Hexane Cracking on ZSM-5 and Faujasite Zeolites: a QM/MM/QCT Study

D. C Tranca; P. M Zimmerman; J Gomes; D Lambrecht; F. J Keil; M Head-Gordon; A. T Bell

doi:10.1021/acs.jpcc.5b07457

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Hexane Cracking on ZSM-5 and Faujasite Zeolites: a QM/MM/QCT Study

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Hexane Cracking on ZSM-5 and Faujasite Zeolites: a QM/MM/QCT Study

D. C Tranca, P. M Zimmerman, J Gomes, D Lambrecht, F. J Keil, M Head-Gordon and A. T Bell

Journal of physical chemistry. C, Vol.119(52), pp.28836-28853

12/31/2015

DOI: 10.1021/acs.jpcc.5b07457

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Abstract

Quantum mechanics/molecular mechanics (QM/MM) models are applied to investigate the adsorption and cracking of n-hexane on ZSM-5 and Faujasite zeolite structures. These simulations account for the long-range electrostatic and midrange van-der-Waals interactions in the zeolite and provide energy barriers that are close to experimental data. The active acidic site was modeled by dispersion corrected density functional theory (DFT, ω B97X-D6-311/G*). The long-range interactions were calculated by molecular mechanics (MM). The adsorbed molecules under investigation are characterized by their thermodynamic properties (adsorption energy and enthalpy). The influence of the zeolite type on the thermodynamic properties is also pointed out. The results reveal that the kinetics of cracking is insensitive to differences in acid strengths. The thermodynamic data obtained are mainly influenced by the adsorption energy of n-hexane on ZSM-5 and/or Faujasite (Y) structures. The pore sizes of the zeolite types can lead to a stronger or weaker adsorption energy. Except for the thermodynamic property investigations in this article, the quasi-classical trajectory method (QCT) is used for investigating the pathways along metastable intermediates toward various cracking products. Not only the reaction barriers but also the reaction dynamics determine the reaction selectivity.

Details

Title: Subtitle: Hexane Cracking on ZSM-5 and Faujasite Zeolites: a QM/MM/QCT Study
Creators: D. C Tranca - Hamburg University of Technology
P. M Zimmerman - University of California, Berkeley
J Gomes - University of California, Berkeley
D Lambrecht - University of California, Berkeley
F. J Keil - Hamburg University of Technology
M Head-Gordon - University of California, Berkeley
A. T Bell - University of California, Berkeley
Resource Type: Journal article
Publication Details: Journal of physical chemistry. C, Vol.119(52), pp.28836-28853
DOI: 10.1021/acs.jpcc.5b07457
NLM abbreviation: J Phys Chem C Nanomater Interfaces
ISSN: 1932-7447
eISSN: 1932-7455
Publisher: American Chemical Society
Language: English
Date published: 12/31/2015
Academic Unit: Chemical and Biochemical Engineering
Record Identifier: 9984197264402771

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