Abstract
Develo** high-performance, low-cost and large-scale absorbent materials is crucial for the treatment of water pollution caused by pollutants leakage and emission. Herein, superelastic and superhydrophobic thermoplastic polymeric nanofibrous aerogels (NFAs) were created for removal pollutants from water by using a facile and effective method. Poly(vinyl alcohol-co-ethylene) (EVOH) nanofibers fabricated by mass-production techniques were used to construct three-dimensional NFAs through combing freeze-drying process and cross-linking treatment. The optimal parameters for creating EVOH NFAs with good formability and resilience, including composition and ratio of dispersion, dosage of cross-linking agent were obtained through experiments. EVOH nanofibers bonded with each other by glutaraldehyde under acidic conditions to from fibrous network structure in EVOH NFAs. The silane-coated EVOH NFAs were prepared through further modification with vapor-phase methyltrichlorosilane. The deposition of siloxane improved mechanical strength and decreased plastic deformation after 500 cyclic compressions. An asperate fibrous and granular siloxane coating was deposited on the surface of EVOH NFAs. The surface water contact angle increased from 104.4° ± 4.0° to 152.7° ± 1.9°, wettability of NFAs transitioned to being superhydrophobic. Silane-coated EVOH NFAs exhibited superior absorption capacity (40–92 g/g) for a variety of organic pollutants. The organic pollutants would be collected and the sorbents could be reused after distillation or squeezing. A successful scale-up of such materials open up a new insight into design polymeric aerogels in low-cost and large-scale with substantial industrial water purification applications.
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Y.Q. Wang, Y. He, Y. Fan, H.J. Li, H. Yu, J. Yu, Y.L. Nie, S.H. Wang, A robust anti-fouling multifunctional aerogel inspired by seaweed for efficient water purification. Sep. Purif. Technol. 259, 118153 (2021)
F. Wang, J.W. Dai, L.Q. Huang, Y. Si, J.Y. Yu, B. Ding, Biomimetic and superelastic slica nanofibrous aerogels with rechargeable bactericidal function for antifouling water disinfection. ACS Nano 14(7), 8975–8984 (2020)
Z.C. Yin, Y.P. Pan, M.T. Bao, Y. Li, Superhydrophobic magnetic cotton fabricated under low carbonization temperature for effective oil/water separation. Sep. Purif. Technol. 266, 118535 (2021)
J.W. Xue, L. Zhu, X. Zhu, H. Li, C. Ma, S.F. Yu, D.F. Sun, F.J. **a, Q.Z. Xue, Tetradecylamine-MXene functionalized melamine sponge for effective oil/water separation and selective oil adsorption. Sep. Purif. Technol. 259, 118106 (2021)
J.W. Lu, D.D. Xu, J.K. Wei, S. Yan, R. **ao, Superoleophilic and flexible thermoplastic polymer nanofiber aerogels for removal of oils and organic solvents. ACS Appl. Mater. Interfaces 9(30), 25533–25541 (2017)
H.Z. Liu, B.Y. Geng, Y.F. Chen, H.Y. Wang, Review on the aerogel-type oil sorbents derived from nanocellulose. ACS Sustain. Chem. Eng. 5(1), 49–66 (2017)
B. Tansel, M. Lee, Removal of crude oil from highly contaminated natural surfaces with corexit dispersants. J. Environ. Manage. 247, 363–370 (2019)
S.S. Long, Y.C. Feng, Y.Z. Liu, L.L. Zheng, L.H. Gan, J. Liu, X.H. Zeng, M.N. Long, Renewable and robust biomass carbon aerogel derived from deep eutectic solvents modified cellulose nanofiber under a low carbonization temperature for oil-water separation. Sep. Purif. Technol. 254, 117577 (2021)
R.C. Prince, R.R. Lessard, J.R. Clark, Bioremediation of marine oil spills. Oil Gas Sci. Technol. 151(4), 495–512 (2004)
A. Jaggi, J.R. Radovic, L.R. Snowdon, S.R. Larter, T.B.P. Oldenburg, Composition of the dissolved organic matter produced during in situ burning of spilled oil. Org. Geochem. 138, 103926 (2019)
Y.S. Lee, Y.T. Lim, W.S. Choi, One-step synthesis of environmentally friendly superhydrophilic and superhydrophobic sponges for oil/water separation. Materials 12(7), 1182 (2019)
S.Y. Liu, J.T. Wang, Eco-friendly and facile fabrication of polyimide mesh with underwater superoleophobicity for oil/water separation via polydopamine/starch hybrid decoration. Sep. Purif. Technol. 250, 117228 (2020)
Z.X. Wang, M.C. Han, J. Zhang, F. He, S.Q. Peng, Y.X. Li, Investigating and significantly improving the stability of tannic acid (TA)-aminopropyltriethoxysilane (APTES) coating for enhanced oil-water separation. J. Membr. Sci. 593, 117383 (2020)
H.C. Bi, X. **e, K.B. Yin, Y.L. Zhou, S. Wan, L.B. He, F. Xu, F. Banhart, L.T. Sun, R.S. Ruoff, Spongy graphene as a highly efficient and recyclable sorbent for oils and organic solvents. Adv. Funct. Mater. 22, 4421–4425 (2012)
P.K. Huang, F. Wu, B. Shen, X.H. Ma, Y.Q. Zhao, M.H. Wu, J. Wang, Z.H. Liu, H.B. Luo, W.G. Zheng, Bio-inspired lightweight polypropylene foams with tunable hierarchical tubular porous structure and its application for oil-water separation. Chem. Eng. J. 370, 1322–1330 (2019)
Y.Y. Tian, H.Z. Ma, Solvent-free green preparation of reusable EG-PVDF foam for efficient oil-water separation. Sep. Purif. Technol. 253, 117506 (2020)
Y.C. Yu, X.L. Shi, L. Liu, J.M. Yao, Highly compressible and durable superhydrophobic cellulose aerogels for oil/water emulsion separation with high flux. J. Mater. Sci. 56(3), 2763–2776 (2021)
C.X. Tang, P. Brodie, Y.Z. Li, N.J. Grishkewich, M. Brunsting, K.C. Tam, Shape recoverable and mechanically robust cellulose aerogel beads for efficient removal of copper ions. Chem. Eng. J. 392, 124821 (2020)
X.D. Cheng, S.Y. Zhu, Y.L. Pan, Y.R. Deng, L. Shi, L.L. Gong, Fire retardancy and thermal behaviors of Cellulose nanofiber/zinc borate aerogel. Cellulose 27, 7463–7474 (2020)
P.Y. Hu, J. Lyu, C. Fu, W.B. Gong, J.H. Liao, W.B. Lu, Y.P. Chen, X.T. Zhang, Multifunctional aramid nanofiber/carbon nanotube hybrid aerogel films. ACS Nano 14(1), 688–697 (2020)
J. Zhu, S.H. Lv, T.H. Yang, T. Huang, H. Yu, Q.H. Zhang, M.F. Zhu, Facile and green strategy for designing ultralight, flexible, and multifunctional PVA nanofiber-based aerogels. Adv. Sustain. Syst. 4, 1900141 (2020)
Z.M. An, C.S. Ye, R.B. Zhang, P. Zhou, Flexible and recoverable SiC nanofiber aerogels for electromagnetic wave absorption. Ceram. Int. 45(17), 22793–22801 (2019)
Y. Si, J.Y. Yu, X.M. Tang, J.L. Ge, B. Ding, Ultralight nanofibre-assembled cellular aerogels with superelasticity and multifunctionality. Nat. Commun. 5, 5802 (2014)
Q.X. Fu, L.F. Liu, Y. Si, J.Y. Yu, B. Ding, Shapeable, underwater superelastic, and highly phosphorylated nanofibrous aerogels for large-capacity and high-throughput protein separation. ACS Appl. Mater. Interfaces 11(47), 44874–44885 (2019)
Z.C. Qian, Z. Wang, Y. Chen, S.R. Tong, M.F. Ge, N. Zhao, J. Xu, Superelastic and ultralight polyimide aerogels as thermal insulators and particulate air filters. J. Mater. Chem. A 6(3), 828–832 (2018)
J. Zhu, G. Sun, Facile fabrication of hydrophilic nanofibrous membranes with an immobilized metal-chelate affinity complex for selective protein separation. ACS Appl. Mater. Interfaces 6(2), 925–932 (2014)
M.F. Li, R. **ao, G. Sun, Formation and morphology development of poly(butylene terephthalate) nanofibers from poly(butylene terephthalate)/cellulose acetate butyrate immiscible blends. Polym. Eng. Sci. 51(5), 835–842 (2011)
P.P. Zhang, D.D. Xu, R. **ao, Morphology development and size control of PA6 nanofibers from PA6/CAB polymer blends. J. Appl. Polym. Sci. 132, 42184 (2015)
M.J. Zhu, G.B. Xu, M.F. Yu, Y.B. Liu, R. **ao, Preparation, properties, and application of polypropylene micro/nanofiber membranes. Polym. Adv. Technol. 23(2), 247–254 (2012)
Q.Z. Liu, J.H. Chen, T. Mei, X.W. He, W.B. Zhong, K. Liu, W.W. Wang, Y.D. Wang, M.F. Li, D. Wang, A facile route to the production of polymeric nanofibrous aerogels for environmentally sustainable applications. J. Mater. Chem. A 6(8), 3692–3704 (2018)
Y.Z. Lin, L.B. Zhong, S. Dou, Z.D. Shao, Q. Liu, Y.M. Zheng, Facile synthesis of electrospun carbon nanofiber/graphene oxide composite aerogels for high efficiency oils absorption. Environ. Int. 128, 37–45 (2019)
Y.Q. Lu, Z.X. Niu, W.Z. Yuan, Multifunctional magnetic superhydrophobic carbonaceous aerogel with micro/nano-scale hierarchical structures for environmental remediation and energy storage. Appl. Surf. Sci. 480, 851–860 (2019)
H.Z. Sai, R. Fu, L. **ng, J.H. **ang, Z.Y. Li, F. Li, T. Zhang, Surface modification of bacterial cellulose aerogels’ web-like skeleton for oil/water separation. ACS Appl. Mater. Interfaces 7(13), 7373–7381 (2015)
K. Lee, J.S. Jur, D.H. Kim, G.N. Parsons, Mechanisms for hydrophilic/hydrophobic wetting transitions on cellulose cotton fibers coated using Al2O3 atomic layer deposition. J. Vac. Sci. Technol. A 30(1), 1–7 (2012)
J.T. Korhonen, M. Kettunen, R.H.A. Ras, O. Ikkala, Hydrophobic nanocellulose aerogels as floating, sustainable, reusable, and recyclable oil absorbents. ACS Appl. Mater. Interfaces 3(6), 1813–1816 (2011)
J.W. Lu, S. Yan, W. Song, K.I. Jacob, R. **ao, Construction and characterization of versatile flexible composite nanofibrous aerogels based on thermoplastic polymeric nanofibers. J. Mater. Sci. 55(19), 8155–8169 (2020)
A.W. Chan, R.A. Whitney, R.J. Neufeld, Kinetic controlled synthesis of pH-responsive network alginate. Biomacromol 9(9), 2536–2545 (2008)
M.A. Shirgholami, M.S. Khalil-Abad, R. Khajavi, M.E. Yazdanshenas, Fabrication of superhydrophobic polymethylsilsesquioxane nanostructures on cotton textiles by a solution-immersion process. J. Colloid Interface Sci. 359(2), 530–535 (2011)
Q.F. Zheng, Z.Y. Cai, S.Q. Gong, Green synthesis of polyvinyl alcohol (PVA)-cellulose nanofibril (CNF) hybrid aerogels and their use as superabsorbents. J. Mater. Chem. A 2(9), 3110–3118 (2014)
G.R.J. Artus, S. Jung, J. Zimmermann, H.P. Gautschi, K. Marquardt, S. Seeger, Silicone nanofilaments and their application as superhydrophobic coating. Adv. Mater. 18(20), 2758–2762 (2006)
Y.T. Wang, L.Y. Chen, H. Cheng, B.J. Wang, X.L. Feng, Z.P. Mao, X.F. Sui, Mechanically flexible, waterproof, breathable cellulose/polypyrrole/polyurethane composite aerogels as wearable heaters for personal thermal management. Chem. Eng. J. 402, 126222 (2020)
H. Cheng, Y.Z. Li, B.J. Wang, Z.P. Mao, H. Xu, L.P. Zhang, Y. Zhong, X.F. Sui, Chemical crosslinking reinforced flexible cellulose nanofiber-supported cryogel. Cellulose 25(1), 573–582 (2018)
Y. Si, X.Q. Wang, L.Y. Dou, J.Y. Yu, B. Ding, Ultralight and fire-resistant ceramic nanofibrous aerogels with temperature-invariant superelasticity. Sci. Adv. 4, eaas8925 (2018)
H.W. Liang, Q.F. Guan, L.F. Chen, Z. Zhu, W.J. Zhang, S.H. Yu, Macroscopic-scale template synthesis of robust carbonaceous nanofiber hydrogels and aerogels and their applications. Angew. Chem. Int. Ed. 51(21), 5101–5105 (2012)
M. Xu, D.N. Futaba, T. Yamada, M. Yumura, K. Hata, Carbon nanotubes with temperature-invariant viscoelasticity from -196° to 1000°C. Science 330(6009), 1364–1368 (2010)
Y. Liu, Y.P. Zhang, T.G. Liao, L. Gao, M. Wang, X. Xu, X.X. Yang, H. Liu, Boron nitride-nanosheet enhanced cellulose nanofiber aerogel with excellent thermal management properties. Carbohydr. Polym. 241, 116425 (2020)
W.B. Zhang, Y.Z. Zhu, X. Liu, D. Wang, J.Y. Li, L. Jiang, J. **, Salt-induced fabrication of superhydrophilic and underwater superoleophobic PAA-g-PVDF membranes for effective separation of oil-in-water emulsions. Angew. Chem. Int. Ed. 53(3), 856–860 (2014)
F. Jiang, Y.L. Hsieh, Amphiphilic superabsorbent cellulose nanofibril aerogels. J. Mater. Chem. A 2(18), 6337–6342 (2014)
Y.P. Su, Z.Y. Li, H.J. Zhou, S.H. Kang, Y.X. Zhang, C.Z. Yu, G.Z. Wang, Ni/carbon aerogels derived from water induced self-assembly of Ni-MOF for adsorption and catalytic conversion of oily wastewater. Chem. Eng. J. 402, 126205 (2020)
A. Mulyadi, Z. Zhang, Y.L. Deng, Fluorine-free oil absorbents made from cellulose nanofibril aerogels. ACS Appl. Mater. Interfaces 8(4), 2732–2740 (2016)
A. Li, H.X. Sun, D.Z. Tan, W.J. Fan, S.H. Wen, X.J. Qing, G.X. Li, S.Y. Li, W.Q. Deng, Superhydrophobic conjugated microporous polymers for separation and adsorption. Energy Environ. Sci. 4(6), 2062–2065 (2011)
P. Song, J.W. Cui, J. Di, D.B. Liu, M.Z. Xu, B.J. Tang, Q.S. Zeng, J. **ong, C.D. Wang, Q. He, L.X. Kang, J.D. Zhou, R.H. Duan, B.B. Chen, S.S. Guo, F.C. Liu, J. Shen, Z. Liu, Carbon microtube aerogel derived from kapok fiber: an efficient and recyclable sorbent for oils and organic solvents. ACS Nano 14(1), 595–660 (2020)
H.C. Bi, Z.Y. Yin, X.H. Cao, X. **e, C.L. Tan, X. Huang, B. Chen, F.T. Chen, Q.L. Yang, X.Y. Bu, X.H. Lu, L.T. Sun, H. Zhang, Carbon fiber aerogel made from raw cotton: a novel, efficient and recyclable sorbent for oils and organic solvents. Adv. Mater. 25(41), 5916–5921 (2013)
Acknowledgements
This work was supported by National Natural Science Foundation of China (Nos. 51803081 and No. 20874010) and Changzhou Sci&Tech Program (No .CJ20210042)
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The funded was provided by National Natural Science Foundation of China (Nos. 51803081, 20874010), Changzhou Sci&Tech Program (No. CJ20210042).
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Supplementary data to this article can be found online at Figs. S1-S12 and Tables S1-S2 showing contact angles, nanofibrous suspensions, frozen nanofibrous suspensions, photographs of EVOH NFAs with different GA contents, mechanisms of cross-linking, ATR-FTIR spectra, EVOH NFAs after releasing loading, proposed silanization reaction, XPS spectra, SEM images, stress-strain curves, physical properties and sorption capacities of various sorbents. (DOCX 6384 kb)
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Lu, J., Jiang, Y., **ao, R. et al. Chemical Vapor Deposition Based Superelastic and Superhydrophoboic Thermoplastic Polymeric Nanofibrous Aerogels for Water Purification. J Inorg Organomet Polym 32, 2975–2985 (2022). https://doi.org/10.1007/s10904-022-02330-z
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DOI: https://doi.org/10.1007/s10904-022-02330-z