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Research output: Contribution to Journal/Magazine › Journal article › peer-review
Research output: Contribution to Journal/Magazine › Journal article › peer-review
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TY - JOUR
T1 - Computational study of H 2 binding to MH 3 (M = Ti, V, or Cr)
AU - Hales, J.J.
AU - Trudeau, M.L.
AU - Antonelli, D.M.
AU - Kaltsoyannis, N.
N1 - © The Royal Society of Chemistry 2019
PY - 2019/4/21
Y1 - 2019/4/21
N2 - 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.
AB - 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.
U2 - 10.1039/c9dt00025a
DO - 10.1039/c9dt00025a
M3 - Journal article
VL - 48
SP - 4921
EP - 4930
JO - Dalton Transactions
JF - Dalton Transactions
SN - 1477-9226
IS - 15
ER -