Display options
Cite
Zimmerman PM, Head-Gordon M, Bell AT. Selection and Validation of Charge and Lennard-Jones Parameters for QM/MM Simulations of Hydrocarbon Interactions with Zeolites. J Chem Theory Comput. 2011;7(6):1695-703doi: 10.1021/ct2001655.
Zimmerman, P. M., Head-Gordon, M., & Bell, A. T. (2011). Selection and Validation of Charge and Lennard-Jones Parameters for QM/MM Simulations of Hydrocarbon Interactions with Zeolites. Journal of chemical theory and computation, 7(6), 1695-703. https://doi.org/10.1021/ct2001655
Zimmerman, Paul M, et al. "Selection and Validation of Charge and Lennard-Jones Parameters for QM/MM Simulations of Hydrocarbon Interactions with Zeolites." Journal of chemical theory and computation vol. 7,6 (2011): 1695-703. doi: https://doi.org/10.1021/ct2001655
Zimmerman PM, Head-Gordon M, Bell AT. Selection and Validation of Charge and Lennard-Jones Parameters for QM/MM Simulations of Hydrocarbon Interactions with Zeolites. J Chem Theory Comput. 2011 Jun 14;7(6):1695-703. doi: 10.1021/ct2001655. Epub 2011 May 20. PMID: 26596433.
Copy Download .nbib Format: NLM
Share it on

J Chem Theory Comput. 2011 Jun 14;7(6):1695-703. doi: 10.1021/ct2001655. Epub 2011 May 20.

Selection and Validation of Charge and Lennard-Jones Parameters for QM/MM Simulations of Hydrocarbon Interactions with Zeolites.

Journal of chemical theory and computation

Paul M Zimmerman, Martin Head-Gordon, Alexis T Bell

Affiliations

  1. Department of Chemistry, University of California, Berkeley , California 94720-1461, United States.
  2. Department of Chemical and Biomolecular Engineering, University of California, Berkeley , California 94720-1462, United States.

PMID: 26596433 DOI: 10.1021/ct2001655

Abstract

Quantum mechanics/molecular mechanics (QM/MM) models are an appealing method for performing zeolite simulations. In QM/MM, a small cluster chosen to encompass the active center is described by QM, while the rest of the zeolite is described by MM. In the present study, we demonstrate that the charges and Lennard-Jones parameters on Si and O must be chosen properly for QM/MM calculations of adsorption energies and activation energies to agree closely with full QM calculations. The selection of parameters for Si and O is based on using the ωB97X-D functional for DFT calculations of the QM region, which is effective in capturing the effects of van der Waals interactions. A comparison of the heats of adsorption for a variety of adsorbates and activation energies for the cracking of propane and butane reveals that energies derived from QM/MM calculation carried out with appropriately selected MM parameters agree to within an rms error of ∼1.5 kcal/mol with QM calculations. To avoid reparametrization for new substrates, Lennard-Jones zeolite parameters are chosen to be compatible with existing CHARMM parameters. Transferability of these parameters is demonstrated by tests utilizing the B3LYP density functional and simulations of MFI and FAU zeolites. Moreover, the computational time for QM/MM calculations is considerably lower than that for QM calculations, and the ratio of computational times decreases rapidly with increasing size of the cluster used to represent the zeolite.

Publication Types