Abstract
The synthesis of Na-Fe-Silicalite-1(80), Na-Fe-Silicalite-1(128), Na-Fe-ZSM-5(78) and Na-Fe-ZSM-5(126) was conducted using the isomorphic substitution method. These catalysts were further modified by the process of silanisation to yield Na-Fe-Silicalite-1(80:Sil), Na-Fe-Silicalite-1(128:Sil), Na-Fe-ZSM-5(78:Sil), and Na-Fe-ZSM-5(126:Sil) (The numbers in brackets represent the Si/Fe molar ratio and Sil represents silanization). The XRD analyses show that only the ZSM-5 phase was present in all the catalysts. These catalysts were tested in the oxidation of n-octane in MeCN using H2O2 as an oxidant. It was found that the selectivity to terminal products increased with increasing the volume of MeCN. Thus, e.g. terminal C8 selectivities could be improved from 17 to 28% using the Na-Fe-Silicalite-1(80) catalyst by increasing the volume of solvent. Furthermore, the Na-Fe-Silicalite-1(80), Na-Fe-Silicalite-1(80:Sil), Na-Fe-Silicalite-1(128) and Na-Fe-Silicalite-1(128:Sil) show terminal selectivities of 28.1, 14.3, 17.6 and 12.3% respectively. In contrast Na-Fe-ZSM-5(78), Na-Fe-ZSM-5(126), Na-Fe-ZSM-5(78:Sil), and Na-Fe-ZSM-5(126:Sil) show terminal selectivities of 24.5, 25.7, 21.3 and 27.3% respectively. Results also showed that the Na-Fe-ZSM-5 catalyst has better selectivity to terminal products than Na-Fe-Silicalite-1.
Similar content being viewed by others
References
G. Prieto, P. Concepción, A. Martínez, E. Mendoza, J. Catal. 280, 274–288 (2011)
B. Pillay, M.R. Mathebula, H.B. Friedrich, Appl. Catal. A 361, 57–64 (2009)
L. Meng, X. Zhu, W. Wannapakdee, R. Pestman, M. Goesten, L. Gao, A. van Hoof, E. Hensen, J. Catal. 361, 135–142 (2018)
O. Myaa, M. Bitaa, I. Louafia, A. Djouadib, MethodsX 5, 277–282 (2018)
T. Ban, S. Kondoh, Y. Ohya, Y. Takahashi, Phys. Chem. Chem. Phys. 1, 5745–5752 (1999)
F. Bauer, W.H. Chen, E. Bilz, A. Freyer, V. Sauerland, S.B. Liu, J. Catal. 251, 258–270 (2007)
C.T. O’Connor, K.P. Möller, H. Manstein, CATTECH 5, 172–182 (2001)
Y.S. Bhat, J. Das, K.V. Rao, A.B. Halgeri, J. Catal. 159, 368–374 (1996)
J.H. Kim, A. Ishida, M. Okajima, M. Niwa, J. Catal. 161, 387–392 (1996)
H.P. Röger, M. Krämer, K.P. Möller, C. T. O’Connor, Micropor. Mesopor. Mater. 21, 607–614 (1998)
Y.S. Bhat, J. Das, A.B. Halgeri, Appl. Catal. A 122, 161–168 (1995)
J. Cejka, N. Filková, B. Wichterlová, G. Eder-Mirth, J.A. Lercher, Zeolites 17, 265–271 (1996)
Z.R. Zhu, Z.K. Xie, Q.L. Chen, D.J. Kong, W. Li, W.M. Yang, C. Li, Micropor. Mesopor. Mater. 101, 169–175 (2007)
T. Hui, W. Jun, R. Xiaoqian, C.H. Demin. Kinetics and reactors. Chin. J. Chem. Eng. 19, 292–298 (2011)
V. Peneau, G. Shaw, R.D. Armstrong, R.L. Jenkins, N. Dimitratos, S.H. Taylor, H.W. Zanthoff, S. Peitz, G. Stochniol, G.J. Hutchings, Catal. Sci. Technol 6, 7521–7531 (2016)
J. Xu, R.D. Armstrong, G. Shaw, N.F. Dummer, S.J. Freakley, S.H. Taylor, G.J. Hutchings, Catal. Today 270, 93–100 (2016)
M.N. Cele, H.B. Friedrich, M.D. Bala, Catal. Commun. 57, 99–102 (2014)
M.N. Cele, H.B. Friedrich, M.D. Bala, J Mol. Catal. 427, 39–44 (2017)
F. Bauer, C.W. Chen, H. Ernst, S.J. Huang, A. Freyer, S.B. Liu, Micropor. Mesopor. Mater. 72, 81–89 (2004)
P. Fejes, I. Kiricsi, K. Lazar, I. Marsi, A. Rockenbauer, L. Korecz, J.B. Nagy, R. Aiello, F. Testa, Appl. Catal. A 242, 247–266 (2003)
P. Fejes, J.B. Nagy, J. Halasz, A. Oszko, Appl. Catal. A 175, 89–104 (1998)
V.D. Gaag, ZSM-5 Type Zeolites: Synthesis and Use in Gas Phase Reaction with Ammonia (Technische Universiteit, Delft, 1987)
B. Michalkiewicz, Appl. Catal. A 277, 147–153 (2004)
R.Q. Long, R.T. Yang, J. Mol. Catal. 194, 80–90 (2000)
A.S. Axon, J. Klinowski, Appl. Catal. A 81, 27–34 (1992)
Acknowledgements
We thank c*change (Grant No. PAR06.2), the NRF, THRIP (Grant No. TP1208035643), Clariant and the University of KwaZulu-Natal for support.
Author information
Authors and Affiliations
Corresponding author
Additional information
Publisher’s Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Electronic supplementary material
Below is the link to the electronic supplementary material.
Rights and permissions
About this article
Cite this article
Cele, M.N., Friedrich, H.B. & Bala, M.D. Evaluation of silanization of Fe-silicalite-1, Na-Fe-ZSM-5 and solvent concentration on the oxidation of n-octane to C8 oxygenates. J Porous Mater 26, 1447–1454 (2019). https://doi.org/10.1007/s10934-019-00731-z
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10934-019-00731-z