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Engineering >> 2023, Volume 23, Issue 4 doi: 10.1016/j.eng.2022.02.017

Membrane Contact Demulsification: A Superhydrophobic ZIF-8@rGO Membrane for Water-in-Oil Emulsion Separation

a State Key Laboratory of Chemical Resource Engineering, College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China

b State Key Laboratory of Chemistry and Utilization of Carbon-Based Energy Resources, College of Chemistry, Xinjiang University, Urumqi 830046, China

c Institute of Physical Chemistry and Electrochemistry, Leibniz Universität Hannover, Hannover D-30167, Germany

d Guangdong Engineering Technology Research Center of Advanced Insulating Coating, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, China

Received: 2021-10-15 Revised: 2021-12-18 Accepted: 2022-02-14 Available online: 2023-02-21

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Abstract

Achieving a water–oil interface imbalance has been identified as a critical factor in the demulsification of water-in-oil emulsions. However, conventional demulsifying membranes generally break the interface balance by depending on a relatively high transmembrane pressure. Here, we present a "contact demulsification" concept to naturally and quickly achieve disruption of the water–oil interface balance. For this purpose, a novel demulsifying membrane with a high flux of the organic component has been developed via the simple vacuum assembly of zeolitic imidazolate framework-8 (ZIF-8)@reduced graphene oxide (rGO) microspheres (ZGS) on a polytetrafluoroethylene (PTFE) support, followed by immobilization processing in a polydimethylsiloxane (PDMS) crosslinking solution. Due to the micro-nano hierarchies of the ZGS, the prepared ZIF-8@rGO@PDMS/PTFE (ZGPP) membranes feature a unique superhydrophobic surface, which results in a water–oil interface imbalance when a surfactant-stabilized water-in-oil emulsion comes into contact with the membrane surface. Under a low transmembrane pressure of 0.15 bar (15 kPa), such membranes show an excellent separation efficiency (~99.57%) and a high flux of 2254 L·m–2·h–1, even for surfactant-stabilized nanoscale water-in-toluene emulsions (with an average droplet size of 57 nm). This "contact demulsification" concept paves the way for developing next-generation demulsifying membranes for water-in-oil emulsion separation.

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References

[ 1 ] Ghaffar A, Chen C, Zhu X, Chen B. Underwater superoleophobic PVA‒GO nanofibrous membranes for emulsified oily water purification. Environ Ence Nano 2019;6(12):3723‒33. link1

[ 2 ] Zeng X, Qian L, Yuan X, Zhou C, Li Z, Cheng J, et al. Inspired by Stenocara beetles: from water collection to high-efficiency water-in-oil emulsion separation. ACS Nano 2017;11(1):760‒9. link1

[ 3 ] Zhang W, Liu N, Cao Y, Lin X, Liu Y, Feng L. Superwetting porous materials for wastewater treatment: from immiscible oil/water mixture to emulsion separation. Adv Mater Interfaces 2017;4(10):1600029. link1

[ 4 ] Chen C, Chen S, Chen L, Yu Y, Weng D, Mahmood A, et al. Underoil superhydrophilic metal felt fabricated by modifying ultrathin fumed silica coatings for the separation of water-in-oil emulsions. ACS Appl Mater Interfaces 2020;12(24):27663‒71. link1

[ 5 ] Wei Y, Qi H, Gong X, Zhao S. Specially wettable membranes for oil‒water separation. Adv Mater Interfaces 2018;5(23):1800576. link1

[ 6 ] Cheryan M, Rajagopalan N. Membrane processing of oily streams. Wastewater treatment and waste reduction. J Membr Sci 1998;151(1):13‒28. link1

[ 7 ] Tummons E, Han Q, Tanudjaja HJ, Hejase CA, Chew JW, Tarabara VV. Membrane fouling by emulsified oil: a review. Sep Purif Technol 2020;248:116919. link1

[ 8 ] Zhang W, Shi Z, Zhang F, Liu X, Jin J, Jiang L. Superhydrophobic and superoleophilic PVDF membranes for effective separation of water-in-oil emulsions with high flux. Adv Mater 2013;25(14):2071‒6. link1

[ 9 ] Macedonio F, Drioli E. Membrane engineering for green process engineering. Engineering 2017;3(3):290‒8. link1

[10] Zhang G, Jin W, Xu N. Design and fabrication of ceramic catalytic membrane reactors for green chemical engineering applications. Engineering 2018;4(6):848‒60. link1

[11] Dai L, Huang K, Xia Y, Xu Z. Two-dimensional material separation membranes for renewable energy purification, storage, and conversion. Green Energy Environ 2021;6(2):193‒211. link1

[12] Wang F, Lei S, Xue M, Ou J, Li W. In situ separation and collection of oil from water surface via a novel superoleophilic and superhydrophobic oil containment boom. Langmuir 2014;30(5):1281‒9. link1

[13] Huang Y, Xiao C, Huang Q, Liu H, Guo Z, Sun K. Robust preparation of tubular PTFE/FEP ultrafine fibers-covered porous membrane by electrospinning for continuous highly effective oil/water separation. J Membr Sci 2018;568:87‒96. link1

[14] Xue Z, Wang S, Lin L, Chen L, Liu M, Feng L, et al. A novel superhydrophilic and underwater superoleophobic hydrogel-coated mesh for oil/water separation. Adv Mater 2011;23(37):4270‒3. link1

[15] Yong J, Huo J, Chen F, Yang Q, Hou X. Oil/water separation based on natural materials with super-wettability: recent advances. Phys Chem Chem Phys 2018;20(39):25140‒63. link1

[16] Liu YQ, Zhang YL, Fu XY, Sun HB. Bioinspired underwater superoleophobic membrane based on a graphene oxide coated wire mesh for efficient oil/water separation. ACS Appl Mater Interfaces 2015;7(37):20930‒6. link1

[17] Lin X, Heo J, Jeong H, Choi M, Chang M, Hong J. Robust superhydrophobic carbon nanofiber network inlay-gated mesh for water-in-oil emulsion separation with high flux. J Mater Chem A 2016;4(46):17970‒80. link1

[18] Yin X, Wang Z, Shen Y, Mu P, Zhu G, Li J. Facile fabrication of superhydrophobic copper hydroxide coated mesh for effective separation of water-in-oil emulsions. Sep Purif Technol 2020;230:115856. link1

[19] Kang H, Zhang X, Li L, Zhao B, Ma F, Zhang J. Polydopamine and poly(dimethylsiloxane) modified superhydrophobic fiberglass membranes for efficient water-in-oil emulsions separation. J Colloid Interface Sci 2020;559:178‒85. link1

[20] Huang M, Si Y, Tang X, Zhu Z, Ding B, Liu L, et al. Gravity driven separation of emulsified oil‒water mixtures utilizing in situ polymerized superhydrophobic and superoleophilic nanofibrous membranes. J Mater Chem A 2013;1(45):14071‒4. link1

[21] Wang X, Xiao C, Liu H, Chen M, Hao J, Wu Y. A study on fabrication of PVDF‒HFP/PTFE blend membranes with controllable and bicontinuous structure for highly effective water-in-oil emulsion separation. RSC Adv 2018;8 (49):27754‒62. link1

[22] Chen L, Si Y, Zhu H, Jiang T, Guo Z. A study on the fabrication of porous PVDF membranes by in-situ elimination and their applications in separating oil/water mixtures and nano-emulsions. J Membr Sci 2016;520:760‒8. link1

[23] Wang X, Xiao C, Liu H, Huang Q, Hao J, Fu H. Poly(vinylidene fluoride‒hexafluoropropylene) porous membrane with controllable structure and applications in efficient oil/water separation. Materials 2018;11(3):443. link1

[24] Chen R, Xu J, Li S, Li Q, Wu H, He Q, et al. Multiscale-structured superhydrophobic/superoleophilic SiO2 composite poly(ether sulfone) membranes with high efficiency and flux for water-in-oil emulsions separation under harsh conditions. New J Chem 2020;44(10):3824‒7. link1

[25] Lei T, Lu D, Xu Z, Xu W, Liu J, Deng X, et al. 2D→3D conversion of superwetting mesh: a simple but powerful strategy for effective and efficient oil/water separation. Sep Purif Technol 2020;242:116244. link1

[26] Ji D, Xiao C, An S, Liu H, Chen K, Hao J, et al. Preparation of PSF/FEP mixed matrix membrane with super hydrophobic surface for efficient water-in-oil emulsion separation. RSC Adv 2018;8(18):10097‒106. link1

[27] Gao N, Xu ZK. Ceramic membranes with mussel-inspired and nanostructured coatings for water-in-oil emulsions separation. Sep Purif Technol 2019;212:737‒46. link1

[28] Gu J, Xiao P, Chen J, Liu F, Huang Y, Li G, et al. Robust preparation of superhydrophobic polymer/carbon nanotube hybrid membranes for highly effective removal of oils and separation of water-in-oil emulsions. J Mater Chem A 2014;2(37):15268‒72. link1

[29] Wu J, Li H, Lai X, Chen Z, Zeng X. Superhydrophobic polydimethylsiloxane@multiwalled carbon nanotubes membrane for effective water-in-oil emulsions separation and quick deicing. Ind Eng Chem Res 2019;58(20):8791‒9. link1

[30] Yang J, Li HN, Chen ZX, He A, Zhong QZ, Xu ZK. Janus membranes with controllable asymmetric configurations for highly efficient separation of oilin- water emulsions. J Mater Chem A 2019;7(13):7907‒17. link1

[31] An YP, Yang J, Yang HC, Wu MB, Xu ZK. Janus membranes with charged carbon nanotube coatings for deemulsification and separation of oil-in-water emulsions. ACS Appl Mater Interfaces 2018;10(11):9832‒40. link1

[32] Shi Z, Zhang W, Zhang F, Liu X, Wang D, Jin J, et al. Ultrafast separation of emulsified oil/water mixtures by ultrathin free-standing single-walled carbon nanotube network films. Adv Mater 2013;25(17):2422‒7. link1

[33] Sun T, Feng L, Gao X, Jiang L. Bioinspired surfaces with special wettability. Acc Chem Res 2005;38(8):644‒52. link1

[34] Pan J, Xiao C, Huang Q, Liu H, Zhang T. ECTFE hybrid porous membrane with hierarchical micro/nano-structural surface for efficient oil/water separation. J Membr Sci 2017;524:623‒30. link1

[35] Yuan X, Li W, Zhu Z, Han N, Zhang X. Thermo-responsive PVDF/PSMA composite membranes with micro/nanoscale hierarchical structures for oil/ water emulsion separation. Colloids Surf A 2017;516:305‒16. link1

[36] Wei Y, Xie Z, Qi H. Superhydrophobic‒superoleophilic SiC membranes with micro-nano hierarchical structures for high-efficient water-in-oil emulsion separation. J Membr Sci 2020;601:117842. link1

[37] Gu J, Fan H, Li C, Caro J, Meng H. Robust superhydrophobic/superoleophilic wrinkled microspherical MOF@rGO composites for efficient oil‍‒‍water separation. Angew Chem Int Ed Engl 2019;58(16):5297‒301. link1

[38] Mao H, Li SH, Zhang AS, Xu LH, Lu JJ, Zhao ZP. Novel MOF-capped halloysite nanotubes/PDMS mixed matrix membranes for enhanced n-butanol permselective pervaporation. J Membr Sci 2020;595:117543. link1

[39] Zhang WD, Sun W, Yang J, Ren ZQ. The study on pervaporation behaviors of dilute organic solution through PDMS/PTFE composite membrane. Appl Biochem Biotechnol 2010;160(1):156‒67. link1

[40] Zhang N, Wu H, Li F, Dong S, Yang L, Ren Y, et al. Heterostructured filler in mixed matrix membranes to coordinate physical and chemical selectivities for enhanced CO2 separation. J Membr Sci 2018;567:272‒80. link1

[41] Zhu Y, Wang J, Zhang F, Gao S, Wang A, Fang W, et al. Zwitterionic nanohydrogel grafted PVDF membranes with comprehensive antifouling property and superior cycle stability for oil-in-water emulsion separation. Adv Funct Mater 2018;28(40):1804121. link1

[42] Zhang WH, Yin MJ, Zhao Q, Jin CG, Wang N, Ji S, et al. Graphene oxide membranes with stable porous structure for ultrafast water transport. Nat Nanotechnol 2021;16(3):337‒43. link1

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