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A novel hydroxofluorographene-coated melamine foam for efficient and repeatable oil removal from water


With the frequent occurrence of oil spill accidents and the continuous discharge of oily water during oil production and transportation, effective oil removal from environmental water by adsorption still faces severe challenges. Here, a novel absorbent hydroxofluorographene-coated melamine foam, namely G(OH)F@MF, with high affinity to oils was fabricated via stepwise assembly. The G(OH)F@MF absorbent achieved effective removal of various oils within 1 min with relatively high adsorption capacities for petrol (89.34 g/g), lubricating oil (89.60 g/g), and peanut oil (104.79 g/g). Furthermore, it could be regenerated by simply squeezing and reused for more than 10 times with an adsorption capacity exceeding 37.12 g/g. In addition, the results indicated that the G(OH)F@MF absorbent was suitable for oil cleanup at a wide range of pH values (4–12) and temperatures (5–45 °C). The adsorption performance of the material was stable in the presence of natural organic matter and even in different water environments. This study can provide a novel sorbent and method for the green, rapid, recyclable, and stable removal of oils from environmental water.

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  1. Cervantes-González E, Rojas-Avelizapa NG, Cruz-Camarillo R, García-Mena J, Rojas-Avelizapa LI (2008) Oil-removal enhancement in media with keratinous or chitinous wastes by hydrocarbon-degrading bacteria isolated from oil-polluted soils. Environ Technol 29(2):171–182

  2. Chantharasupawong P, Philip R, Narayanan TN, Sudeep PM, Mathkar A, Ajayan PM, Thomas J (2012) Optical power limiting in fluorinated graphene oxide: an insight into the nonlinear optical properties. J Phys Chem C 116(49):25955–25961

  3. Cheng SH, Zou KQ, Okino F, Gutierrez HR, Gupta A, Shen N, Eklund PC, Sofo J, Zhu JQ (2010) Reversible fluorination of graphene: evidence of a two-dimensional wide bandgap semiconductor. Phys Rev B 81(20):205435

  4. Cheryan M, Rajagopalan N (1998) Membrane processing of oily streams. Wastewater treatment and waste reduction. J Membr Sci 151(1):13–28

  5. Ding L, Snoeyink V, Mariñas BJ, Yue ZR, Economy J (2008) Effects of powdered activated carbon pore size distribution on the competitive adsorption of aqueous atrazine and natural organic matter. Environ Sci Technol 42(4):1227–1231

  6. Elraies KA, Tan IM (2010) Design and application of a new acid-alkali-surfactant flooding formulation for Malaysian reservoirs. Soc Pet Eng.

  7. František K, Otyepka M (2013) Band gaps and optical spectra of chlorographene, fluorographene and graphane from G0W0, GW0 and GW calculations on top of PBE and HSE06 orbitals. J Chem Theory Comput 9(9):4155–4164

  8. Ge J, Shi LA, Wang YC (2017) Joule-heated graphene-wrapped sponge enables fast clean-up of viscous crude-oil spill. Nat Nanotechnol 12(5):434–440

  9. Gregg SJ, Sing KSW (1982) Adsorption, surface area and porosity, 2nd edn. Academic Press, London

  10. Hyung H, Kim JH (2008) Natural organic matter (NOM) adsorption to multi-walled carbon nanotubes: effect of NOM characteristics and water quality parameters. Environ Sci Technol 42(12):4416–4421

  11. Jiang L, Liu Y, Liu S, Zeng G, Hu X, Hu X, Guo Z, Tan X, Wang L, Wu Z (2017) Adsorption of estrogen contaminants by graphene nanomaterials under natural organic matter preloading: comparison to carbon nanotube, biochar, and activated carbon. Environ Sci Technol 51(11):6352–6359

  12. Jonker MTO, Muijs B (2010) Using solid phase micro extraction to determine salting-out (Setschenow) constants for hydrophobic organic chemicals. Chemosphere 80(3):223–227

  13. Joshi RK, Alwarappan S, Yoshimura M, Sahajwalla V, Nishina Y (2015) Graphene oxide: the new membrane material. Appl Mater Today 1(1):1–12

  14. Kim SK, Chang H, Choi JW, Huang JX, Jiang HD (2014) Aerosol processing of graphene and its application to oil absorbent and glucose biosensor. KONA Powder Part J 31:111–125

  15. Li BB, Liu XY, Zhang XY, Chai WB, Ma YN, Tao JJ (2015) Facile preparation of graphene-coated polyurethane sponge with superhydrophobic/superoleophilic properties. J Polym Res 22(10):190

  16. Lin KYA, Chen YC, Phattarapattamawong S (2016) Efficient demulsification of oil-in-water emulsions using a zeolitic imidazolate framework: adsorptive removal of oil droplets from water. J Colloid Interface Sci 478:96–106

  17. Liu HD, Liu ZY, Yang MB, He Q (2013) Surperhydrophobic polyurethane foam modified by graphene oxide. J Appl Polym Sci 130:3530–3536

  18. Liu HZ, Geng BY, Chen YF, Wang HY (2016) A review on the aerogel-type oil sorbents derived from nanocellulose. ACS Sustain Chem Eng 5(1):49–66

  19. Lv XS, Tian DH, Peng YY, Li JX, Jiang GM (2019) Superhydrophobic magnetic reduced graphene oxide-decorated foam for efficient and repeatable oil-water separation. Appl Surf Sci 466:937–945

  20. Ma WJ, Zhao JT, Oderinde O, Han JQ, Liu ZC, Gao BH, Xiong RH, Zhang QL, Jiang SH, Huang CB (2018) Durable superhydrophobic and superoleophilic electrospun nanofibrous membrane for oil-water emulsion separation. J Colloid Interface Sci 532:12–23

  21. Mao HY, Laurent S, Chen W, Akhavan O, Imani M, Ashkarran AA (2013) Graphene: promises, facts, opportunities, and challenges in nanomedicine. Chem Rev 113(5):3407–3424

  22. Martins SE, Withers F, Dubois M, Craciun MF, Russo S (2013) Tuning the transport gap of functionalized graphene via electron beam irradiation. New J Phys 15(3):033024

  23. Mullin JV, Champ MA (2003) Introduction/overview to in situ burning of oil spills. Spill Sci Technol Bull 8(4):323–330

  24. Nair RR, Blake P, Grigorenko AN, Novoselov KS, Booth TJ, Stauber T (2008) Fine structure constant defines visual transparency of graphene. Science 320(5881):1308

  25. Novoselov KS, Geim AK, Morozov SV, Jiang D, Zhang Y, Dubonos SV (2004) Electric field effect in atomically thin carbon films. Science 306(5696):666–669

  26. Peigney A, Laurent C, Flahaut E, Bacsa RR, Rousset A (2001) Specific surface area of carbon nanotubes and bundles of carbon nanotubes. Carbon 39(4):507–514

  27. Peng M, Chen GQ, Zeng GM, Chen AW, He K, Huang ZZ, Hu L, Shi JB, Li H, Yuan L, Huang TT (2018) Superhydrophobic kaolinite modified graphene oxide-melamine sponge with excellent properties for oil-water separation. Appl Clay Sci 163:63–71

  28. Pham VH, Dickerson JH (2014) Superhydrophobic silanized melamine sponges as high efficiency oil absorbent materials. ACS Appl Mater Interfaces 6(16):14181–14188

  29. Pinto J, Athanassiou A, Fragouli D (2016) Effects of the porous structure of polymer foams on the remediation of oil spills. J Phys D Appl Phys 49(14):145601

  30. Pinto J, Heredia-Guerrero JA, Athaanassiou A, Fragouli D (2017) Reusable nanocomposite-coated polyurethane foams for the remediation of oil spills. Int J Environ Sci Technol 14:2055–2066

  31. Poh HL, Šimek P, Sofer Z, Pumera M (2013) Halogenation of graphene with chlorine, bromine, or iodine by exfoliation in a halogen atmosphere. Chem Eur J 19(8):2655–2662

  32. Ruan C, Ai K, Li X, Lu L (2014) A superhydrophobic sponge with excellent absorbency and flame retardancy. Angew Chem Int Ed Engl 53(22):5556–5560

  33. Saha P, Dashairya L (2018) Reduced graphene oxide modified melamine formaldehyde (rGO@MF) superhydrophobic sponge for efficient oil-water separation. J Porous Mater 25(5):1475–1488

  34. Sahin H, Topsakal M, Ciraci S (2011) Structures of fluorinated graphenes and their signatures. Phys Rev B 83(11):115432

  35. Song S, Yang H, Su CP, Jiang ZB, Lu Z (2016) Ultrasonic-microwave assisted synthesis of stable reduced graphene oxide modified melamine foam with superhydrophobicity and high oil adsorption capacities. Chem Eng J 306:504–511

  36. Sun HG, Yang XB, Zhang YQ, Cheng XQ, Xu YC, Bai YP, Shao L (2018) Segregation-induced in situ hydrophilic modification of poly (vinylidene fluoride) ultrafiltration membranes via sticky poly (ethylene glycol) blending. J Membr Sci 563:22–30

  37. Tjandra R, Lui G, Veilleux A, Broughton J, Chiu G, Yu AP (2015) Introduction of an enhanced binding of reduced graphene oxide to polyurethane sponge for oil adsorption. Ind Eng Chem Res 54(14):3657–3663

  38. Tuček J, Holá K, Bourlinos AB, Błoński P, Bakandritsos A, Ugolotti J, Dubecký M, Karlický F, Ranc V, Čépe K, Otyepka M, Zbořil R (2017) Room temperature organic magnets derived from sp3 functionalized graphene. Nat Commun 8:14525

  39. Xia CB, Li YB, Fei T, Gong WL (2018) Facile one-pot synthesis of superhydrophobic reduced graphene oxide-coated polyurethane sponge at the presence of ethanol for oil-water separation. Chem Eng J 345:648–658

  40. Xie WH, Shiu WY, Mackay D (1997) A review of the effect of salts on the solubility of organic compounds in seawater. Mar Environ Res 44(4):429–444

  41. Yang X, Wang Z, Shao L (2017) Construction of oil-unidirectional membrane for integrated oil collection with lossless transportation and oil-in-water emulsion purification. J Membr Sci 549(1):67–74

  42. Zbořil R, Karlický F, Bourlinos AB, Steriotis TA, Stubos AK, Georgakilas V (2010) Graphene fluoride: a stable stoichiometric graphene derivative and its chemical conversion to graphene. Small (Weinheim an der Bergstrasse, Germany) 6(24):2885–2891

  43. Zhang XT, Liu DY, Ma YL, Nie J, Sui GX (2017) Super-hydrophobic graphene coated polyurethane (GN@PU) sponge with great oil-water separation performance. Appl Surf Sci 422:116–124

  44. Zhao XK, Yang GP, Gao XC (2003) Studies on the sorption behaviors of nitrobenzene on marine sediments. Chemosphere 52(5):917–925

  45. Zhao J, Guo QJ, Wang X, Xie HL, Chen YZ (2016) Recycle and reusable melamine sponge coated by graphene for highly efficient oil-absorption. Colloids Surf A Physicochem Eng Asp 488:93–99

  46. Zheng MP, Xia JT, Gu MY, Chen ZZ (1999) Preparation and study on fluoride graphite. J Mater Eng 8:21–23

  47. Zhu YW, Murali S, Cai WW, Li XS, Suk JW, Potts JR (2010) Graphene and graphene oxide: synthesis, properties, and applications. Cheminform 22(46):3906–3924

  48. Zhu Q, Pan Q, Liu F (2011) Facile removal and collection of oils from water surfaces through superhydrophobic and superoleophilic sponges. J Phys Chem C 115(35):17464–17470

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This study was supported by the National Natural Science Foundation of China (No. 51779076); the Foundation for Innovative Research Groups of the National Natural Science Foundation of China (No. 51421006); the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD); and the Top-Notch Academic Programs Project of Jiangsu Higher Education Institutions (TAPP).

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Correspondence to Yi Li.

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Zhou, X., Li, Y., Zhang, C. et al. A novel hydroxofluorographene-coated melamine foam for efficient and repeatable oil removal from water. Environ Sci Pollut Res (2020).

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  • Hydroxofluorographene
  • Melamine foam
  • Oil removal
  • Oil/water separation
  • Recyclability