Citation: LIU Xiao-Qiang, TIAN Zhi-Yue, CHU Wei, XUE Ying. CH₄, CO₂ and H₂OAdsorption on Nonmetallic Atom-Decorated Graphene Surfaces[J]. Acta Physico-Chimica Sinica, ;2014, 30(2): 251-256. doi: 10.3866/PKU.WHXB201312243 shu

CH₄, CO₂ and H₂OAdsorption on Nonmetallic Atom-Decorated Graphene Surfaces

1.
1 Key Laboratory of Green Chemistry and Technology of the Ministry of Education, College of Chemistry, Sichuan University, Chengdu 610064, P. R. China;
2 College of Chemical Engineering, Sichuan University, Chengdu 610065, P. R. China

Received Date: 4 November 2013
Available Online: 24 December 2013
Fund Project: 国家重点基础研究发展规划项目(973)(2011CB201202) (973)(2011CB201202)国家自然科学基金(21173151)资助 (21173151)

As an unconventional gas, coalbed methane (CBM) is a desirable alternative energy source to conventional fossil fuels such as coal, oil, and natural gas. In this work, non-metallic atom X (X=H, O, N, S, P, Si, F, or Cl)- decorated Gr (graphene) (X-Gr) was used to represent the surface models of coal with structural heterogeneity. Using density functional theory, the adsorption of the CBM component Y (Y=CH₄, CO₂, H₂O) on X-Gr was systematically investigated. The results indicate that CH₄, CO₂, and H₂O are weakly bound to X-Gr, and the interactions between the adsorbate and the surface can be described as physisorption, which was identified through the density of states and electronic density difference analysis. Furthermore, CH₄ has very large adsorption energies to H- and Cl-decorated graphene. The dopants X, such as N, O, F, and Cl, are very od adsorbents for CO₂ and the influence of the dopants N and Cl cannot be ignored for the adsorption of H₂O. In general, the adsorption energies of H₂O on X-Gr are larger than those of CO₂, while CH₄ has the lowest adsorption energies, namely, the order of adsorption is H₂O> CO₂>CH₄. Consequently, the injection of H₂O or CO₂ into methane-rich coal seams strongly enhances the CBM recovery efficiency via competitive adsorption with CH₄ on the coal surface. The results provide a molecular-level insight into the interactions between CBM and X-Gr, and might offer useful information for recovery and purification of coalbed methane.
- Density functional theory,
- Coalbed methane,
- Nonmetallic atom-doped graphene,
- Adsorption
1. [1]
  
  (1) Boyer, C. M.; Bai, Q. Z. Int. J. Coal. Geol. 1998, 35, 349. doi: 10.1016/S0166-5162(97)00041-4
2. [2]
  (2) Liang, B.; Sun,W.; Qi, Q.; Li, H. Int. J. Min. Sci. Technol. 2012,22, 891. doi: 10.1016/j.ijmst.2012.12.006
3. [3]
  (3) Chen, G.; Yang, J.; Liu, Z. Energy Fuels 2012, 26, 4583. doi: 10.1021/ef3001168
4. [4]
  (4) Xie, H.; Zhao, X.; Liu, J.; Zhang, R.; Xue, D. Int. J. Min. Sci. Technol. 2012, 22, 749. doi: 10.1016/j.ijmst.2012.12.010
5. [5]
  (5) Jiang,W. P. China Coalbed Methane 2009, 6, 19. [降文萍. 中国煤层气, 2009, 6, 19.]
6. [6]
  (6) Liu, Y. Y.;Wilcox, J. Environ. Sci. Technol. 2011, 45, 809. doi: 10.1021/es102700c
7. [7]
  (7) Kowalczyk, P.; Gauden, P. A.; Terzyk, A. P.; Furmaniak, S.;Harris, P. J. F. J. Phys. Chem. C 2012, 116, 13640. doi: 10.1021/jp302776z
8. [8]
  (8) Jiang, Q.; Chu,W.; Sun,W. J.; Liu, F. S.; Xue, Y. Acta Phys. -Chim. Sin. 2012, 28, 1101. [蒋倩, 储伟, 孙文晶,刘凤嗣, 薛英. 物理化学学报, 2012, 28, 1101.] doi: 10.3866/PKU.WHXB201203054
9. [9]
  (9) Li, S.; Tang, D.; Xu, H.; Yang, Z.; Guo, L. Energy Fuels 2012,26, 5005. doi: 10.1021/ef300432m
10. [10]
  (10) Mathews, J. P.; Chaffee, A. L. Fuel 2012, 96, 1. doi: 10.1016/j.fuel.2011.11.025
11. [11]
  (11) Vejahati, F.; Xu, Z.; Gupta, R. Fuel 2010, 89, 904. doi: 10.1016/j.fuel.2009.06.013
12. [12]
  (12) Zhao, J.; Buldum, A.; Han, J.; Lu, J. P. Nanotechnology 2002,13, 195. doi: 10.1088/0957-4484/13/2/312
13. [13]
  (13) Liu, Y.;Wilcox, J. Environ. Sci. Technol. 2012, 47, 95.
14. [14]
  (14) Qiu, N. X.; Xue, Y.; Guo, Y.; Sun,W. J.; Chu,W. Comp. Theor. Chem. 2012, 992, 37. doi: 10.1016/j.comptc.2012.04.024
15. [15]
  (15) Mo, J. J.; Xue, Y.; Liu, X. Q.; Qiu, N. X.; Chu,W.; Xie, H. P.Surf. Sci. 2013, 616, 85. doi: 10.1016/j.susc.2013.05.009
16. [16]
  (16) Liu, X. Q.; Xue, Y.; Tian, Z. Y.; Mo, J. J.; Qiu, N. X.; Chu,W.Xie, H. P. App. Surf. Sci. 2013, 285P, 190.
17. [17]
  (17) Qu, S.; Yang, J.; Liu, Z. Energy Fuels 2012, 26, 3928. doi: 10.1021/ef300123s
18. [18]
  (18) Segall, M. D.; Lindan, P. J. D.; Probert, M. J.; Pickard, C. J.;Hasnip, P. J.; Clark, S. J.; Payne, M. C. J. Phys.: Condes. Matter 2002, 14, 2717. doi: 10.1088/0953-8984/14/11/301
19. [19]
  (19) Ceperley, D. M.; Alder, B. J. Phys. Rev. Lett. 1980, 45, 566. doi: 10.1103/PhysRevLett.45.566
20. [20]
  (20) Vanderbilt, D. Phys. Rev. B: Condes. Matter 1990, 41,7892. doi: 10.1103/PhysRevB.41.7892
21. [21]
  (21) Monkhorst, H. J.; Pack, J. D. Phys. Rev. B 1976, 13, 5188. doi: 10.1103/PhysRevB.13.5188
22. [22]
  (22) Fujimoto, Y.; Saito, S. Phys. Rev. B 2011, 84, 245446.
23. [23]
  (23) Nakada, K.; Ishii, A. Solid State Commun. 2011, 151, 13. doi: 10.1016/j.ssc.2010.10.036
24. [24]
  (24) Rubea, M.; Kysilka, J.; Nachtigall, P.; Bludsky, O. Phys. Chem. Chem. Phys. 2010, 12, 6438. doi: 10.1039/c001155j
25. [25]
  (25) Vidali, G.; Ihm, G.; Kim, H. Y.; Cole, M.W. Surf. Sci. Rep.1991, 12, 135. doi: 10.1016/0167-5729(91)90012-M
26. [26]
  (26) Mohammad, S. A.; Gasem, K. A. M. Energy Fuels 2012, 26,557. doi: 10.1021/ef201422e
27. [27]
  (27) Firouzi, M.;Wilcox, J. Microporous Mesoporous Mat. 2012,158, 195. doi: 10.1016/j.micromeso.2012.02.045
28. [28]
  (28) Hu, H.; Li, X.; Fang, Z.;Wei, N.; Li, Q. Energy 2010, 35,2939. doi: 10.1016/j.energy.2010.03.028
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沈阳化工大学材料科学与工程学院沈阳 110142

CH4, CO2 and H2OAdsorption on Nonmetallic Atom-Decorated Graphene Surfaces

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通讯作者: 陈斌, bchen63@163.com

CH₄, CO₂ and H₂OAdsorption on Nonmetallic Atom-Decorated Graphene Surfaces