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Molecular model construction of Danhou lignite and study on adsorption of CH4 by oxygen functional groups

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Abstract

In view of the frequent occurrence of gas accidents in coal mines, the mechanism of oxygen-containing functional groups (OCFGs) in Danhou lignite adsorbing gas was studied by experiment and simulation. Elemental analysis, X-ray photoelectron spectroscopy (XPS), solid-state 13C nuclear magnetic resonance spectroscopy (13C-NMR), and adsorption experiment of CH4 were applied to establish the macromolecular model of Danhou lignite. Then, molecular mechanics (MM) and molecular dynamics (MD) were utilized to optimize the coal macromolecular model, and the density of coal was determined via adding periodic boundary conditions. The mechanism of gas adsorption by OCFGs was studied by grand canonical Monte Carlo (GCMC) and density functional theory (DFT). The results showed that the aromatic structures mostly exist in the form of pyrenes; the structure of aliphatic carbons are mostly methylene and methine groups; the alkanes are mostly long chains; oxygen atoms are mainly in the form of hydroxyl groups and ether groups; nitrogen atoms are mainly in the form of pyridines; and the density of Danhou lignite is 1.25 g/cm3. The isotherm adsorption curve and Langmuir adsorption curve have a good fit, a single coal molecule reaches saturation after absorbing four CH4 molecules, and the error between experiment and simulation is small. The results of DFT calculation showed that the adsorption of CH4 by OCFGs is affected by the adsorption positions and adsorption directions. Due to CH4 molecules are affected by different electrostatic forces, the adsorption capacities of OCFGs are different, and the order is carbonyl groups > ether bonds > hydroxyl groups > carboxyl groups. The results can be used for reference in the prevention and control of coal and gas outburst.

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Data availability

All data generated or analyzed during this study are included in this published article.

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

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Funding

This study was funded by the National Key R&D Program of China (Grant No. 2016YFC0801800), the National Natural Science Foundation of China (Grant No. 51704299 and Grant No. 51804311), and the Open Research Fund of State Key Laboratory of Coal Mine Safety Technology (Project No. sklcmst102).

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Authors and Affiliations

  1. School of Emergency Management and Safety Engineering, China University of Mining and Technology (Beijing), No. ding 11 College Road, Haidian District, Beijing, 100083, China

    Hongqing Zhu, Yujia Huo, Xin He, Wei Wang, Shuhao Fang & Yilong Zhang

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  1. Hongqing Zhu
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  2. Yujia Huo
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  3. Xin He
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  4. Wei Wang
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  5. Shuhao Fang
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  6. Yilong Zhang
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Contributions

Hongqing Zhu and Yujia Huo conceived and designed the study. All authors participated in the experimental process. Yujia Huo and Xin He were involved in the data analysis. Yujia Huo and Xin He wrote the first draft of the manuscript. Wei Wang, Shuhao Fang, and Yilong Zhang revised the first draft. All authors have read and approved the final manuscript.

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Correspondence to Yujia Huo.

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Zhu, H., Huo, Y., He, X. et al. Molecular model construction of Danhou lignite and study on adsorption of CH4 by oxygen functional groups. Environ Sci Pollut Res 28, 25368–25381 (2021). https://doi.org/10.1007/s11356-021-12399-7

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  • DOI: https://doi.org/10.1007/s11356-021-12399-7

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