Impact of Zeolite Structure on Entropic-Enthalpic Contributions to Alkane Monomolecular Cracking: An IR Operando Study.

作者: Shashikant A. Kadam , Haoguang Li , Richard F. Wormsbecher , Arnaud Travert

DOI: 10.1002/CHEM.201800793

关键词:

摘要: The monomolecular cracking rates of propane and n-butane over MFI, CHA, FER TON zeolites were determined simultaneously with the coverage active sites at reaction condition using IR operando spectroscopy. This allowed direct determination adsorption thermodynamics intrinsic rate parameters. results show that zeolite confinement mediates enthalpy-entropy trade-offs only adsorbed state, leaving true activation energy insensitive to or alkane structure while entropy was found increase confinement. Hence, relative alkanes within pores are mostly governed by entropy.

参考文章(33)
S.M. Babitz, B.A. Williams, J.T. Miller, R.Q. Snurr, W.O. Haag, H.H Kung, Monomolecular cracking of n-hexane on Y, MOR, and ZSM-5 zeolites Applied Catalysis A-general. ,vol. 179, pp. 71- 86 ,(1999) , 10.1016/S0926-860X(98)00301-9
Thomas Steiner, Gautam R. Desiraju, Distinction between the weak hydrogen bond and the van der Waals interaction Chemical Communications. pp. 891- 892 ,(1998) , 10.1039/A708099I
Aditya Bhan, Enrique Iglesia, A link between reactivity and local structure in acid catalysis on zeolites. Accounts of Chemical Research. ,vol. 41, pp. 559- 567 ,(2008) , 10.1021/AR700181T
W. Vermeiren, J.-P. Gilson, Impact of Zeolites on the Petroleum and Petrochemical Industry Topics in Catalysis. ,vol. 52, pp. 1131- 1161 ,(2009) , 10.1007/S11244-009-9271-8
S. Kotrel, M. P. Rosynek, J. H. Lunsford, Intrinsic Catalytic Cracking Activity of Hexane over H−ZSM-5, H−β and H−Y Zeolites Journal of Physical Chemistry B. ,vol. 103, pp. 818- 824 ,(1999) , 10.1021/JP982538L
C RAMACHANDRAN, B WILLIAMS, J VANBOKHOVEN, J MILLER, Observation of a compensation relation for n-hexane adsorption in zeolites with different structures: implications for catalytic activity Journal of Catalysis. ,vol. 233, pp. 100- 108 ,(2005) , 10.1016/J.JCAT.2005.04.017
M. Stockenhuber, J. A. Lercher, F. Eder, Bronsted acid and pore controlled siting of alkanes sorption in acidic molecular sieves The Journal of Physical Chemistry. ,vol. 101, pp. 5414- 5419 ,(1997) , 10.1021/JP9706487