 |
 |
 |
 |
 |
 |
Sains
Malaysiana 49(1)(2020): 75-84
http://dx.doi.org/10.17576/jsm-2020-4901-09
Effect of Crystallinity of Zeolite
Beta on Physicochemical Properties and Performance of Cobalt Catalysts
(Kesan Habluran Beta Zeolit pada Sifat Fisikokimia dan Prestasi Pemangkin
Kobalt)
PIAW PHATAI1, SIRINUCH LOIHA2, SANCHAI PRAYOONPOKARACH3 & JATUPORN WITTAYAKUN3*
1Department of Chemistry, Faculty of Science, Udon
Thani Rajabhat University, Udon Thani 41000, Thailand
2Department of Chemistry, Faculty of Science,
Khon Kaen University, Khon Kaen 40002, Thailand
3School of Chemistry, Institute of Science,
Suranaree University of Technology, Nakhon Ratchasima 30000, Thailand
Diserahkan:
6 September 2019/Diterima: 10 Oktober 2019
ABSTRACT
In the present work, the effect of crystallinity of zeolite beta in a
sodium form (NaBEA) on physicochemical properties and performance of NaBEA-supported cobalt catalysts
was investigated. The incipient wetness impregnation method was utilized in
the synthesis of NaBEA-supported cobalt catalysts with various Co loadings (4, 7 and 10 wt. %). NaBEA materials with
high and low crystallinities (NaBEA-H and NaBEA-L) were synthesized using fumed silica with aging times of 72
and 48 h, respectively. In comparison to NaBEA-L, higher XRD peak intensities and surface area were observed
for NaBEA-H. After impregnation, NaBEA-L displayed better dispersion of Co species and lower reducibility
than NaBEA-H due to stronger metal-support interaction. Catalytic performance for n-butane hydrogenolysis via Co/NaBEA-H and Co/NaBEA-L catalysts was compared. In butane hydrogenolysis, the higher conversion was attained
using Co/NaBEA-H with 7 and 10 wt. % when compared to Co/NaBEA-L with similar loadings. Multiple hydrogenolysis occurred on all catalysts producing
methane as the only product. The most effective catalyst was determined to be 7Co/NaBEA-H due to the higher
surface area and uniform particles of the cobalt species.
Keywords: Butane hydrogenolysis; cobalt; crystallinity; metal dispersion; zeolite
beta
ABSTRAK
Dalam kertas ini, kesan habluran beta zeolit dalam bentuk natrium (NaBEA) pada sifat
fisikokimia dan prestasi pemangkin kobalt disokong-NaBEA dikaji. Kaedah impregnasi
basah peringkat awal telah digunakan dalam sintesis pemangkin kobalt
disokong-NaBEA dengan pelbagai pembebanan Co (4, 7 dan 10 % bt.). Bahan NaBEA dengan habluran tinggi dan
rendah (NaBEA-H dan NaBEA-L) telah disintesis menggunakan silika wasap dengan perumuran masa 72 dan
48 jam. Berbanding NaBEA-L, puncak keamatan XRD yang tinggi dan luas permukaan
diperhatikan untuk NaBEA-H. Selepas impregnasi, NaBEA-L menunjukkan serakan spesies Co yang lebih baik dan
pengurangan yang rendah daripada NaBEA-H disebabkan oleh interaksi sokongan logam yang kuat. Prestasi pemangkinan
untuk hidrogenolisis n-butana melalui pemangkin Co/NaBEA-H dan Co/NaBEA-L telah dibandingkan. Dalam hidrogenolisis butana, penukaran tinggi telah dicapai
menggunakan 7 and 10 % bt. Co/NaBEA-H jika dibandingkan dengan Co/NaBEA-L untuk pembebanan yang sama. Pelbagai hidrogenolisis berlaku kepada semua pemangkin yang
mengeluarkan metana. Pemangkin yang paling berkesan adalah 7Co/NaBEA-H disebabkan luas permukaan yang tinggi serta zarah seragam
spesies kobalt.
Kata kunci: Beta zeolit; butana hidrogenolisis; kobalt; habluran; serakan logam
RUJUKAN
Adebajo, M.O. & Frost, R.L. 2005. Oxidative benzene methylation with methane over MCM-41 and zeolite catalysts: Effect of framework aluminum, SiO2/Al2O3 ratio, and
zeolite pore structure. Energy Fuel 19(3): 783-790.
Altwasser, S.,
Welker, C., Traa, Y. & Weitkamp, J. 2005. Catalytic
cracking of n-octane on small-pore zeolites. Microporous and Mesoporous Materials 83(1-3): 345-356.
Baerlocher, C. & McCusker, L.B. 2017. Database of Zeolite Structures. http://www.iza-structure.org/databases/.
Bayati, B.,
Babaluo, A.A. & Karimi, R. 2008. Hydrothermal
synthesis of nanostructure NaA zeolite: The
effect of synthesis parameters on zeolite seed size and crystallinity. Journal of the European Ceramic Society 28(14): 2653-2657.
Bazin, D., Kovács, I.,
Guczi, L., Parent, P.,
Laffon, C., De Groot, F., Ducreux, O. & Lynch J. 2000. Genesis of Co/SiO2 catalysts: XAS study at
the cobalt LIII, II absorption edges. Journal
of Catalysis 189(2): 456-462.
Bressel, A., Donauer, T., Sealy, S. & Traa, Y. 2008. Influence of
aluminum content, crystallinity and crystallite size of zeolite Pd/H-ZSM-5 on the catalytic performance in the
dehydroalkylation of toluene with ethane. Microporous and
Mesoporous Materials 109(1-3): 278-286.
Byrappa, K. & Yoshimura, M. 2001. Handbook
of Hydrothermal Technology-A Technology
for Crystal Growth and Materials Processing. Norwich: William Andrew Publishing.
Camblor, M.A., Corma, A. & Valencia, S. 1998. Characterization of nanocrystalline zeolite Beta. Microporous and
Mesoporous Materials 25(1-3): 59-74.
Čejka, J.,
Kotrla, J. &
Krejči, A. 2004. Disproportionation of trimethyl
benzenes over large pore zeolites: Catalytic
and adsorption study. Applied
Catalysis A: General 277(1-2): 191-199.
Chansiriwat, W.,
Tanangteerapong, D. & Wantala,
K. 2016. Synthesis of zeolite from coal fly ash by hydrothermal
method without adding alumina and silica sources: Effect of aging temperature and time. Sains Malaysiana 45(11): 1723-1731.
Chan, T.K. & Smith, K.J. 1990. Oxidative coupling of methane over cobalt-magnesium and manganese-magnesium mixed oxide catalysts. Applied Catalysis 60(1): 13-31.
Chao, K.J., Lin, C.C., Lin, C.H., Wu, H.C., Tseng, C.W. & Chen, S.H. 2000. n-Heptane
hydroconversion on platinum-loaded
mordenite and beta zeolites: The
effect of reaction pressure. Applied
Catalysis A: General 203(2): 211-220.
Chen, H.H., Shen, S.C., Chen, X.C. & Kawi, S. 2004. Selective
catalytic reduction of NO over Co/beta-zeolite: Effects of synthesis condition of beta-zeolites,
Co precursor, Co loading method and reductant. Applied Catalysis B: Environmental 50(1): 37-47.
Chu, W.,
Chernavskii, P.A., Gengembre, L.,
Pankina, G.A., Fongerland, P. & Khodakov, A.Y. 2007. Cobalt species in promoted cobalt alumina-supported Fischer-Tropsch
catalysts. Journal of
Catalysis 252(2): 215-230.
Davis, B.H. & Occelli, M.L. 2016. Chapter 8: Fischer-Tropsch
synthesis: Effect of CO
conversion on product selectivities during deactivation or by changing space
velocity at stable conditions over unpromoted and Ru-promoted
25%Co/Al2O3 catalysts. In Fischer-Tropsch Synthesis, Catalysts, and
Catalysis: Advances and
Applications. 1st edition. Boca Raton: CRC Press. pp. 134-140.
Espinosa, G., Domínguez, J.M., Morales-Pacheco, P., Tobon, A., Aguilar, M. & Benítez, J. 2011. Catalytic
behavior of Co/(Nanoβ-Zeolite) bifunctional catalysts for Fischer-Tropsch reactions. Catalysis Today 166(1): 47-52.
Girardon, J.S., Quinet, E.,
Griboval-Constant, A.,
Chernavskii, P.A., Gengembre, L. & Khodakov, A.Y. 2007. Cobalt dispersion, reducibility, and surface sites in
promoted silica-supported
Fischer–Tropsch catalysts. Journal of Catalysis 248(2): 143-157.
Guczi, L. & Kiricsi, I. 1999. Zeolite supported mono- and bimetallic systems: Structure and performance as CO
hydrogenation catalysts. Applied
Catalysis A: General 186(1-2): 375-394.
Guo, W.,
Xiong, C., Huang, L. & Li, Q. 2001. Synthesis and characterization of
composite molecular sieves comprising zeolite Beta with MCM-41 structures. Journal of Materials Chemistry 11(7): 1886-1890.
Hong, J.,
Chernavskii, P.A., Khodakov, A.Y. & Chu, W. 2009. Effect of
promotion with ruthenium on the structure and catalytic performance of
mesoporous silica (smaller and
larger pore) supported
cobalt Fischer-Tropsch
catalysts. Catalysis Today 140(3-4): 135-141.
Jabloński,
J.M., Okal, J., Potoczna-Petru, D. & Krajczyk, L. 2003. High temperature reduction with hydrogen, phase
composition, and activity of cobalt/silica catalysts. Journal of
Catalysis 220(1): 146-160.
Jacobs, G.,
Ji, Y., Davis,
B.H.,
Cronauer, D., Kropf, A.J. &
Marshall, C.L. 2007. Fischer-Tropsch
synthesis: Temperature
programmed EXAFS/XANES
investigation of the influence of support type, cobalt loading, and noble metal
promoter addition to the reduction behavior of cobalt oxide particles. Applied Catalysis A: General 333(2): 177-191.
Jansen, J.C., Creyghton, E.J., Njo, S.L., van Koningveld, H. & van Bekkum, H. 1997. On the remarkable behavior of zeolite Beta in acid catalysis. Catalysis Today 38(2): 205-212.
Karami, D. & Rohani, S. 2009. Synthesis of pure zeolite Y using
soluble silicate, a two-level factorial
experimental design. Chemical
Engineering and Processing: Process
Intensification 48(8): 1288-1292.
Khemthong, P.,
Klysubun, W.,
Prayoonpolarach, S., Roessner, F. & Wittayakun, J. 2010a. Comparison between cobalt and cobalt-platinum
supported on zeolite NaY: Cobalt
reducibility and their catalytic performance for butane hydrogenolysis. Journal of Industrial and Engineering
Chemistry 16(4): 531-538.
Khemthong, P.,
Klysubun, W.,
Prayoonpokarach, S., Roessner, F. & Wittayakun, J. 2010b. Reducibility of cobalt species impregnated on NaY and HY
zeolites. Materials Chemistry and Physics 212(1-2): 131-137.
Khodakov, A.Y., Lynch, J.,
Bazin, D., Rebours, B.,
Zanier, N., Moisson, B. & Chaumette, P. 1997. Reducibility of
cobalt species in silica-supported
Fischer-Tropsch catalysts. Journal of Catalysis 168(1): 16-25.
Loiha, S.,
Prayoonpokatach, S.,
Songsiriritthigun, P. &
Wittayakun, J. 2009. Synthesis of zeolite beta with
pretreated rice husk silica and its transformation to ZSM-12. Materials Chemistry and Physics 115(2-3): 637-640.
Lomot, D.,
Juszczyk, W., Karpinski, Z. & Larsson, R. 2002. Hydrogenolysis of ethane on silica-supported cobalt
catalysts. Journal of
Molecular Catalysis A: Chemical 186(1-2): 163-172.
Nicolaides, C.P. 1999. A novel family of solid acid catalysts: Substantially amorphous or partially crystalline zeolitic
materials. Applied
Catalysis A: General 185(2): 211-217.
Petitto, S.C., Marsh, E.M., Carson, G.A. & Langell, M.A. 2008. Cobalt oxide surface chemistry: The interaction of CoO(100),
Co3O4(110) and Co3O4(111) with oxygen and water. Journal of Molecular Catalysis A: Chemical 281(1-3): 49-58.
Storck, S.,
Bretinger, H. & Maier, W.F. 1998. Characterization of micro- and mesoporous solids by physisorption
methods and pore-size analysis. Applied Catalysis A: General 174(1-2): 137-146.
Tompkins, H.G. & Augis, J.A. 1981. The oxidation of cobalt in air from room temperature to
467°C. Oxidation of Metals 16(5-6): 355-369.
Wang, W.J. & Chen, Y.W. 1991. Influence of metal loading on the reducibility and
hydrogenation activity of cobalt/alumina
catalysts. Applied
Catalysis 77(2): 223-233.
|
|||
|
