Citation: SUN Chengzhen, BAI Bofeng. Selective Permeation of Gas Molecules through a Two-Dimensional Graphene Nanopore[J]. Acta Physico-Chimica Sinica, ;2018, 34(10): 1136-1143. doi: 10.3866/PKU.WHXB201801301 shu

Selective Permeation of Gas Molecules through a Two-Dimensional Graphene Nanopore

SUN Chengzhen ,
BAI Bofeng ^,

State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Xi'an 710049, P. R. China

Corresponding author: BAI Bofeng, bfbai@mail.xjtu.edu.cn
Received Date: 18 December 2017
Revised Date: 15 January 2018
Accepted Date: 26 January 2018
Available Online: 30 October 2018
Fund Project: The project was supported by the National Natural Science Foundation of China (51506166), China National Funds for Distinguished Young Scientists (51425603) and National Science Foundation for Post-doctoral Scientists of China (2016T90915)China National Funds for Distinguished Young Scientists 51425603National Science Foundation for Post-doctoral Scientists of China 2016T90915the National Natural Science Foundation of China 51506166

Selective molecular permeation through two-dimensional nanopores is of great importance for nanoporous graphene membranes. In this study, we investigate the selective permeation characteristics of gas molecules through a nitrogen-and hydrogen-modified graphene nanopore using molecular dynamics simulations. We reveal the mechanisms of selective molecular permeation from the aspects of molecular size and structure, pore configuration, and interactions between gas molecules and graphene. The results show that the permeances of different molecules are different, and the following order is observed in our study: H₂O > H₂S > CO₂ > N₂ > CH₄. Molecular permeance is related to the molecular size, mass, and molecular density on the graphene surface. The molecular permeation rate is inversely proportional to the molecular mass based on gas kinetic theory, while the molecular density on the graphene surface exerts a positive effect on molecular permeation. The permeance of H₂O molecules is the highest owing to their smallest diameter, while the permeance of CH₄ molecules is the lowest owing to their biggest diameter; in these cases, the molecular size is a dominating factor. For H₂S and CO₂ molecules, the diameters of H₂S molecules are larger than those of CO₂ molecules, but the interactions between H₂S molecules and graphene are stronger, resulting in a stronger permeation ability of H₂S molecules. Between CO₂ and N₂ molecules, CO₂ molecules show higher permeation rates owing to smaller diameters and stronger interactions with graphene. The graphene surface also shows nonuniform molecular density distribution owing to molecular permeation through graphene nanopores. Because of the doped nitrogen atoms, the CH₄ molecules prefer to permeate from the left and right sides of the graphene nanopore, while the other molecules prefer to permeate from the center of the nanopore owing to their small diameters. For the molecules that show stronger interactions with graphene, the molecular density on the graphene surface is higher; accordingly, the residence time on the graphene surface is longer and the experience time period during permeation is also longer. The mechanisms identified in this study can provide theoretical guidelines for the application of graphene-based membranes. In addition, the permeance of gas molecules in the graphene nanopore adopted in this study is on the order of 10^-3 mol·s^-1·m^-2·Pa^-1, and the selectivity of other molecules relative to CH₄ molecules is also high, showing that the membranes based on this type of nanopore can be employed in natural gas processing and other separation industries.
- Graphene nanopore,
- Selective permeation,
- Gas molecules,
- Molecular dynamics
1. [1]
  Geim, A. K.; Novoselov, K. S. Nat. Mater. 2007, 6, 183. doi: 10.1038/nmat1849 doi: 10.1038/nmat1849
2. [2]
  Lee, C.; Wei, X. D.; Kysar, J. W.; Hone, J. Science 2008, 321, 385. doi: 10.1126/science.1157996 doi: 10.1126/science.1157996
3. [3]
  Lei, G. -P.; Liu, C.; Xie, H. Acta Phys. -Chim. Sin. 2015, 31, 660. doi: 10.3866/PKU.WHXB201501291
4. [4]
  Zhao, S. -J.; Zhang, W.; Deng, H. -N.; Liu, W. Acta Phys. -Chim. Sin. 2016, 32, 723. doi: 10.3866/PKU.WHXB201512141
5. [5]
  Jiang, D. E.; Cooper, V. R.; Dai, S. Nano Lett. 2009, 9, 4019. doi: 10.1021/nl9021946@proofing doi: 10.1021/nl9021946@proofing
6. [6]
  Kim, H. W.; Yoon, H. W.; Yoon, S. -M.; Yoo, B. M.; Ahn, B. K.; Cho, Y. H.; Shin, H. J.; Yang, H.; Paik, U.; Kwon, S.; et al. Science 2013, 342, 91. doi: 10.1126/science.1236098 doi: 10.1126/science.1236098
7. [7]
  Koenig, S. P.; Wang, L. D.; Pellegrino, J.; Bunch, J. S. Nat. Nanotechnol. 2012, 7, 728. doi: 10.1038/nnano.2012.162 doi: 10.1038/nnano.2012.162
8. [8]
  Li, H.; Song, Z.; Zhang, X.; Huang, Y.; Li, S.; Mao, Y.; Ploehn, H. J.; Bao, Y.; Yu, M. Science 2013, 342, 95. doi: 10.1126/science.1236686 doi: 10.1126/science.1236686
9. [9]
  Sun, C.; Wen, B.; Bai, B. Sci. Bull. 2015, 60, 1807. doi: 10.1007/s11434-015-0914-9 doi: 10.1007/s11434-015-0914-9
10. [10]
  Wen, B. Y.; Sun, C. Z.; Bai, B. F. Acta Phys. -Chim. Sin. 2015, 31, 261. doi: 10.3866/PKU.WHXB201411271
11. [11]
  Sun, C.; Wen, B.; Bai, B. Chem. Eng. Sci. 2015, 138, 616. doi: 10.1016/j.ces.2015.08.049 doi: 10.1016/j.ces.2015.08.049
12. [12]
  Du, H. L.; Li, J. Y.; Zhang, J.; Su, G.; Li, X. Y.; Zhao, Y. L. J. Phys. Chem. C 2011, 115, 23261. doi: 10.1021/jp206258u doi: 10.1021/jp206258u
13. [13]
  Schrier, J. ACS Appl. Mater. Interf. 2012, 4, 3745. doi: 10.1021/am300867d doi: 10.1021/am300867d
14. [14]
  Shan, M.; Xue, Q.; Jing, N.; Ling, C.; Zhang, T.; Yan, Z.; Zheng, J. Nanoscale 2012, 4, 5477. doi: 10.1039/C2NR31402A doi: 10.1039/C2NR31402A
15. [15]
  Drahushuk, L. W.; Strano, M. S. Langmuir 2012, 28, 16671. doi: 10.1021/la303468r doi: 10.1021/la303468r
16. [16]
  Sun, C.; Boutilier, M. S. H.; Au, H.; Poesio, P.; Bai, B.; Karnik, R.; Hadjiconstantinou, N. G. Langmuir 2014, 30, 675. doi: 10.1021/la403969g doi: 10.1021/la403969g
17. [17]
  Wen, B.; Sun, C.; Bai, B. Phys. Chem. Chem. Phys. 2015, 17, 23619. doi: 10.1039/c5cp03195h doi: 10.1039/c5cp03195h
18. [18]
  Liu, H.; Dai, S.; Jiang, D. Nanoscale 2013, 5, 9984. doi: 10.1039/c3nr02852f doi: 10.1039/c3nr02852f
19. [19]
  Wu, T.; Xue, Q.; Ling, C.; Shan, M.; Liu, Z.; Tao, Y.; Li, X. J. Phys. Chem. C 2014, 118, 7369. doi: 10.1021/jp4096776 doi: 10.1021/jp4096776
20. [20]
  Hauser, A. W.; Schwerdtfeger, P. Phys. Chem. Chem. Phys. 2012, 14, 13292. doi: 10.1039/c2cp41889d doi: 10.1039/c2cp41889d
21. [21]
  Celebi, K.; Buchheim, J.; Wyss, R. M.; Droudian, A.; Gasser, P.; Shorubalko, I.; Kye, J. -I.; Lee, C.; Park, H. G. Science 2014, 344, 289. doi: 10.1126/science.1249097 doi: 10.1126/science.1249097
22. [22]
  Stuart, S. J.; Tutein, A. B.; Harrison, J. A. J. Chem. Phys. 2000, 112, 6472. doi: 10.1063/1.481208 doi: 10.1063/1.481208
23. [23]
  Lei, G.; Liu, C.; Xie, H.; Song, F. Chem. Phys. Lett. 2014, 599, 127. doi: 10.1016/j.cplett.2014.03.040 doi: 10.1016/j.cplett.2014.03.040
24. [24]
  Chae, K.; Violi, A. J. Chem. Phys. 2011, 134, 044537. doi: 10.1063/1.3512918 doi: 10.1063/1.3512918
25. [25]
  Jorgensen, W. L.; Chandrasekhar, J.; Madura, J. D.; Impey, R. W.; Klein, M. L. J. Chem. Phys. 1983, 79, 926. doi: 10.1063/1.445869 doi: 10.1063/1.445869
26. [26]
  Liu, H.; Chen, Z.; Dai, S.; Jiang, D. -E. J. Solid State Chem. 2015, 224, 2. doi: 10.1016/j.jssc.2014.01.030 doi: 10.1016/j.jssc.2014.01.030
27. [27]
  http://www.wiredchemist.com/chemistry/data/bond_energies_lengths.html(accessed on May 3, 2017).
28. [28]
  Harris, J. G.; Yung, K. H. J. Phys. Chem. 1995, 99, 12021. doi: 10.1021/j100031a034 doi: 10.1021/j100031a034
29. [29]
  Kamath, G.; Lubna, N.; Potoff, J. J. J. Chem. Phys. 2005, 123, 124505. doi: 10.1063/1.2049278 doi: 10.1063/1.2049278
30. [30]
  Sun, C.; Bai, B. Phys. Chem. Chem. Phys. 2017, 19, 3894. doi: 10.1039/c6cp06267a doi: 10.1039/c6cp06267a
31. [31]
  Sun, C.; Bai, B. Appl. Therm. Eng. 2017, 116, 724. doi: 10.1016/j.applthermaleng.2017.02.002 doi: 10.1016/j.applthermaleng.2017.02.002
1. [1]
  Yu Peng , Yue Wang , Tian-Jiao Chen , Jing-Jing Chen , Jin-Ling Yang , Ting Gong , Ping Zhu . A fungal CYP from Beauveria bassiana with promiscuous steroid hydroxylation capabilities. Chinese Chemical Letters, 2024, 35(5): 108818-. doi: 10.1016/j.cclet.2023.108818
2. [2]
  Xiaochen Zhang , Fei Yu , Jie Ma . 多角度数理模拟在电容去离子中的前沿应用. Acta Physico-Chimica Sinica, 2024, 40(11): 2311026-. doi: 10.3866/PKU.WHXB202311026
3. [3]
  Shule Liu . Application of SPC/E Water Model in Molecular Dynamics Teaching Experiments. University Chemistry, 2024, 39(4): 338-342. doi: 10.3866/PKU.DXHX202310029
4. [4]
  Cheng-Da Zhao , Huan Yao , Shi-Yao Li , Fangfang Du , Li-Li Wang , Liu-Pan Yang . Amide naphthotubes: Biomimetic macrocycles for selective molecular recognition. Chinese Chemical Letters, 2024, 35(4): 108879-. doi: 10.1016/j.cclet.2023.108879
5. [5]
  Shuanglin TIAN , Tinghong GAO , Yutao LIU , Qian CHEN , Quan XIE , Qingquan XIAO , Yongchao LIANG . First-principles study of adsorption of Cl₂ and CO gas molecules by transition metal-doped g-GaN. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1189-1200. doi: 10.11862/CJIC.20230482
6. [6]
  Qihan Lin , Jiabin Xing , Yue-Yang Liu , Gang Wu , Shi-Jia Liu , Hui Wang , Wei Zhou , Zhan-Ting Li , Dan-Wei Zhang . taBOX: A water-soluble tetraanionic rectangular molecular container for conjugated molecules and taste masking for berberine and palmatine. Chinese Chemical Letters, 2024, 35(5): 109119-. doi: 10.1016/j.cclet.2023.109119
7. [7]
  Hanqing Zhang , Xiaoxia Wang , Chen Chen , Xianfeng Yang , Chungli Dong , Yucheng Huang , Xiaoliang Zhao , Dongjiang Yang . Selective CO2-to-formic acid electrochemical conversion by modulating electronic environment of copper phthalocyanine with defective graphene. Chinese Journal of Structural Chemistry, 2023, 42(10): 100089-100089. doi: 10.1016/j.cjsc.2023.100089
8. [8]
  Zhigang Zeng , Changzhou Liao , Lei Yu . Molecules for COVID-19 treatment. Chinese Chemical Letters, 2024, 35(7): 109349-. doi: 10.1016/j.cclet.2023.109349
9. [9]
  Chenghao Ge , Peng Wang , Pei Yuan , Tai Wu , Rongjun Zhao , Rong Huang , Lin Xie , Yong Hua . Tuning hot carrier transfer dynamics by perovskite surface modification. Chinese Chemical Letters, 2024, 35(10): 109352-. doi: 10.1016/j.cclet.2023.109352
10. [10]
  Xinqiong Li , Guocheng Rao , Xi Peng , Chan Yang , Yanjing Zhang , Yan Tian , Xianghui Fu , Jia Geng . Direct detection of C9orf72 hexanucleotide repeat expansions by nanopore biosensor. Chinese Chemical Letters, 2024, 35(5): 109419-. doi: 10.1016/j.cclet.2023.109419
11. [11]
  Ji Liu , Dongsheng He , Tianjiao Hao , Yumin Hu , Yan Zhao , Zhen Li , Chang Liu , Daquan Chen , Qiyue Wang , Xiaofei Xin , Yan Shen . Gold mineralized "hybrid nanozyme bomb" for NIR-II triggered tumor effective permeation and cocktail therapy. Chinese Chemical Letters, 2024, 35(9): 109296-. doi: 10.1016/j.cclet.2023.109296
12. [12]
  Fang-Yuan Chen , Wen-Chao Geng , Kang Cai , Dong-Sheng Guo . Molecular recognition of cyclophanes in water. Chinese Chemical Letters, 2024, 35(5): 109161-. doi: 10.1016/j.cclet.2023.109161
13. [13]
  Xiaoyan Peng , Xuanhao Wu , Fan Yang , Yefei Tian , Mingming Zhang , Hongye Yuan . Gas sensors based on metal-organic frameworks: challenges and opportunities. Chinese Journal of Structural Chemistry, 2024, 43(3): 100251-100251. doi: 10.1016/j.cjsc.2024.100251
14. [14]
  Xianxu Chu , Lu Wang , Junru Li , Hui Xu . Surface chemical microenvironment engineering of catalysts by organic molecules for boosting electrocatalytic reaction. Chinese Chemical Letters, 2024, 35(8): 109105-. doi: 10.1016/j.cclet.2023.109105
15. [15]
  Hongxia Li , Xiyang Wang , Du Qiao , Jiahao Li , Weiping Zhu , Honglin Li . Mechanism of nanoparticle aggregation in gas-liquid microfluidic mixing. Chinese Chemical Letters, 2024, 35(4): 108747-. doi: 10.1016/j.cclet.2023.108747
16. [16]
  Shiyu Hou , Maolin Sun , Liming Cao , Chaoming Liang , Jiaxin Yang , Xinggui Zhou , Jinxing Ye , Ruihua Cheng . Computational fluid dynamics simulation and experimental study on mixing performance of a three-dimensional circular cyclone-type microreactor. Chinese Chemical Letters, 2024, 35(4): 108761-. doi: 10.1016/j.cclet.2023.108761
17. [17]
  Kezhen Qi , Shu-yuan Liu , Ruchun Li . Selective dissolution for stabilizing solid electrolyte interphase. Chinese Chemical Letters, 2024, 35(5): 109460-. doi: 10.1016/j.cclet.2023.109460
18. [18]
  Caihong Mao , Yanfeng He , Xiaohan Wang , Yan Cai , Xiaobo Hu . Synthesis and molecular recognition characteristics of a tetrapodal benzene cage. Chinese Chemical Letters, 2024, 35(8): 109362-. doi: 10.1016/j.cclet.2023.109362
19. [19]
  Tian Cao , Xuyin Ding , Qiwen Peng , Min Zhang , Guoyue Shi . Intelligent laser-induced graphene sensor for multiplex probing catechol isomers. Chinese Chemical Letters, 2024, 35(7): 109238-. doi: 10.1016/j.cclet.2023.109238
20. [20]
  Rui Liu , Jinbo Pang , Weijia Zhou . Monolayer water shepherding supertight MXene/graphene composite films. Chinese Journal of Structural Chemistry, 2024, 43(10): 100329-100329. doi: 10.1016/j.cjsc.2024.100329

Get Citation

PDF

XML

Metrics

PDF Downloads(7)
Abstract views(268)
HTML views(43)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142