Document Type : Regular Article


1 Department of Chemical Engineering, Borujerd Branch, Islamic Azad University, Borujerd, Iran

2 Department of Chemical Engineering, Amirkabir University of Technology (Tehran Polytechnic), Tehran, Iran

3 Department of Chemical and Petroleum Engineering, Razi University, Kermanshah, Iran


The polysulfone mixed matrix membranes (MMM) with different concentrations of graphene oxide (0, 0.25, 0.5 wt % of the polymer) are fabricated by a phase separation method. The cross-sectional structures and their upper surface were assessed by the (SEM) surface roughness of the membranes assessed by (AFM). The mechanical and thermal stability of the fabricated membranes were evaluated as well. The separation of Carbon dioxide, nitrogen and methane from natural gas was considered. Also, by increasing the concentration of graphene oxide in the polymer matrix, the thickness of the spongy structure increases and the holes of the finger-like membranes are also destroyed. From the cross-sectional images of the outer surface of the MMM, it was concluded that an active selector layer was created on the lower surface of the membrane. The membrane tensile strength and the length of the membrane at fracture point increased slightly with an increase in the concentration of graphene oxide. Transition Glass temperature of the membrane increased by the addition of graphene oxide to the structure. From TGA analysis, in the presence of graphene oxide, the thermal stability improved. From the gas permeation test, by the addition of 0.25 % of graphene oxide to the polymer, CO2 permeability was increased from 61.22 GPU to 76.04 GPU, while the addition of 0.5 wt % resulted in a lower permeability (69.55 GPU). The Nitrogen gas permeation flux of membranes decreased from 10.93 GPU to 3.91 GPU by the addition of 0.50 wt % of graphene oxide. The Methane gas permeation flux is reduced from 11.31 GPU to 6.95 GPU and 4.92 GPU by the addition of 0.25 % and 0.50 % of graphene oxide respectively. In conclusion, an increase in the concentration of graphene oxide increased the carbon dioxide selectivity.


Main Subjects

  • Kuila, T., Bose, S., Mishra, A. K., Khanra, P., Kim, N. H. and Lee, J. H., “Chemical functionalization of graphene and its applications”,Progress in Materials Science, 57, 1061 (2012).
  • Yang, X., Wang, X., Yang, J., Li, J. and Wan, L., “Functionalization of graphene using trimethoxysilanes and its reinforcement on polypropylene nanocomposites”, Chemical Physics Letters, 570, 125 (2013).
  • Li, X., Cheng, Y., Zhang, H., Wang, S., Jiang, Z., Guo, R. and Wu, H., “Efficient CO2 capture by functionalized graphene oxide nanosheets as fillers to fabricate multi-permselective mixed matrix membranes”, ACS Applied Materials & Interfaces, 7 (9), 5528 (2015).
  • Checchetto, R., Miotello, A., Nicolais, L. and Carotenuto, G., “Gas transport through nanocomposite membrane composed by polyethylene with dispersed graphite nanoplatelets”, Journal of Membrane Science, 463, 196 (2014).
  • Liu, H., Huang, W., Yang, X., Dai, K., Zheng, G., Liu, C., Shen, C., Yan, X., Guo, J. and Guo, Z., “Organic vapor sensing behaviors of conductive thermoplastic polyurethane–graphene nanocomposites”, Journal of Materials Chemistry, C, 4, 4459 (2016).
  • Ganesh, B. M., Isloor, A. M. and Ismail, A. F., “Enhanced hydrophilicity and salt rejection study of graphene oxide-polysulfone mixed matrix membrane”, Desalination, 313, 199 (2013).
  • Yadav, M., Rhee, K. Y. and Park, S. J., “Synthesis and characterization of graphene oxide / carboxymethylcellulose / alginate composite blend films”, Carbohydrate Polymers, 110, 18 (2014).
  • Wang, Y., He, Q., Qu, H., Zhang, X., Guo, J., Zhu, J., Zhao, G., Colorado, H. A., Yu, J., Sun, L., Bhana, S., Khan, M. A., Huang, X., Young, D. P., Wang, H., Wang, X., Wei, S. and Guo, Z., “Magnetic graphene oxide nanocomposites: nanoparticles growth mechanism and property analysis”,Journal of Materials Chemistry, C, 2, 9478 (2014).
  • Liu, H., Li, Y., Dai, K., Zheng, G., Liu, C., Shen, C., Yan, X., Guo, J. and Guo, Z., “Electrically conductive thermoplastic elastomer nanocomposites at ultralow graphene loading levels for strain sensor applications”Journal of Materials Chemistry, C, 4, 157 (2016).
  • Zhao, L., Cheng, C., Chen, Y. F., Wang, T., Du, C. H. and Wu, L. G., “Enhancement on the permeation performance of polyimide mixed matrix membranes by incorporation of graphene oxide with different oxidation degrees”, Polymers for Advanced Technologies, 26 (4), 330 (2015).
  • Ionita, M., Pandele, A. M., Crica, L. and Pilan, L., “Improving the thermal and mechanical properties of polysulfone by incorporation of graphene oxide”, Composites Part B: Engineering, 59, 133 (2014).
  • Zulhairun, A. K., Ng, B. C., Ismail, A. F., Surya Murali, R. and Abdullah, M. S., “Production of mixed matrix hollow fiber membrane for CO2/CH4 separation”, Separation and Purification Technology, 137, 1 (2014).
  • Zulhairun, A. K., Ismail, A. F., Matsuura, T., Abdullah, M. S. and Mustafa, A., “Asymmetric mixed matrix membrane incorporating organically modified clay particle for gas separation”, Chemical Engineering Journal, 241, 495 (2014).
  • Zulhairun, A. K. and Ismail, A. F., “The role of layered silicate loadings and their dispersion states on the gas separation performance of mixed matrix membrane”, Journal of Membrane Science, 468, 20 (2014).
  • Kim, S., Chen, L., Johnson, J. K. and Marand, E., “Polysulfone and functionalized carbon nanotube mixed matrix membranes for gas separation: Theory and experiment”, Journal of Membrane Science, 294 (1-2), 147 (2007).
  • Zhao, Y., Ding, H. and Zhong, Q., “Preparation and characterization of aminated graphite oxide for CO2 capture”, Applied Surface Science, 258 (10), 4301 (2012).
  • Md Nordin, N. A. H., Racha, S. M., Matsuura, T., Misdan, N., Abdullah Sani, N. A., Ismail, A. F. and Mustafa, A., “Facile modification of ZIF-8 mixed matrix membrane for CO2/CH4 separation: Synthesis and preparation”, RSC Advances, 5 (54), 43110 (2015).
  • Md Nordin, N. A. H., Ismail, A. F., Mustafa, A., Surya Murali, R. and Matsuura, T., “The impact of ZIF-8 particle size and heat treatment on CO2/CH4 separation using asymmetric mixed matrix membrane”, RSC Advances, 4 (94), 52530 (2014).
  • Shen, J., Zhang, M., Liu, G., Guan, K. and Jin, W., “Size effects of graphene oxide on mixed matrix membranes for CO2 separation”, AIChE Journal, 62 (8), 2843 (2016).
  • Zahri, K., Wong, K. C., Goh, P. S. and Ismail, A. F., “Graphene oxide/ polysulfone hollow fiber mixed matrix membrane for gas separation”, RSC Advances, 6 (92), 89130 (2016).
  • Mahmoud, K. A., Mansoor, B., Mansour, A. and Khraisheh, M., “Functional graphene nanosheets: The next generation membranes for water desalination”, Desalination, 356, 208 (2015).
  • Chang, D. W., Choi, H. -J., Jeon, I. -Y., Seo, J. M., Dai, L. and Baek, J. B., “Solvent-free mechanochemical reduction of graphene oxide”, Carbon, 77, 501 (2014).
  • Wu, T., Wang, X., Qiu, H., Gao, J., Wang, W. and Liu, Y., “Graphene oxide reduced and modified by soft nanoparticles and its catalysis of the Knoevenagel condensation”, Journal of Materials Chemistry, 22 (11), 4772 (2012).
  • Thi Vu, T. H., Thi Tran, T. T., Thi Le, H. N., Thi Nguyen, P. H., Bui, N. Q. and Essayem, N., “A new green approach for the reduction of graphene oxide nanosheets using caffeine”, Bulletin of Materials Science, 38 (3), 667 (2015).
  • Loryuenyong, V., Totepvimarn, K., Eimburanapravat, P., Boonchompoo, W. and Buasri, A., “Preparation and characterization of reduced graphene oxide sheets via water-based exfoliation and reduction methods”, Advances in Materials Science and Engineering, 2013, Article ID 923403, (2013).
  • Rahbari-Sisakht, M., Ismail, A. F., Rana, D. and Matsuura, T., “A novel surface modified polyvinylidene fluoride hollow fiber membrane contactor for CO2 absorption”, Journal of Membrane Science, 415-416, 221 (2012).
  • Lan, Y., Liu, H., Cao, X., Zhao, S., Dai, K., Yan, X., Zheng, G., Liu, C., Shen, C. and Guo, Z., “Electrically conductive thermoplastic polyurethane/ polypropylene nanocomposites with selectively distributed graphene”, Polymer, 97, 11 (2016).
  • Aditya Kiran, S., Lukka Thuyavan, Y., Arthanareeswaran, G., Matsuura, T. and Ismail, A. F., “Impact of graphene oxide embedded polyethersulfone membranes for the effective treatment of distillery effluent”, Chemical Engineering Journal, 286, 528 (2016).
  • Nwanonenyi, S. C., Obidiegwu, M. U. and Onuegbu, G. C., “Effects of particle sizes, filler contents and compatibilization on the properties of linear low density polyethylene filled periwinkle shell powder”, The International Journal of Engineering and Science (IJES), 2 (2), 1 (2013).
  • Hashemifard, S. A., Ismail, A. F. and Matsuura, T., “Mixed matrix membrane incorporated with large pore size halloysite nanotubes (HNTs) as filler for gas separation: Morphological diagram”, Chemical Engineering Journal, 172 (1), 581 (2011).
  • Baker, R. W., Membrane technology and applications, 3rd edition, Wiley, p. 11 (2012).
  • Kiadehi, A. D., Jahanshahi, M., Rahimpour, A. and Ghoreyshi, S. A. A., “The effect of functionalized carbon nano-fiber (CNF) on gas separation performance of polysulfone (PSf) membranes”, Chemical Engineering and Processing: Process Intensification, 90, 41 (2015).
  • Junaidi, M. U. M., Leo, C. P., Kamal, S. N. M., Ahmad, A. L. and Chew, T. L., “Carbon dioxide removal from methane by using polysulfone/SAPO-44 mixed matrix membranes”, Fuel Processing Technology, 112, 1 (2013).