pp 1–12 | Cite as

Fabrication of robust superhydrophobic filter paper for oil/water separation based on the combined octadecanoyl chain bonding and polymer grafting via surface-initiated ATRP

  • Kangmin Zhang
  • Miaomiao Wang
  • Mingyuan Wu
  • Qingyun Wu
  • Jiuyi Liu
  • Jianjun Yang
  • Jianan ZhangEmail author
Original Research


Effective separation of oil and water has always been a long-term challenge. Here we introduce a facile and fluorine-free method to fabricate superhydrophobic and superoleophilic filter paper without the decoration of solid particles for robust oil/water separation. After chemically bonding octadecanoyl and α-bromoisobutyryl groups on the surface of filter paper through simultaneous esterification with stearoyl chloride and α-bromoisobutyryl bromide (BiBB) to obtain C18-FP-g-Br, superhydrophobic poly(styrene-co-acrylonitrile) (SAN) grafted filter paper (C18-FP-g-SAN) was fabricated via surface-initiated atom transfer radical polymerization. The obtained C18-FP-g-SAN showed a water contact angle of 153° and achieved a separation efficiency exceeding 98.5% after ten different typical oil/water separation processes due to the synergistically combined contributions of bonded octadecanoyl chain and grafted SAN. C18-FP-g-SAN remained high separation efficiency after 10 cycles of use and treatment with strong acidic or basic solution. The excellent reusability and chemical stability of C18-FP-g-SAN promise its practical applications of continuous oil/water separation and oil spillage cleanup.

Graphic abstract


Filter paper Oil/water separation SI-ATRP Superhydrophobicity Superoleophilicity 



This work was financially supported by National Natural Science Foundation of China (51973001), the Major Program of University Natural Science Research Project of Anhui Province (KJ2019ZD01), the Key Projects of Innovation Program for Returned Scholars of Anhui Province (2019LCX006), and the Open fund for Discipline Construction, Institute of Physical Science and Information Technology, Anhui University (Grant No. 201813).


  1. Balamurali B, Victor B, Hess DW (2008) Fabrication of “roll-off” and “sticky” superhydrophobic cellulose surfaces via plasma processing. Langmuir 24:4785–4790CrossRefGoogle Scholar
  2. Cao N, Yang B, Barras A, Szunerits S, Boukherroub R (2017) Polyurethane sponge functionalized with superhydrophobic nanodiamond particles for efficient oil/water separation. Chem Eng J 307:319–325CrossRefGoogle Scholar
  3. Carlmark A, Malmström EE (2003) ATRP grafting from cellulose fibers to create block-copolymer grafts. Biomacromolecules 4:1740–1745CrossRefGoogle Scholar
  4. Cassie ABD, Baxter S (1944) Wettability of porous surfaces. Trans Faraday Soc 40:546–551CrossRefGoogle Scholar
  5. Cervin NT, Aulin C, Larsson PT, Wågberg L (2012) Ultra porous nanocellulose aerogels as separation medium for mixtures of oil/water liquids. Cellulose 19:401–410CrossRefGoogle Scholar
  6. Cho SC, Yong CH, Cho SG, Ji YY, Chang SH, Han SU (2009) Surface modification of polyimide films, filter papers, and cotton clothes by HMDSO/toluene plasma at low pressure and its wettability. Curr Appl Phys 9:1223–1226CrossRefGoogle Scholar
  7. Chu Z, Feng Y, Seeger S (2014) Oil/water separation with selective superantiwetting/superwetting surface saterials. Angew Chem Int Ed Engl 54:2328–2338CrossRefGoogle Scholar
  8. Feng X, Shi Y, Jia L, Wu Y (2015) Fabrication of filter paper with tunable wettability and its application in oil–water separation. J Sol Gel Sci Technol 76:129–137CrossRefGoogle Scholar
  9. Ge J, Zhao HY, Zhu HW, Huang J, Shi LA, Yu SH (2016) Advanced sorbents for oil-spill cleanup: recent advances and future perspectives. Adv Mater 28:10459–10490CrossRefGoogle Scholar
  10. Gupta S, Tai NH (2015) Carbon materials as oil sorbents: a review on the synthesis and performance. J Mater Chem A 4:1550–1565CrossRefGoogle Scholar
  11. Hua Z, Wang H, Niu H, Gestos A, Wang X, Tong L (2012) Fluoroalkyl silane modified silicone rubber/nanoparticle composite: a super durable, robust superhydrophobic fabric coating. Adv Mater 24:2409–2412CrossRefGoogle Scholar
  12. Huang X, Wen X, Cheng J, Yang Z (2012) Sticky superhydrophobic filter paper developed by dip-coating of fluorinated waterborne epoxy emulsion. Appl Surf Sci 258:8739–8746CrossRefGoogle Scholar
  13. Joye SB (2015) Deepwater horizon, 5 years on. Science 349:592–593CrossRefGoogle Scholar
  14. Kraemer EO (1938) Molecular weights of celluloses and cellulose derivates. Ind Eng Chem 30:1200–1203CrossRefGoogle Scholar
  15. Li SH, Huang JY, Ge MZ, Li SW, Xing TL, Chen GQ, Liu YQ, Zhang KQ, Al-Deyab SS, Lai YK (2015) Controlled grafting superhydrophobic cellulose surface with environmentally-friendly short fluoroalkyl chains by ATRP. Mater Des 85:815–822CrossRefGoogle Scholar
  16. Li Y, Li Q, Zhang C, Peng C, Bai N, Xi X (2017) Intelligent self-healing superhydrophobic modification of cotton fabrics via surface-initiated ARGET ATRP of styrene. Chem Eng J 323:134–142CrossRefGoogle Scholar
  17. Liang K, Wang Q, Xiong S, Yong W (2014) Turning low-cost filter papers to highly efficient membranes for oil/water separation by atomic-layer-deposition-enabled hydrophobization. Ind Eng Chem Res 53:16516–16522CrossRefGoogle Scholar
  18. Loría-Bastarrachea MI, Carrillo-Escalante HJ, Aguilar-Vega MJ (2010) Grafting of poly(acrylic acid) onto cellulosic microfibers and continuous cellulose filaments and characterization. J Appl Polym Sci 83:386–393CrossRefGoogle Scholar
  19. Peng CW, Chang KC, Weng CJ, Lai MC, Hsu CH, Hsu SC, Li SY, Wei Y, Yeh JM (2013) UV-curable nanocasting technique to prepare bio-mimetic super-hydrophobic non-fluorinated polymeric surfaces for advanced anticorrosive coatings. Polym Chem 4:926–932CrossRefGoogle Scholar
  20. Phanthong P, Reubroycharoen P, Kongparakul S, Samart C, Wang Z, Hao X, Abudula A, Guan G (2018) Fabrication and evaluation of nanocellulose sponge for oil/water separation. Carbohydr Polym 190:184–189CrossRefGoogle Scholar
  21. Schrope M (2011) Oil spill: deep wounds. Nature 472:152–154CrossRefGoogle Scholar
  22. Simpson JT, Hunter SR, Aytug T (2015) Superhydrophobic materials and coatings: a review. Rep Prog Phys 78:086501CrossRefGoogle Scholar
  23. Wang H, Fang J, Cheng T, Ding J, Qu L, Dai L, Wang X, Lin T (2008) One-step coating of fluoro-containing silica nanoparticles for universal generation of surface superhydrophobicity. Chem Commun 7:877–879CrossRefGoogle Scholar
  24. Wang B, Liang W, Guo Z, Liu W (2015) Biomimetic super-lyophobic and super-lyophilic materials applied for oil/water separation: a new strategy beyond nature. Chem Soc Rev 44:336–361CrossRefGoogle Scholar
  25. Wenzel RN (1936) Resistance of solid surfaces to wetting by water. Ind Eng Chem 28:988–994CrossRefGoogle Scholar
  26. Xue Z, Wang S, Lin L, Chen L, Liu M, Feng L, Jiang L (2011) A novel superhydrophilic and underwater superoleophobic hydrogel-coated mesh for oil/water separation. Adv Mater 23:4270–4273CrossRefGoogle Scholar
  27. Yang C, Tartaglino U, Persson BNJ (2006) Influence of surface roughness on superhydrophobicity. Phys Rev Lett 97:116103CrossRefGoogle Scholar
  28. Yao L, Sathasivam S, Song J, Crick CR, Carmalt CJ, Parkin IP (2015) Robust self-cleaning surfaces that function when exposed to either air or oil. Science 347:1132–1135CrossRefGoogle Scholar
  29. Ye S, Cao Q, Wang Q, Wang T, Peng Q (2016) A highly efficient, stable, durable, and recyclable filter fabricated by femtosecond laser drilling of a titanium foil for oil–water separation. Sci Rep 6:37591CrossRefGoogle Scholar
  30. Yu T, Xu G, Wang X, Yang J, Hu J (2014) Fabrication of oil–water separation filter paper by simple impregnation with fluorinated poly-acrylate emulsion. BioResources 9:4421–4429Google Scholar
  31. Yuan D, Zhang T, Guo Q, Qiu F, Yang D, Ou Z (2018a) Recyclable biomass carbon@SiO2@MnO2 aerogel with hierarchical structures for fast and selective oil–water separation. Chem Eng J 351:622–630CrossRefGoogle Scholar
  32. Yuan D, Zhang T, Guo Q, Qiu F, Yang D, Ou Z (2018b) Superhydrophobic hierarchical biomass carbon aerogel assembled with TiO2 nanorods for selective immiscible oil/water mixture and emulsion separation. Ind Eng Chem Res 57:14758–14766CrossRefGoogle Scholar
  33. Yue X, Zhang T, Yang D, Qiu F, Li Z (2018) Janus ZnO-cellulose/MnO2 hybrid membranes with asymmetric wettability for highly-efficient emulsion separations. Cellulose 25:5951–5965CrossRefGoogle Scholar
  34. Yue X, Li Z, Zhang T, Yang D, Qiu F (2019) Design and fabrication of superwetting fiber-based membranes for oil/water separation applications. Chem Eng J 364:292–309CrossRefGoogle Scholar
  35. Zhang YL, Xia H, Kim E, Sun HB (2012) Recent developments in superhydrophobic surfaces with unique structural and functional properties. Soft Matter 8:11217–11231CrossRefGoogle Scholar
  36. Zhou X, Zhang Z, Xu X, Guo F, Zhu X, Men X, Ge B (2013) Robust and durable superhydrophobic cotton fabrics for oil/water separation. ACS Appl Mater Interfaces 5:7208–7214CrossRefGoogle Scholar
  37. Zimmermann J, Reifler FA, Fortunato G, Gerhardt LC, Seeger S (2010) A simple, one-step approach to durable and robust superhydrophobic textiles. Adv Funct Mater 18:3662–3669CrossRefGoogle Scholar
  38. Zou H, Lin S, Tu Y, Liu G, Hu J, Li F, Miao L, Zhang G, Luo H, Liu F (2013) Simple approach towards fabrication of highly durable and robust superhydrophobic cotton fabric from functional diblock copolymer. J Mater Chem A 1:11246–11260CrossRefGoogle Scholar
  39. Zulkifli NI, Samat N, Anuar H, Zainuddin N (2015) Mechanical properties and failure modes of recycled polypropylene/microcrystalline cellulose composites. Mater Des 69:114–123CrossRefGoogle Scholar

Copyright information

© Springer Nature B.V. 2019

Authors and Affiliations

  1. 1.School of Chemistry and Chemical EngineeringAnhui UniversityHefeiPeople’s Republic of China
  2. 2.Anhui Province Key Laboratory of Environment-Friendly Polymer MaterialsHefeiPeople’s Republic of China
  3. 3.Institute of Physical Science and Information TechnologyAnhui UniversityHefeiPeople’s Republic of China

Personalised recommendations