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Structural Characterization of Protonated Water Clusters Confined in HZSM-5 Zeolites

  • John H. Hack
    John H. Hack
    Department of Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, Chicago, Illinois 60637, United States
    More by John H. Hack
  • James P. Dombrowski
    James P. Dombrowski
    Department of Chemical and Biological Engineering, Northwestern University, Evanston, Ilinois 60208−3120, United States
  • Xinyou Ma
    Xinyou Ma
    Department of Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, Chicago, Illinois 60637, United States
    Chicago Center for Theoretical Chemistry, The University of Chicago, Chicago, Illinois 60637, United States
    More by Xinyou Ma
  • Yaxin Chen
    Yaxin Chen
    Department of Chemical and Biological Engineering, Northwestern University, Evanston, Ilinois 60208−3120, United States
    More by Yaxin Chen
  • Nicholas H. C. Lewis
    Nicholas H. C. Lewis
    Department of Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, Chicago, Illinois 60637, United States
  • William B. Carpenter
    William B. Carpenter
    Department of Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, Chicago, Illinois 60637, United States
  • Chenghan Li
    Chenghan Li
    Department of Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, Chicago, Illinois 60637, United States
    Chicago Center for Theoretical Chemistry, The University of Chicago, Chicago, Illinois 60637, United States
    More by Chenghan Li
  • Gregory A. Voth*
    Gregory A. Voth
    Department of Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, Chicago, Illinois 60637, United States
    Chicago Center for Theoretical Chemistry, The University of Chicago, Chicago, Illinois 60637, United States
    *Email for G.A.V.: [email protected]
  • Harold H. Kung*
    Harold H. Kung
    Department of Chemical and Biological Engineering, Northwestern University, Evanston, Ilinois 60208−3120, United States
    *Email for H.H.K.: [email protected]
  • , and 
  • Andrei Tokmakoff*
    Andrei Tokmakoff
    Department of Chemistry, James Franck Institute, and Institute for Biophysical Dynamics, The University of Chicago, Chicago, Illinois 60637, United States
    *Email for A.T.: [email protected]
Cite this: J. Am. Chem. Soc. 2021, 143, 27, 10203–10213
Publication Date (Web):July 1, 2021
https://doi.org/10.1021/jacs.1c03205
Copyright © 2021 American Chemical Society

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    Abstract

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    A molecular description of the structure and behavior of water confined in aluminosilicate zeolite pores is a crucial component for understanding zeolite acid chemistry under hydrous conditions. In this study, we use a combination of ultrafast two-dimensional infrared (2D IR) spectroscopy and ab initio molecular dynamics (AIMD) to study H2O confined in the pores of highly hydrated zeolite HZSM-5 (∼13 and ∼6 equivalents of H2O per Al atom). The 2D IR spectrum reveals correlations between the vibrations of both terminal and H-bonded O–H groups and the continuum absorption of the excess proton. These data are used to characterize the hydrogen-bonding network within the cluster by quantifying single-, double-, and non-hydrogen-bond donor water molecules. These results are found to be in good agreement with the statistics calculated from an AIMD simulation of an H+(H2O)8 cluster in HZSM-5. Furthermore, IR spectral assignments to local O–H environments are validated with DFT calculations on clusters drawn from AIMD simulations. The simulations reveal that the excess charge is detached from the zeolite and resides near the more highly coordinated water molecules in the cluster. When they are taken together, these results unambiguously assign the complex IR spectrum of highly hydrated HZSM-5, providing quantitative information on the molecular environments and hydrogen-bonding topology of protonated water clusters under extreme confinement.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.1c03205.

    • Detailed methods section, zeolite characterization by XRD, SEM, 1H MAS NMR, and FTIR, fitting details for FTIR and 2D IR spectra, and calculated harmonic spectra (PDF)

    • Cartesian coordinates for a calculated structure (XYZ)

    • Cartesian coordinates for a calculated structure (XYZ)

    • Cartesian coordinates for a calculated structure (XYZ)

    • Cartesian coordinates for a calculated structure (XYZ)

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