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A density functional theory study on the adsorption reaction mechanism of double CO2 on the surface of graphene defects

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Abstract

Much research has been done on reactions of a single CO2 molecule with a graphene surface. In this paper, density functional theory calculations are used to investigate the adsorption and reaction of double CO2 on the surface of single vacancy (SV) and divacancy (DV) defect graphene. The study found that due to the mutual repulsion between CO2 and the size of the SV defect, it is difficult for two CO2 molecular to be adsorbed directly above the SV defect at the same time. Regardless of SV or DV, the adsorption of the first CO2 in the defect center will have a beneficial effect on the adsorption of the second CO2. In addition, the transition state calculation of the CO2 reaction on the DV plane was carried out, and the adsorption behavior was analyzed and studied. This in-depth study is helpful to the understanding of the reaction behavior of CO2 on graphene, and further exploration in the direction of the effective application of graphene to the reaction and adsorption of CO2.

Graphical abstract

Our work explores the adsorption behavior of CO2 on graphene surfaces, the physical and chemical adsorption of double CO2 at the defect was studied and analyzed.

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Data availability

The datasets used or analyzed during the current study are available from the corresponding author on reasonable request.

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Funding

The authors acknowledge the financial support of the financial support from the Young Elite Scientist Sponsorship Program by CAST (YESS20210090), and the National Natural Science Foundation of China (51974019, 51804025 and 51774032). All calculations were performed with the support of the Niagara supercomputer at the SciNet HPC Consortium in the Compute/Calcul Canada national computing platform. SciNet is funded by the Canada Foundation for Innovation under the auspices of Compute Canada, the Government of Ontario, Ontario Research Fund—Research Excellence, and the University of Toronto. The authors acknowledge Prof. Mansoor Barati of the University of Toronto for the technical support.

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Authors and Affiliations

  1. School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, 30 Xueyuan Rd., Haidian District, Beijing, 100083, People’s Republic of China

    Shujie Zhang, Zeng Liang, Kejiang Li & Jianliang Zhang

  2. College of Materials Science and Engineering, Chongqing University, Chongqing, People’s Republic of China

    Shan Ren

Authors
  1. Shujie Zhang
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  2. Zeng Liang
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  3. Kejiang Li
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  4. Jianliang Zhang
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Contributions

Shujie Zhang: computation, simulation, analysis, and draft writing. Kejiang Li: analysis and interpretation of data for the work and modify the manuscript. Zeng Liang: discussion, modify the manuscript, and participate in discussions. Jianliang Zhang: investigation, supervision, and funding acquisition.

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Correspondence to Kejiang Li or Shan Ren.

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Supplementary Information

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894_2022_5105_MOESM1_ESM.docx

Supplementary file1. The adsorption energies of four kinds of physical adsorption structures on the plane: original graphene surface; SW surface defects; Single vacancy defect surface; Double vacancy defect surface, the data in bold in the table is the optimal adsorption energy. (DOCX 35 KB)

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Zhang, S., Liang, Z., Li, K. et al. A density functional theory study on the adsorption reaction mechanism of double CO2 on the surface of graphene defects. J Mol Model 28, 118 (2022). https://doi.org/10.1007/s00894-022-05105-y

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  • DOI: https://doi.org/10.1007/s00894-022-05105-y

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