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
1. [1]
  Hassanein A, Sizyuk V. Potential Design Problems for ITER Fusion Device[J]. Sci. Rep., 2021,11(1)2069. doi: 10.1038/s41598-021-81510-2
2. [2]
  Cristescu I R, Cristescu I, Doerr L, Glugla M, Murdoch D. Tritium Inventories and Tritium Safety Design Principles for the Fuel Cycle of ITER[J]. Nucl. Fusion, 2007,47(7):S458-S463. doi: 10.1088/0029-5515/47/7/S08
3. [3]
  Glugla M, Lasser R, Dorr L, Murdoch D K, Haange R, Yoshida H. The Inner Deuterium/Tritium Fuel Cycle of ITER[J]. Fusion Eng. Des., 2003,69(1/2/3/4):39-43.
4. [4]
  Glugla M, Caldwell-Nichols C, Cristescu I R, Doerr L, Hellriegel G, Laesser R, Murdoch D, Schaefer P. Protection of the Primary Circuits and Effect on the Design of the Inner Deuterium/Tritium Fuel Cycle of ITER[J]. Fusion Eng. Des., 2005,75-79:637-643. doi: 10.1016/j.fusengdes.2005.06.047
5. [5]
  Chen Z, Hu X X, Ye M Y, Wirth B D. Deuterium Transport and Retention Properties of Representative Fusion Blanket Structural Materials[J]. J. Nucl. Mater., 2021,549152904. doi: 10.1016/j.jnucmat.2021.152904
6. [6]
  Fridman A. Plasma Chemistry. Philadelphia: Drexel University, 2008: 5
7. [7]
  Bogaerts A, Neyts E, Gijbels R, van der Mullen J. Gas Discharge Plasmas and Their Applications. Spectrochim[J]. Acta Pt. B—Atom. Spectr., 2002,57(4):609-658. doi: 10.1016/S0584-8547(01)00406-2
8. [8]
  Federici G, Anderl R A, Andrew P, Brooks J N, Causey R A, Coad J P, Cowgill D, Doerner R P, Haasz A A, Janeschitz G, Jacob W, Longhurst G R, Nygren R, Peacock A, Pic M A, Philipps V, Roth J, Skinner C H, Wampler W R. In-Vessel Tritium Retention and Removal in ITER[J]. J. Nucl. Mater., 1999,266:14-29.
9. [9]
  Song J, Xiong Y, Lang L, Shi Y, Ba J, Jing W, He M. Radiochemical Reaction of DT/T₂ and CO under High Pressure[J]. J. Hazard. Mater., 2019,378120720. doi: 10.1016/j.jhazmat.2019.05.113
10. [10]
  Douglas D L. Tritium-Carbon Monoxide Reaction[J]. J. Chem. Phys., 1955,23(8):1558-1559.
11. [11]
  O′hira S, Nakamura H, Okuno K, Taylor D J, Sherman R H. Beta-Decay Induced Reaction Studies of Tritium by Laser Raman Spectroscopy[J]. Fusion Technol., 1995,28(3):1239-1243.
12. [12]
  Styring P, Quadrelli E A, Armstrong K. Carbon Dioxide Utilisation: Closing the Carbon Cycle. Amsterdam: Elsevier, 2014: 9-20
13. [13]
  Aresta M, Dibenedetto A, Angelini A. Catalysis for the Valorization of Exhaust Carbon: From CO₂ to Chemicals, Materials, and Fuels. Technological Use of CO₂[J]. Chem. Rev., 2014,114(3):1709-1742. doi: 10.1021/cr4002758
14. [14]
  Centi G, Quadrelli E A, Perathoner S. Catalysis for CO₂ Conversion: A Key Technology for Rapid Introduction of Renewable Energy in the Value Chain of Chemical Industries[J]. Energy Environ. Sci., 2013,6(6):1711-1731. doi: 10.1039/c3ee00056g
15. [15]
  Eliasson B, Kogelschatz U, Xue B, Zhou L M. Hydrogenation of Carbon Dioxide to Methanol with a Discharge-Activated Catalyst[J]. Ind. Eng. Chem. Res., 1998,37(8):3350-3357. doi: 10.1021/ie9709401
16. [16]
  Hayashi N, Yamakawa T, Baba S. Effect of Additive Gases on Synthesis of Organic Compounds from Carbon Dioxide Using Non-thermal Plasma Produced by Atmospheric Surface Discharges[J]. Vacuum, 2006,80(11/12):1299-1304.
17. [17]
  Zeng Y, Tu X. Plasma-Catalytic CO₂ Hydrogenation at Low Temperatures[J]. IEEE Trans. Plasma Sci., 2016,44(4):405-411. doi: 10.1109/TPS.2015.2504549
18. [18]
  de Bie C, van Dijk J, Bogaerts A. CO₂ Hydrogenation in a Dielectric Barrier Discharge Plasma Revealed[J]. J. Phys. Chem. C, 2016,120(44):25210-25224. doi: 10.1021/acs.jpcc.6b07639
19. [19]
  Maya L. Plasma-Assisted Reduction of Carbon Dioxide in the Gas Phase[J]. J. Vac. Sci. Technol. A, 2000,18(1):285-287. doi: 10.1116/1.582148
20. [20]
  de la Fuente J F, Moreno S H, Stankiewicz A I, Stefanidis G D. A New Methodology for the Reduction of Vibrational Kinetics in Nonequilibrium Microwave Plasma: Application to CO₂ Dissociation[J]. React. Chem. Eng., 2016,1(5):540-554. doi: 10.1039/C6RE00044D
21. [21]
  Kano M, Satoh G, Iizuka S. Reforming of Carbon Dioxide to Methane and Methanol by Electric Impulse Low-Pressure Discharge with Hydrogen[J]. Plasma Chem. Plasma Process., 2012,32(2):177-185. doi: 10.1007/s11090-011-9333-0
22. [22]
  Bogaerts A, Kozák T, van Laer K, Snoeckx R. Plasma-Based Conversion of CO₂: Current Status and Future Challenges[J]. Faraday Discuss., 2015:217-232.
23. [23]
  Corrigan S J. Dissociation of Molecular Hydrogen by Electron Impact[J]. J. Chem. Phys., 1965,43(12):4381-4386. doi: 10.1063/1.1696701
24. [24]
  SHI C Y, REN L, KONG F A. Chemical Reaction and Energy Transfer between Hot H Atoms and CO₂ Molecules[J]. Chinese J. Chem. Phys., 2006,19(6):473-477. doi: 10.3969/j.issn.1674-0068.2006.06.002
25. [25]
  Zhao Y, Truhlar D G. The M06 Suite of Density Functionals for Main Group Thermochemistry, Thermochemical Kinetics, Noncovalent Interactions, Excited States, and Transition Elements: Two New Functionals and Systematic Testing of Four M06-Class Functionals and 12 Other Function[J]. Theor. Chem. Acc., 2008,120(1/2/3):215-241.
26. [26]
  Zhao Y, Truhlar D G. Density Functionals with Broad Applicability in Chemistry[J]. Acc. Chem. Res., 2008,41(2):157-167. doi: 10.1021/ar700111a
27. [27]
  Frisch M J, Pople J A, Binkley J S. Self-Consistent Molecular Orbital Methods 25. Supplementary Functions for Gaussian Basis Sets[J]. J. Chem. Phys., 1984,80(7):3265-3269. doi: 10.1063/1.447079
28. [28]
  Lu T, Chen Q X. Shermo: A General Code for Calculating Molecular Thermochemistry Properties[J]. Comput. Theor. Chem., 2021,1200113249. doi: 10.1016/j.comptc.2021.113249
29. [29]
  Lu T. TSTcalculator. http://sobereva.com/310
30. [30]
  DONG Y Y, WANG Y, ZHANG F Y. Inorganic and Analytical Chemistry. 3rd ed, . Beijing: Science Press 2011: 45
31. [31]
  Fukui K. The Path of Chemical Reactions—The IRC Approach[J]. Acc. Chem. Res., 1981,14(12):363-368. doi: 10.1021/ar00072a001
32. [32]
  Jiang Z, Xiao T, Kuznetsov V L, Edwards P P. Turning Carbon Dioxide into Fuel[J]. Philos. Trans. R. Soc. A-Math. Phys. Eng. Sci., 2010,368(1923):3343-3364.
33. [33]
  Rayne S. Review of the Carbon Dioxide Splitting Patent Literature[J]. Nature Precedings, 2008.
34. [34]
  Snoeckx R, Bogaerts A. Plasma Technology—A Novel Solution for CO₂ Conversion?[J]. Chem. Soc. Rev., 2017,46(19):5805-5863.
35. [35]
  XIONG Y F, LEI Q H, LIU L, JING W Y. Researches on Irradiation Properties of Deuterium-Tritium Mixed Gases with CO₂ in Room Temperature[J]. Nuclear Science and Techniques, 2018,6(3):55-60.
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First-Principles Calculation of H/CO2 Interaction in Plasma: A Density Functional Theory-Based Study

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