Computational study of H 2 binding to MH 3 (M = Ti, V, or Cr)

Hales, J.J. and Trudeau, M.L. and Antonelli, D.M. and Kaltsoyannis, N. (2019) Computational study of H 2 binding to MH 3 (M = Ti, V, or Cr). Dalton Transactions, 48 (15). pp. 4921-4930. ISSN 1477-9226

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A series of amorphous materials based on hitherto elusive early transition metal hydrides MH 3 (M = Ti, V, and Cr) and capable of binding H 2 via the Kubas interaction has shown great promise for hydrogen storage applications, approaching US DoE system targets in some cases [Phys. Chem. Chem. Phys., 2015, 17, 9480; Chem. Mat., 2013, 25, 4765; J. Phys. Chem. C, 2016, 120, 11407]. We here apply quantum chemical computational techniques to study models of the H 2 binding sites in these materials. Starting with monomeric MH 3 (M = Ti, V, and Cr) we progress to M 2 H 6 and then pentametallic systems, analyzing the H 2 binding geometries, energies, vibrational frequencies and electronic structure, finding clear evidence of significant Kubas binding. Dihydrogen binding energies range from 22 to 53 kJ mol -1 . In agreement with experiment, we conclude that while TiH 3 binds H 2 exclusively through the Kubas interaction, VH 3 and CrH 3 additionally physisorb dihydrogen, making these more attractive for practical applications.

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Journal Article
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Dalton Transactions
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© The Royal Society of Chemistry 2019
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Deposited On:
15 May 2019 08:05
Last Modified:
28 Sep 2023 23:38