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Dehydrogenation mechanisms of liquid organic hydrogen carriers over Pt, Pd, Rh, and Ni surfaces : Cyclohexane as a model compound

Li, Xinbao LU ; Shen, Pengfei ; Han, Xinyi ; Wang, Yucheng ; Zhu, Yingying and Wu, Zan LU (2021) In Applied Surface Science 543.
Abstract

In order to make a better understanding of dehydrogenation mechanisms of liquid organic hydrogen carriers, cyclohexane was selected as a model compound to carry out its decomposition studies over Pt(1 1 1), Pd(1 1 1), Rh(1 1 1), and Ni(1 1 1) surfaces via periodic density functional theory calculations. The adsorption geometries and adsorption energies of reaction intermediates were presented. Similar linear relationships of the adsorption energies with respect to the number of hydrogen removal over these four surfaces were revealed for C6Hx* (x = 8–12). Seven elementary reactions for cyclohexane successive dehydrogenation to C6H5* were considered. The initial dehydrogenation of... (More)

In order to make a better understanding of dehydrogenation mechanisms of liquid organic hydrogen carriers, cyclohexane was selected as a model compound to carry out its decomposition studies over Pt(1 1 1), Pd(1 1 1), Rh(1 1 1), and Ni(1 1 1) surfaces via periodic density functional theory calculations. The adsorption geometries and adsorption energies of reaction intermediates were presented. Similar linear relationships of the adsorption energies with respect to the number of hydrogen removal over these four surfaces were revealed for C6Hx* (x = 8–12). Seven elementary reactions for cyclohexane successive dehydrogenation to C6H5* were considered. The initial dehydrogenation of C6H12* to generate C6H11* were identified as the rate-determining steps over all surfaces, association with activation energies of 1.04, 1.06, 0.96, and 1.14 eV for Pt(1 1 1), Pd(1 1 1), Rh(1 1 1), and Ni(1 1 1), respectively. The reactivity of dehydrogenation was in the order of Rh(1 1 1) > Pt(1 1 1) > Pd(1 1 1) > Ni(1 1 1).

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author
; ; ; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
Cyclohexane, DFT, Hydrogen, LOHC, Mechanism
in
Applied Surface Science
volume
543
article number
148769
publisher
Elsevier
external identifiers
  • scopus:85098474459
ISSN
0169-4332
DOI
10.1016/j.apsusc.2020.148769
language
English
LU publication?
yes
id
4930d1db-247e-42f2-8f89-4185033f1d90
date added to LUP
2021-01-12 14:18:12
date last changed
2023-11-20 20:09:56
@article{4930d1db-247e-42f2-8f89-4185033f1d90,
  abstract     = {{<p>In order to make a better understanding of dehydrogenation mechanisms of liquid organic hydrogen carriers, cyclohexane was selected as a model compound to carry out its decomposition studies over Pt(1 1 1), Pd(1 1 1), Rh(1 1 1), and Ni(1 1 1) surfaces via periodic density functional theory calculations. The adsorption geometries and adsorption energies of reaction intermediates were presented. Similar linear relationships of the adsorption energies with respect to the number of hydrogen removal over these four surfaces were revealed for C<sub>6</sub>Hx* (x = 8–12). Seven elementary reactions for cyclohexane successive dehydrogenation to C<sub>6</sub>H<sub>5</sub>* were considered. The initial dehydrogenation of C<sub>6</sub>H<sub>12</sub>* to generate C<sub>6</sub>H<sub>11</sub>* were identified as the rate-determining steps over all surfaces, association with activation energies of 1.04, 1.06, 0.96, and 1.14 eV for Pt(1 1 1), Pd(1 1 1), Rh(1 1 1), and Ni(1 1 1), respectively. The reactivity of dehydrogenation was in the order of Rh(1 1 1) &gt; Pt(1 1 1) &gt; Pd(1 1 1) &gt; Ni(1 1 1).</p>}},
  author       = {{Li, Xinbao and Shen, Pengfei and Han, Xinyi and Wang, Yucheng and Zhu, Yingying and Wu, Zan}},
  issn         = {{0169-4332}},
  keywords     = {{Cyclohexane; DFT; Hydrogen; LOHC; Mechanism}},
  language     = {{eng}},
  publisher    = {{Elsevier}},
  series       = {{Applied Surface Science}},
  title        = {{Dehydrogenation mechanisms of liquid organic hydrogen carriers over Pt, Pd, Rh, and Ni surfaces : Cyclohexane as a model compound}},
  url          = {{http://dx.doi.org/10.1016/j.apsusc.2020.148769}},
  doi          = {{10.1016/j.apsusc.2020.148769}},
  volume       = {{543}},
  year         = {{2021}},
}