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Supercell Models of Brønsted and Lewis Sites in Zeolites

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Handbook of Materials Modeling

Abstract

Zeolites are three-dimensional, crystalline silicate-based materials of interest for catalysis and separations. Computational models of zeolites must capture their three-dimensional structure, the intrinsic microscopic heterogeneity introduced by heteroatom substitutions that underlie their interesting chemical behavior, and the dynamic nature of reactive sites within the pores of molecular dimensions. Here we describe the use of supercell density functional theory (DFT) models for tackling these problems, focusing primarily on Brønsted acidic and Cu-exchanged chabazite (CHA) zeolites and their chemistry related to the catalytic chemistry of nitrogen oxides ( NOx). We describe considerations important in model construction, applications of ab initio molecular dynamics to structure annealing and accurate computations of reaction and activation free energies, first-principles thermodynamics approaches for predicting site compositions at realistic conditions, and approaches for incorporating heteroatom distributions into material models.

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Acknowledgements

This work was prepared in part with the financial support of the BASF Corporation. Numerous valuable discussions with C. Paolucci, H. Li, A. DeBellis, and I. Müller are gratefully acknowledged.

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Authors and Affiliations

  1. Department of Chemical and Biomolecular Engineering, University of Notre Dame, Notre Dame, IN, USA

    Sichi Li & William F. Schneider

Authors
  1. Sichi Li
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  2. William F. Schneider
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Correspondence to William F. Schneider .

Editor information

Editors and Affiliations

  1. Institute of Physics, École Polytechnique Fédérale de Lausanne, Lausanne, Switzerland

    Wanda Andreoni

  2. Department of Nuclear Science & Engineering, Massachusetts Institute of Technology, Cambridge, MA, USA

    Sidney Yip

Section Editor information

  1. Department of Chemistry & Biochemistry, University of California at Santa Barbara, Santa Barbara, CA, USA

    Horia Metiu

  2. Theoretische Chemie, Technical University, München, Germany

    Karsten Reuter

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Li, S., Schneider, W.F. (2018). Supercell Models of Brønsted and Lewis Sites in Zeolites. In: Andreoni, W., Yip, S. (eds) Handbook of Materials Modeling. Springer, Cham. https://doi.org/10.1007/978-3-319-50257-1_4-1

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  • DOI: https://doi.org/10.1007/978-3-319-50257-1_4-1

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  • Publisher Name: Springer, Cham

  • Print ISBN: 978-3-319-50257-1

  • Online ISBN: 978-3-319-50257-1

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