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High Field 33S Solid State NMR and First-Principles Calculations in Potassium Sulfates

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Steacie Institute for Molecular Sciences, National Research Council, 100 Sussex Drive, Ottawa, K1A 0R6, Ontario, Canada
* Corresponding author: Phone: 613-993-5638, Fax: 613-990-1555, E-mail: [email protected]
Cite this: J. Phys. Chem. A 2010, 114, 1, 309–316
Publication Date (Web):October 30, 2009
https://doi.org/10.1021/jp908206c
Copyright © Published 2009 by the American Chemical Society

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    Abstract

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    A set of potassium sulfates presenting a variety of sulfur environments (K2SO4, KHSO4, K2S2O7, and K2S2O8) has been studied by 33S solid state NMR at 21 T. Low natural abundance (0.75%) and small gyromagnetic ratio of 33S presented a serious challenge even at such a high magnetic field. Nevertheless, using the QCPMG technique we were able to obtain good signals from the sites with CQ values approaching 16 MHz. Assignment of the sites and the relative orientations of the EFG tensors were assisted by quantum mechanical calculations using the Gaussian 98 and CASTEP packages. The Gaussian 98 calculations were performed using the density functional method and gauge independent atomic orbitals on molecular clusters of about 100−120 atoms. The CASTEP calculations utilized periodic boundary conditions and a gauge-including projector augmented-wave pseudopotential approach. Although only semiquantitative agreement is observed between the experimental and calculated parameters, the calculations are a very useful aid in the interpretation of experimental data.

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    Correlation between the experimental chemical shifts and calculated absolute shieldings, table of calculated Euler angles, source code of the program used for generation of clusters for G98 calculations, complete G98 input files for all the clusters used in calculations. This information is available free of charge via the Internet at http://pubs.acs.org.

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