Citation: Xue-Feng WANG, Chong-Yu SHEN, Ji-Liang WU, Xiao-Qiu YE. First-Principles Calculation of H/CO₂ Interaction in Plasma: A Density Functional Theory-Based Study[J]. Chinese Journal of Inorganic Chemistry, ;2022, 38(8): 1470-1476. doi: 10.11862/CJIC.2022.158 shu

First-Principles Calculation of H/CO₂ Interaction in Plasma: A Density Functional Theory-Based Study

1.
Science and Technology on Surface Physics and Chemistry Laboratory, Mianyang, Sichuan 621908, China
2.
Institute of Materials, China Academy of Engineering Physics, Mianyang, Sichuan 621900, China

Corresponding author: Xiao-Qiu YE, xiaoqiugood@sina.com
Received Date: 14 December 2021
Revised Date: 23 April 2022

Figures(3)

An in-depth understanding of the microscopic mechanism of the reaction of hydrogen isotopes with CO₂ under irradiation conditions can provide data support for the optimal design of the deuterium-tritium fuel cycle process for fusion reactors. Based on this, the microscopic reaction mechanism of H₂ and CO₂ under the condition of plasma discharge was studied by first-principles calculation, and the influences of different temperatures and hydrogen isotope effect on the reaction process were studied. The principal calculation was carried out by the Gaussian 09 software package. The enthalpies and activation energies of these reactions were measured at the level of M06-2X/6-311++G (3d2f, 3p2d). Four initial reaction paths are obtained by using the intrinsic reaction coordinate (IRC) algorithm and finding the transition state of the combined reaction. The thermodynamic easiness of the two pathways to produce CH₄ and CH₃OH and the influence of different hydrogen isotopes on each reaction were compared and studied. It is found that the spontaneous decay of tritium or the high-energy electrons in the plasma will induce hydrogen isotopes to react with CO₂ to form products such as CO, H₂O, CH₄, and CH₃OH; after the high-energy electrons induce the dissociation of CO₂, there are four initial reaction paths. Complex reactions can occur on their own, and there are two tendencies to this complex reaction. Raising the reaction temperature has a certain promoting effect on the conversion of CO₂ into organic matter (CH₄ and CH₃OH).
- CO₂ conversion,
- hydrogen isotope,
- density functional theory,
- plasma,
- reaction path
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First-Principles Calculation of H/CO₂ Interaction in Plasma: A Density Functional Theory-Based Study