Graphene-Coated Poly(ethylene terephthalate) Nonwoven Hollow

Apr 22, 2019 - Hence, these filtration materials have much limitation to deal with .... then gradually tilting the PGNW until the water droplet began ...
0 downloads 0 Views 12MB Size
Download PDF
This is an open access article published under an ACS AuthorChoice License, which permits copying and redistribution of the article or any adaptations for non-commercial purposes.

Article Cite This: ACS Omega 2019, 4, 7237−7245

http://pubs.acs.org/journal/acsodf

Graphene-Coated Poly(ethylene terephthalate) Nonwoven Hollow Tube for Continuous and Highly Effective Oil Collection from the Water Surface Tai Zhang,†,‡ Changfa Xiao,*,†,‡ Jian Zhao,†,‡ Jinxue Cheng,‡ Kaikai Chen,†,‡ and Yan Huang‡ †

School of Textile Science and Engineering and ‡State Key Laboratory of Separation Membranes and Membrane Processes, Tianjin Polytechnic University, Tianjin 300387, China

ACS Omega 2019.4:7237-7245. Downloaded from pubs.acs.org by 31.40.211.73 on 04/22/19. For personal use only.

S Supporting Information *

ABSTRACT: Graphene (GE) has attracted significant attention on account of its unique structure and superior performance, arousing a new research field for materials science. Herein, a novel GE-coated poly(ethylene terephthalate) nonwoven (PGNW) hollow tube (PGNW-T) was fabricated for continuous and highly effective oil collection from the water surface. The PGNW was prepared via a dip-spray coating method, which possessed superhydrophobicity−superoleophilicity and could absorb a variety of oils or organic solvents with the absorption capacity (Q) value of 18−34 times its own weight. Then, PGNW-T was obtained through winding the PGNW on the surface of a porous polypropylene hollow tube. As-prepared PGNW-T was competent for dynamic oil collection with high flux (18 799.94 L/m2 h), outstanding separation efficiency (97.14%), and excellent recyclability (>96% after 10 cycles) from the oil/water mixture. In particular, a miniature device based on as-prepared PGNW-T was developed for continuous thin oil film collection, which could dynamically “catch up” floated oils or organic solvents from the water surface. Finally, our strategy is extremely facile to scale up, showing its huge potential application in practical oil-spill remediation.

1. INTRODUCTION Over the past few decades, along with the rapid development of industry, oil spill and chemical leakage accidents have a catastrophic impact on the aquatic system and pose a severe threat to human lives.1,2 Consequently, the development of oilspill removal technology has attracted tremendous attention from both research community and general public. There are many traditional methods, such as skimmers,3 in situ burning,4 solidifiers,5 bioremediation,6 dispersants,7 and using absorbents,8 to deal with large amounts of oil spill. Among these technologies, porous absorbents have been frequently used for oil-spill remediation owing to their low cost and eco-friendly treating process. Unfortunately, these kinds of absorbents, including bentonite, zeolite, corn stalk, and activated carbon,9−11 still have limitations for practical oil-spill cleanup including low selectivity (absorb both oil and water), inferior absorption capacity, and poor recyclability. To overcome the drawbacks of traditional absorbents, numerous efforts have been carried out to develop new suoperhydrophobic−superoleophilic porous absorbents, including metal oxides,12 porous boron nitride,13 carbon based sponge,14 and swellable oleophilic polymer absorbents.15 In general, they possessed excellent oil absorption capacity (Q) and could selectively absorb oil while repelling water, thus showing good performance for oil collection. However, they could not absorb oil anymore when the absorbents reached the © 2019 American Chemical Society

Q value and have to stop and desorb inner oils by squeezing or distillation for reuse. Consequently, this noncontinuous process is still a relatively ineffective method along with the time-consuming and cost-expensive process. More recently, filtration materials with superhydrophobic−superoleophilic properties, such as metallic mesh16,17and polymeric membranes,18,19 have aroused considerable attention for oil/water separation owing to their continuous separation ability and outstanding separation efficiency, but they often suffered low flux, high energy consuming, and easy surface fouling due to their small pore size (96% after 10 cycles), the exceptional corrosion resistance ability was also provided for practical application. Furthermore, a miniature device based on PGNW-T was developed for continuous thin oil film collection, which shows excellent collection ability for various floated oils and organic solvents. Our strategy is easy to scale up and may provide a new solution for dealing with large-area oil spill remediation.

Reusability under different environment conditions (including acid, alkali, or salt conditions) was also extremely important in practical application. To investigate the recyclability of PGNW-T, the oil/water separation test for kerosene/distilled water, kerosene/1 mol/L HCl solution, kerosene/1 mol/L NaOH solution, kerosene/1 mol/L NaCl solution was repeated 10 times, respectively, and the oil/water separation efficiency was calculated for each group of test. As shown in Figure 10, there is no significant decrease of oil/

Figure 10. Reusability of PGNW-T under different environment conditions.

water separation efficiency during 10 cycles even under strong acid, strong alkali, and salt conditions. The separation efficiencies of PGNW-T all remained above 96% after 10 cycles, and the stable oil collection ability of PGNW-T was contributed by the strong interfacial bonding between the GE sheet and PET nonwoven. The result showed not only the excellent recyclability but also superior corrosion resistance ability of PGNW-T. The above results show the outstanding oil/water separation ability of PGNW-T, but in practical oil-spill accidents, the oil spill generally spread around very fast and a thin oil film was easily formed on the water surface. In particular, this thin oil film needs to be collected immediately to alleviate further detriment. Apparently, the vertical insertion of PGNW-T to treat oil spills is a relatively less-effective method because of its limited contact area with oils. If PGNW-T could float on the water surface horizontally and move freely on the water surface for oil spill treatment, its valid contact area with oils could be dramatically improved, and that must make our PGNW-T more efficacious and more flexible to deal with the thin oil film on the water surface. Herein, a miniature device based on PGNW-T was developed to continuously collect thin oil films on the water surface, and its structure diagram is shown in Figure 11. A water tank (500 mm × 200 mm × 150 mm) which contained 9000 mL of water and 250 mL of kerosene spreading on its surface was employed to simulate actual oil spill on the water surface. Two PGNW-Ts were floated on the

3. EXPERIMENTAL DETAILS 3.1. Materials. GE (sheet size: 7−10 μm, 1−3 layer) and PET nonwoven (140 g/m2, thickness = 5 mm) were purchased from Xiamen Knano Graphene Technology Co., Ltd., Xiamen and Handan Hengyong Protective & Clean Products Co., Ltd., Handan, respectively. PVDF (Solef 6010) was obtained from Solvay Chemical Industry Co., Ltd., Shanghai. The PP hollow tube (diameter = 10 mm, wall thickness = 2 mm) was provided by Suzhou Wolong Plastic Product Co., Ltd., Suzhou. N,NDimethylacetamide (DMAc), N,N-dimethylformamide

Figure 11. Structure diagram of a continuous thin oil film collection device. 7242

DOI: 10.1021/acsomega.9b00428 ACS Omega 2019, 4, 7237−7245

ACS Omega

Article

Figure 12. Continuous thin oil film collection process by the miniature device.

treatment for 2 h to get a uniform GE dispersion. Then, 1 g of PVDF was dissolved in 50 mL of DMAc with vigorous stirring at 70 °C for 2 h to form a homogenous PVDF/DMAc solution. PET nonwoven was first cleaned by distilled water and then dried in a drum wind drying oven at 70 °C for 6 h to completely remove the moisture. The resultant PET nonwoven was dipped into the above-mentioned GE dispersion for 60 s and dried in the oven at 70 °C for 2 h, and GE-coated PET nonwoven was obtained. Repeat the dipping and drying process above for adjusting the amount of GE loading on PET nonwoven. To enhance the adhesion of the GE sheet on PET nonwoven, the above-mentioned PVDF/DMAc solution was then sprayed onto the PET nonwoven which underwent three times the dipping and drying process (GNW) using a spray gun (0.1 MPa compressed air gas, both sides were sprayed for 10 s), after drying in the drum wind drying oven at 60 °C for 48 h to allow the solvent to be removed completely, and PGNW was obtained. 3.3. Preparation of the PGNW Hollow Tube (PGNWT). A piece of as-prepared PGNW (100 mm × 100 mm) was wrapped on a porous PP hollow tube (150 mm), which was obtained by drilling the holes on the surface of the PP hollow tube (diameter of holes = 0.5 mm, spacing of each holes = 0.5 mm) through a bench drill, both sides of the PP hollow tube were reserved 30 mm nonporous area for joint connection. The edge of the PGNW wrapped on the PP hollow tube was sealed, and finally, PGNW-T was obtained. The preparation process of PGNW-T is shown in Figure 15. 3.4. Characterization. The morphology of the samples was observed by FESEM (S4800, Hitachi). WCA and OCA were measured on an optical contact angle meter (model DSA100, KRUSS) by dropping water and oil droplets (2 μL)

Figure 13. Separation efficiency of various oil and organic solvents by the miniature device.

(DMF), ethyl alcohol, and chloroform were purchased from Tianji Kermel Chemical Reagents Co., Ltd., Tianjin. Xylene, butyl acrylate, methyl methacrylate, benzene, toluene, and nonanol were obtained from Aladdin Reagent Co., Ltd., Shanghai. Kerosene and diesel were obtained from Tianjin Kailida Chemical Co., Ltd., Tianjin. Engine oil, palm oil, pump oil, and soybean oil were purchased from local store. All reagents were used as received without further purification. 3.2. Preparation of GE-Coated PET Nonwoven (PGNW). The fabrication process of PGNW is shown in Figure 14. Typically, 2 g of GE and 1000 mL of ethyl alcohol were mixed in a beaker and then subjected to ultrasonic

Figure 14. Scheme for the fabrication process of PGNW.

Figure 15. Scheme for the fabrication process of PGNW-T. 7243

DOI: 10.1021/acsomega.9b00428 ACS Omega 2019, 4, 7237−7245

ACS Omega

Article

Figure 16. Schematic diagram of the continuous oil/water separation apparatus based on PGNW-T.

onto the samples at ambient temperature, and five positions of each sample were measured. The surface chemistries of the samples were characterized by XPS (K-alpha, Thermo Scientific,); the C 1s peak at 284.5 eV was used for adjusting the binging energies. The Q value was measured by the following process: a piece of PGNW (0.2 g) was immersed into different oils or organic solvents (including engine oil, pump oil, soybean oil, palm oil, butyl acrylate, DMF, diesel, kerosene, and toluene) until saturation, then the saturated PGNW was placed on a strainer for 1 min, and finally weighed. The Q (g/g) value of PGNW was calculated according to eq 136−38 Q=

ms − mi mi

J=

(3)

where J is the oil flux (L/m2 h), V is the total volume of the collected oil (L), A is the effective contact area of PGNW-T with oils (m2), and T is the operation time (h). All of the experiments were performed in triplicate.

■

ASSOCIATED CONTENT

S Supporting Information *

The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsomega.9b00428. Surface wettability of pristine nonwoven and PGNW (Figure S1); the instantaneous sliding behavior of a water droplet (dyed with rhodamine B) on the surface of PGNW (Figure S2) (PDF) Continuous oil/water separation process using PGNWT (Movies S1−S4); the continuous thin oil film collection process by the miniature device (Movie S5) (ZIP)

(1)

where ms and mi are the weight of PGNW before and after absorption (g), respectively. 3.5. Continuous Oil/Water Separation Test of PGNWT. A continuous oil/water separation test via PGNW-T was conducted using a laboratory-scale experimental setup (Figure 16), and the dead-end vacuum-pressure filtration method was carried out as previously described.39 Briefly, 250 mL of oils (including kerosene, diesel, engine oil, and palm oil) was poured into a 500-mL measuring cylinder containing 250 mL of water, and then the mixture was kept stationary for 120 s to form a hierarchical oil/water mixture. A length of PGNW-T with one-end sealed was then dipped into the mixture, and then connected to a vacuum system (by suction flask, vacuum meter, valve and vacuum pump) for continuous oil collection under vacuum pressure (−5 kPa). Oil/water separation efficiency was calculated as in eq 2 V − Vw η= a × 100% Vb

V A×T

■

AUTHOR INFORMATION

Corresponding Author

*E-mail: (C. Xiao) [email protected]. ORCID

Changfa Xiao: 0000-0003-0614-7348 Jian Zhao: 0000-0002-0953-096X Notes

The authors declare no competing financial interest.

■

ACKNOWLEDGMENTS The authors gratefully acknowledge the research funding provided by the Industrial innovation project of TJOA (BHSF2017-01), National Natural Science Foundation of China (51673149), and National Science Foundation of Tianjin (17JCQNJC02700, Greenpathway-18JCYBJC43500).

(2)

where η is the oil/water separation efficiency (%), Vb is the volume of oil before separation (mL), Va is the volume of collected oil after separation (mL), and Vw is the volume of collected water after separation (mL). To determine the oil flux of PGNW-T during the separation process, oils were continuously poured into a cylinder so that PGNW-T could be always submerged by oils (Figure 16). The permeation flux was calculated according to eq 3

■

REFERENCES

(1) Jernelöv, A. How to defend against future oil spills. Nature 2010, 466, 182−183.

7244

DOI: 10.1021/acsomega.9b00428 ACS Omega 2019, 4, 7237−7245

ACS Omega

Article

(22) Gao, Y.; Shi, W.; Wang, W.; Leng, Y.; Zhao, Y. Inkjet Printing Patterns of Highly Conductive Pristine Graphene on Flexible Substrates. Ind. Eng. Chem. Res. 2014, 53, 16777−16784. (23) Hao, J.; Xiao, C.; Zhang, T.; Zhao, J.; Fan, Z.; Chen, L. Preparation and Performance of PET-Braid-Reinforced Poly(vinylidene fluoride)/Graphene Hollow-Fiber Membranes. Ind. Eng. Chem. Res. 2016, 55, 2174−2182. (24) Bi, H.; Xie, X.; Yin, K.; Zhou, Y.; Wan, S.; Ruoff, R. S.; Sun, L. Highly enhanced performance of spongy graphene as an oil sorbent. J. Mater. Chem. A. 2014, 2, 1652−1656. (25) Wu, C.; Huang, X.; Wu, X.; Qian, R.; Jiang, P. Mechanically flexible and multifunctional polymer-based graphene foams for elastic conductors and oil-water separators. Adv. Mater. 2013, 25, 5658− 5662. (26) Dong, X.; Chen, J.; Ma, Y.; Wang, J.; Chanpark, M. B.; Liu, X.; Wang, L.; Huang, W.; Chen, P. Superhydrophobic and superoleophilic hybrid foam of graphene and carbon nanotube for selective removal of oils or organic solvents from the surface of water. Chem. Commun. 2012, 48, 10660−10662. (27) Zhang, X.; Liu, D.; Ma, Y.; Nie, J.; Sui, G. Super-hydrophobic graphene coated polyurethane (GN@PU) sponge with great oil-water separation performance. Appl. Surf. Sci. 2017, 422, 116−124. (28) Ge, B.; Zhang, Z.; Zhu, X.; Men, X.; Zhou, X.; Xue, Q. A graphene coated cotton for oil/water separation. Compos. Sci. Technol. 2014, 102, 100−105. (29) Liu, Y.; Ma, J.; Wu, T.; Wang, X.; Huang, G.; Liu, Y.; Qiu, H.; Li, Y.; Wang, W.; Gao, J. Cost-effective reduced graphene oxidecoated polyurethane sponge as a highly efficient and reusable oilabsorbent. ACS Appl. Mater. Interfaces 2013, 5, 10018−10026. (30) Ge, J.; Shi, L. A.; Wang, Y. C.; Zhao, H. Y.; Yao, H. B.; Zhu, Y. B.; Zhang, Y.; Zhu, H. W.; Wu, H. A.; Yu, S. H. Joule-heated graphene-wrapped sponge enables fast clean-up of viscous crude-oil spill. Nat. Nanotechnol. 2017, 12, 434−440. (31) Wang, Z.; Changfa, X.; Jian, Z.; Xiao, H. U.; Naiku, X. U. Preparation of Reduced Graphene Oxide-based Melamine Sponge and Its Absorption Properties. Chem. J. Chin. Univ. 2014, 35, 2410− 2417. (32) Zhang, J.; Seeger, S. Polyester Materials with Superwetting Silicone Nanofilaments for Oil/Water Separation and Selective Oil Absorption. Adv. Funct. Mater. 2011, 21, 4699−4704. (33) Cassie, A. B. D.; Baxter, S. Wettability of porous surfaces. Trans. Faraday Soc. 1944, 40, 546−551. (34) Ji, D.; Xiao, C.; An, S.; Liu, H.; Chen, K.; Hao, J.; Tai, Z. Preparation of PSF/FEP mixed matrix membrane with super hydrophobic surface for efficient water-in-oil emulsion separation. RSC Adv. 2018, 8, 10097−10106. (35) Zhao, J.; Han, P.; Quan, Q.; Shan, Y.; Zhang, T.; Wang, J.; Xiao, C. A convenient oil-water separator from polybutylmethacrylate/graphene-deposited polyethylene terephthalate nonwoven fabricated by a facile coating method. Prog. Org. Coat. 2018, 115, 181− 187. (36) Shang, B.; Wang, Y.; Peng, B.; Deng, Z. Bioinspired polydopamine particles-assisted construction of superhydrophobic surfaces for oil/water separation. J. Colloid Interface Sci. 2016, 482, 240−251. (37) Wang, Y.; Shang, B.; Hu, X.; Bo, P.; Deng, Z. Temperature Control of Mussel-Inspired Chemistry toward Hierarchical Superhydrophobic Surfaces for Oil/Water Separation. Adv. Mater. Interfaces 2016, 4, No. 1600727. (38) Li, J.; Yan, L.; Tang, X.; Feng, H.; Hu, D.; Zha, F. Robust Superhydrophobic Fabric Bag Filled with Polyurethane Sponges Used for Vacuum-Assisted Continuous and Ultrafast Absorption and Collection of Oils from Water. Adv. Mater. Interfaces 2016, 3, No. 1500770. (39) Zhang, T.; Xiao, C. F.; Hao, J. Q.; Zhao, J.; Fan, Z. W.; Chen, K. K. Studies on Nonwoven Fabric Reinforced PVDF/GE Oilabsorptive Composite Membrane. Acta Polym. Sin. 2016, 9, 1198− 1205.

(2) Ma, Q.; Cheng, H.; Fane, A. G.; Wang, R.; Zhang, H. Recent Development of Advanced Materials with Special Wettability for Selective Oil/Water Separation. Small 2016, 12, 2186−2202. (3) Broje, V.; Keller, A. A. Improved Mechanical Oil Spill Recovery Using an Optimized Geometry for the Skimmer Surface. Environ. Sci. Technol. 2006, 40, 7914−7918. (4) Aurell, J.; Gullett, B. K. Aerostat sampling of PCDD/PCDF emissions from the gulf oil spill in situ burns. Environ. Sci. Technol. 2010, 44, 9431−9437. (5) Rosales, P. I.; Suidan, M. T.; Venosa, A. D. A laboratory screening study on the use of solidifiers as a response tool to remove crude oil slicks on seawater. Chemosphere 2010, 80, 389−395. (6) Swannell, R. P.; Lee, K.; Mcdonagh, M. Field evaluations of marine oil spill bioremediation. Microbiol. Rev. 1996, 60, 342−365. (7) Kujawinski, E. B.; Soule, M. C. K.; Valentine, D. L.; Boysen, A. K.; Longnecker, K.; Redmond, M. C. Fate of Dispersants Associated with the Deepwater Horizon Oil Spill. Environ. Sci. Technol. 2011, 45, 1298−1306. (8) Chung, C.-H.; Liu, W.-C.; Hong, J.-L. Superhydrophobic Melamine Sponge Modified by Cross-Linked Urea Network as Recyclable Oil Absorbent Materials. Ind. Eng. Chem. Res. 2018, 57, 8449−8459. (9) Ahmad, A. L.; Sumathi, S.; Hameed, B. H. Residual oil and suspended solid removal using natural adsorbents chitosan, bentonite and activated carbon: A comparative study. Chem. Eng. J. 2005, 108, 179−185. (10) Rajaković-Ognjanović, V.; Aleksić, G.; Lj, R. Governing factors for motor oil removal from water with different sorption materials. J. Hazard. Mater. 2008, 154, 558−563. (11) Husseien, M.; Amer, A. A.; Elmaghraby, A.; Hamedallah, N. A comprehensive characterization of corn stalk and study of carbonized corn stalk in dye and gas oil sorption. J. Anal. Appl. Pyrolysis 2009, 86, 360−363. (12) Guo, Z.-G.; Liu, W. M. Superhydrophobic spiral Co3O4 nanorod arrays. Appl. Phys. Lett. 2007, 90, No. 193108. (13) Lei, W.; Portehault, D.; Liu, D.; Qin, S.; Chen, Y. Porous boron nitride nanosheets for effective water cleaning. Nat. Commun. 2016, 4, No. 1777. (14) Sun, H.; Li, A.; Zhu, Z.; Liang, W.; Zhao, X.; La, P.; Deng, W. Superhydrophobic activated carbon-coated sponges for separation and absorption. ChemSusChem 2013, 6, 1057−1062. (15) Yuan, X.; Chung, T. C. M. Novel Solution to Oil Spill Recovery: Using Thermodegradable Polyolefin Oil Superabsorbent Polymer (Oil−SAP). Energy Fuels 2012, 26, 4896−4902. (16) Jiang, B.; Zhang, H.; Zhang, L.; Sun, Y.; Xu, L.; Sun, Z.; Gu, W.; Chen, Z.; Yang, H. Novel One-Step, in Situ Thermal Polymerization Fabrication of Robust Superhydrophobic Mesh for Efficient Oil/ Water Separation. Ind. Eng. Chem. Res. 2017, 56, 11817−11826. (17) Li, J.; Xu, C.; Guo, C.; Tian, H.; Zha, F.; Guo, L. Underoil superhydrophilic desert sand layer for efficient gravity-directed waterin-oil emulsions separation with high flux. J. Mater. Chem. A. 2018, 6, 223−230. (18) 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, 623−630. (19) Long, Y.; Shen, Y.; Tian, H.; Yang, Y.; Feng, H.; Li, J. Superwettable Coprinus comatus coated membranes used toward the controllable separation of emulsified oil/water mixtures. J. Membr. Sci. 2018, 565, 85−94. (20) Si, Y.; Fu, Q.; Wang, X.; Zhu, J.; Yu, J.; Sun, G.; Ding, B. Superelastic and Superhydrophobic Nanofiber-Assembled Cellular Aerogels for Effective Separation of Oil/Water Emulsions. ACS Nano 2015, 9, 3791−3799. (21) Dodoo-Arhin, D.; Fabiane, M.; Bello, A.; Manyala, N. Graphene: Synthesis, Transfer, and Characterization for DyeSensitized Solar Cells Applications. Ind. Eng. Chem. Res. 2013, 52, 14160−14168. 7245

DOI: 10.1021/acsomega.9b00428 ACS Omega 2019, 4, 7237−7245