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Quantum chemistry as a tool to assess energetic and spectroscopic properties of C1 and C2 hydrocarbons in MOF-74-Mg

Theoretical Chemistry Accounts volume 137, Article number: 42 (2018) Cite this article

Abstract

Periodic boundary conditions as implemented within a linear combination of atomic orbital approach are applied to determine the infrared spectra of methane, acetylene, ethylene, and ethane in MOF-74-Mg. Intensities and frequency shifts with respect to the molecules in the gas phase are described and discussed with respect to geometrical arrangements and structural modifications of the molecules adsorbed in the framework. Given the predictive nature of the work and in the attempt of providing a better ground for comparison with experimental spectroscopic observations, different molecular loadings are considered where one (low loading), three (medium loading), and six (full loading) molecules are adsorbed at the primary adsorption binding site identified by the MgO5 inorganic brick of the MOF structure. In addition, enthalpies of adsorption are reported for methane and acetylene whose addition to previous works by the same authors, provides an overall assessment at electronic structure level of the energetic behavior of C1–C4 hydrocarbons in MOF-74-Mg. Calculations are conducted at B3LYP-D2* level of theory as implemented in the Crystal14 program.

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Acknowledgements

LV thanks Prof. Roberto Dovesi for the opportunity of contributing to this TCA issue in memory of Dr. Claudio Zicovich-Wilson. Claudio will be always remembered not only for his contribution to the scientific community but, and foremost, for his kindness, humbleness, sharpness, and sense of humor. The authors acknowledge the Department of Chemistry and Michigan Technological University for support, and startup allocation. Results reported in this work were obtained through the use of superior, a high-performance computing cluster at Michigan Technological University. The contents of this paper reflect the views and opinions of the authors, who are solely responsible for the accuracy of the data reported herein.

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  1. Department of Chemistry, Michigan Technological University, Houghton, MI, 49931, USA

    Gemechis D. Degaga & Loredana Valenzano

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  1. Gemechis D. Degaga
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  2. Loredana Valenzano
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Correspondence to Loredana Valenzano.

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Published as part of the special collection of articles “In Memoriam of Claudio Zicovich.”

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Degaga, G.D., Valenzano, L. Quantum chemistry as a tool to assess energetic and spectroscopic properties of C1 and C2 hydrocarbons in MOF-74-Mg. Theor Chem Acc 137, 42 (2018). https://doi.org/10.1007/s00214-018-2227-y

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  • DOI: https://doi.org/10.1007/s00214-018-2227-y

Keywords

  • MOF
  • PBC
  • Light hydrocarbons
  • Separation
  • Heats of adsorption
  • IR spectra
  • Long-range forces
  • DFT

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