanocrystalline zeolite L synthesized from rice husk ash. Journal of the American Ceramic Society 95: 805-808.

Wong, S.F., Deekomwong, K., Wittayakun, J., Ling, T.C., Muraza, O., Adam, F., Ng, E.P. 2017a. Crystal growth study of KF nanozeolite and its catalytic behavior in Aldol condensation of benzaldehyde and heptanal enhanced by microwave heating. Materials Chemistry and Physics 196: 295-301.

Wong, S.F., Awala, H., Vincente, A., Retoux, R., Ling, T.C., Mintova, S., Mukti, R.R. & Ng, E.P. 2017b. KF zeolite nanocrystals synthesized from organic-template-free precursor mixture. Microporous and Mesoporous Materials 249: 105-110.

Zou, J., Yu, Q. & Shang, Z. 2001. Correlation between empirical solvent polarity scales and computed quantities derived from molecular surface electrostatic potentials. Journal of the Chemical Society, Perkin Transactions 2: 1439-1443.

 

*Pengarang untuk surat-menyurat; email: epng@usm.my

 

 

 

 

sebelumnya