Flat mixed matrix membranes incorporating MIL-53(Al) and polyethersulfone for highly selective H2/CO2 and H2/CH4 separation
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Keywords:
hydrogen separation, MIL-53(Al), membranes, PES
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Abstract
The integration of metal-organic frameworks (MOFs) as fillers in hybrid membranes commonly termed mixed matrix membranes (MMMs) represents a significant advancement in the field of gas separation technology. This present study proposes novel MMMs for the separation of H2, CH4, and CO2. The Material Institute of Lavoisier framework (MIL-53(Al)) was incorporated into a polyethersulfone (PES) matrix at filler loadings of 10%, 20%, and 30% (w/w). IR and SEM analyses confirmed that the irregular MIL-53(Al) particles were uniformly dispersed within the PES matrix. The gas separation performance was evaluated using both single gas feeds (H2, CO2, CH4) and mixed gas feeds (H2/CO2 and CO2/CH4) under 2 bar pressure at 30 °C. In comparison to the pristine PES membrane, the incorporation of MIL-53(Al) considerably enhanced gas permeability, with the 30% MIL-53(Al)@PES membrane demonstrating remarkable single-gas permeation performance. It is also notable that the membrane containing 20% MIL-53(Al) achieved the highest selectivity for H2/CO2 and CO2/CH4 (3.28), representing a 54.72% improvement over the pristine PES membrane. Interestingly, almost all MIL-53(Al)@PES membranes exhibited exceptional H2/CO2 separation performance, exceeding the Robeson upper bound. However, for the H2/CH4 and CO2/CH4 mixed gas separation tests, the selectivity of 1.82 and 0.32, respectively, was observed for the 20% MIL-53(Al) membrane, closely resembling the performance of the pure PES membrane. The present work demonstrates that the integration of MIL-53(Al) into PES is an effective strategy to enhance membrane penetrability and H2/CO2 separation performance, thereby highlighting its potential for the improvement of MOF-based mixed matrix membranes for selective gas separation.
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Pratama, J. H., Rahman, B. F., Azhari, F., Gunawan, T., Widiastuti, N., Fansuri, H., … Lestari, W. W. (2026). Flat mixed matrix membranes incorporating MIL-53(Al) and polyethersulfone for highly selective H2/CO2 and H2/CH4 separation. Communications in Science and Technology, 11(1), 191–199. https://doi.org/10.21924/cst.11.1.2026.1954
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References
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3. K. A. Dahl, J. T. Abatzoglou, C. A. Phillips, J. P. Ortiz-Partida, R. Licker, R., L. D. Merner, et al., Quantifying the contribution of major carbon producers to increases in vapor pressure deficit and burned area in western US and southwestern Canadian forests, Environ. Res. Lett. 18 (2023).
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5. R. Holze, On efficiencies, emissions, and the colors of hydrogen—An update, Energy Storage Convers. 1 (2023) 304–304.
6. K. Oka, Y. Kaiwa, M. Kataoka, K. Fujita, Ichi, and K. Oyaizu, A Polymer Sheet-Based Hydrogen Carrier, European J. Org. Chem. (2020) 5876–5879.
7. H. Wang, J. Xu, L. Sheng, X. Liu, Y. Lu, and W. Li, A review on bio-hydrogen production technology, Int. J. Energy Res. 42 (2018) 3442–3453.
8. N. Ain, A. M. Amin, H. Fatimah, and M. Zaid, A Review of Photocatalytic Water Splitting for Hydrogen Production Using Tandem Solar Cell. (2023).
9. I. Staffell, D. Scamman, A. Velazquez Abad, P. Balcombe, P. E. Dodds, P. Ekins, et al., The role of hydrogen and fuel cells in the global energy system, Energy Environ. Sci. 12 (2019) 463–491.
10. C. J. Quarton and S. Samsatli, The value of hydrogen and carbon capture, storage and utilisation in decarbonising energy: Insights from integrated value chain optimisation, Appl. Energy. 257 (2020).
11. M. S. Akhtar, R. Dickson, and J. J. Liu, Life Cycle Assessment of Inland Green Hydrogen Supply Chain Networks with Current Challenges and Future Prospect,. ACS Sustain. Chem. Eng. 9 (2021) 17152–17163.
12. M. Markiewicz, Y. Q. Zhang, A. Bösmann, N. Brückner, J. Thöming, P. Wasserscheid, et al., Environmental and health impact assessment of Liquid Organic Hydrogen Carrier (LOHC) systems – challenges and preliminary results, Energy Environ. Sci. 8 (2015) 1035–1045.
13. A. Golmakani, S. A. Nabavi, and V. Manović, Effect of impurities on ultra-pure hydrogen production by pressure vacuum swing adsorption, J. Ind. Eng. Chem. 82 (2020) 278–289.
14. M. El-Shafie, Hydrogen separation using palladium-based membranes: Assessment of H2 separation in a catalytic plasma membrane reactor, Int. J. Energy Res. 46 (2022) 3572–3587.
15. S. Nayebossadri, J. D. Speight, and D. Book, Hydrogen separation from blended natural gas and hydrogen by Pd-based membranes, Int. J. Hydrogen Energy. 44 (2019) 29092–29099.
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17. A.M. Alghamdi, F. Fadhillah, Thin film composite polyelectrolyte multilayer nanofiltration membrane fabricatedusing spin assisted layer by layer assembly: Application of solution diffusion film mode, Communications in Science and Technology, 5 (2020) 10–15.
18. B. Haider, M. R. Dilshad, M. Atiq ur Rehman, M. S. Akram, and M. Kaspereit, Highly permeable innovative PDMS coated polyethersulfone membranes embedded with activated carbon for gas separation, J. Nat. Gas Sci. Eng. 81 (2020).
19. F. Ahmadijokani, S. Ahmadipouya, H. Molavi, and M. Arjmand, Amino-silane-grafted NH2-MIL-53(Al)/polyethersulfone mixed matrix membranes for CO2/CH4 separation, Dalt. Trans. 48 (2019) 13555–13566.
20. P. Gozali-Balkanloo, M. Mahmoudian and, M. T. Hosseinzadeh, A comparative study between MMT-Fe3O4/PES, MMT-HBE/PES, and MMT-acid activated/PES mixed matrix membranes, Chem. Eng. J. 396 (2020) 125188.
21. T. D. Kusworo, D.P. Qudratun, Utomo, Indriyanti, and I. R. Ramadhan, Enhancement of separation performance of nano hybrid PES –TiO2 membrane using three combination effects of ultraviolet irradiation, ethanol-acetone immersion, and thermal annealing process for CO2 remova, J. Environ. Chem. Eng. 6 (2018) 2865–2873.
22. M. Safak-Boroglu and A. B. Yumru, Gas separation performance of 6FDA-DAM-ZIF-11 mixed-matrix membranes for H2/CH4 and CO2/CH4 separation, Sep. Purif. Technol. 173 (2017) 269–279.
23. C. M. Gao, J. C. Chen, S. H. Liu, Y. Q. Xing, S. F. Ji, H. Y. Chen, et al., Development of hydrophilic PES membranes using F127 and HKUST-1 based on the RTIPS method: Mitigate the permeability-selectivity trade-off, Environ. Res. 196, (2021).
24. W. W. Lestari, M. A. Khafidhin, R. Wijiyanti, N. Widiastuti, D. S. Handayani, U. S. F. Arrozi, et al, Novel mixed matrix membranes based on polyethersulfone and MIL-96 (Al) for CO2 gas separation. Chem. Pap. 75 (2021) 3337–3351 (2021).
25. W. W. Lestari, R. Al Adawiyah, M. A. Khafidhin, R. Wijiyanti, N. Widiastuti, and D. S. Handayani, CO2gas separation using mixed matrix membranes based on polyethersulfone/MIL-100(Al), Open Chem. 19, (2021) 307–321.
26. S. C. Hess, R. N. Grass, and W. J. Stark, MOF Channels within Porous Polymer Film: Flexible, Self-Supporting ZIF-8 Poly(ether sulfone) Composite Membrane, Chem. Mater. 28 (2016) 7638–7644.
27. N. Ercan, C. Kocyigit, A. Durmus, and A. Kasgoz, Cyclic olefin copolymer (COC)-metal organic framework (MOF) mixed matrix membranes (MMMs) for H2/CO2 separation, J. Nat. Gas Sci. Eng. 95, (2021).
28. S. Meshkat, S. Kaliaguine, and D. Rodrigue, Mixed matrix membranes based on amine and non-amine MIL-53(Al) in Pebax® MH-1657 for CO2 separation. Sep. Purif. Technol. 200 (2018) 177–190.
29. M. Loloei, S. Kaliaguine, and D. Rodrigue, Mixed matrix membranes based on NH2-MIL-53 (Al) and 6FDA-ODA polyimide for CO2 separation: Effect of the processing route on improving MOF-polymer interfacial interaction, Sep. Purif. Technol. 270, (2021).
30. W. W. Lestari, L. Yunita, T. E. Saraswati, E. Heraldy, M. A. Khafidhin, Y. K. Krisnandi, et al., Fabrication of composite materials MIL-100(Fe)/Indonesian activated natural zeolite as enhanced CO2 capture material, Chem. Pap. 2021 757. 75 (2021) 3253–3263.
31. S. Basu, A. Cano-Odena, and I. F. J. Vankelecom, MOF-containing mixed-matrix membranes for CO2/CH4 and CO2/N2 binary gas mixture separations, Sep. Purif. Technol. 81 (2011) 31–40.
32. R. Adams, C. Carson, J. Ward, R. Tannenbaum, and W Koros, Metal organic framework mixed matrix membranes for gas separations. Microporous Mesoporous Mater, 131 (2010) 13–20.
33. S. Japip, Y. Xiao, and T. S. Chung, Particle-Size Effects on Gas Transport Properties of 6FDA-Durene/ZIF-71 Mixed Matrix Membranes, Ind. Eng. Chem. Res. 55 (2016) 9507–9517.
34. K. Xie, Q. Fu, J. Kim, H. Lu, Y. He, Q Zhao, et al, Increasing both selectivity and permeability of mixed-matrix membranes: Sealing the external surface of porous MOF nanoparticles, J. Memb. Sci. 535 (2017) 350–356.
35. T. Gunawan, R. P. Rahayu, R. Wijiyanti, W. N. W. Salleh, and N. Widiastuti, P84/Zeolite-Carbon Composite Mixed Matrix Membrane for CO 2 /CH 4 Separation. Indones, J. Chem. 19 (2019) 650–659.
36. R. Lin, L. Ge, S. Liu, V. Rudolph, and Z. Zhu, Mixed-Matrix Membranes with Metal–Organic Framework-Decorated CNT Fillers for Efficient CO2 Separation, ACS Appl. Mater. Interfaces. 7 (2015) 14750–14757.
37. T. Gunawan, N. Widiastuti, H. Fansuri, W. N. Wan Salleh, A F. Ismail, R. Lin, et. al., The utilization of micro-mesoporous carbon-based filler in the P84 hollow fibre membrane for gas separation, R. Soc. Open Sci. 8, (2021).
38. A. Chakraborty and H. Acharya, Magnetically separable Fe3O4 NPs/MIL-53(Al) nanocomposite catalyst for intrinsic OPD oxidation and colorimetric hydrogen peroxide detection. Colloids Surfaces A Physicochem, Eng. Asp. 624, (2021).
39. T. R. Katugampalage, C. Ratanatawanate, P. Opaprakasit, C. Kaewsaneha, and P. Sreearunothai, A smart magnetically separable MIL-53(Al) MOF-coated nano-adsorbent for antibiotic pollutant removal with rapid and non-contact inductive heat regeneration, Chem. Eng. J. Adv. 8 (2021) 100160.
40. A. Khodayari and S. Sohrabnezhad, Fabrication of MIL-53(Al)/Ag/AgCl plasmonic nanocomposite: An improved metal organic framework based photocatalyst for degradation of some organic pollutants, J. Solid State Chem. 297 (2021).
41. J. Han, W. Lee, J. M. Choi, R. Patel, and B. R. Min, Characterization of polyethersulfone/polyimide blend membranes prepared by a dry/wet phase inversion: Precipitation kinetics, morphology and gas separation. J. Memb, Sci. 351 (2010) 141–148.
42. T. H. Novita, W. W. Lestari, J. H. Pratama, T. Gunawan, N. Widiastuti, and D. S. Handayani, Novel mixed matrix membranes (MMMs) based on metal–organic framework (MOF) [Mg3(BTC)2]/poly-ether sulfone (PES): preparation and application for CO2 gas separation, Journal of Polymer Research, 28 (2021) 434
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