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Cellulose

, Volume 19, Issue 5, pp 1731–1741 | Cite as

Biointeractive antibacterial fibres using polyelectrolyte multilayer modification

  • Josefin Illergård
  • Ute Römling
  • Lars Wågberg
  • Monica EkEmail author
Original Paper

Abstract

Contact-active antibacterial surfaces are a novel tool in the antibacterial battle. The preparation of such surfaces usually involves harsh reaction conditions and organic solvents. A more sustainable alternative would involve physical adsorption of water-soluble polyelectrolytes using a renewable substrate. Here, highly charged cationic polyvinylamines (PVAm), with or without hydrophobic modifications, have been adsorbed onto the naturally anionic cellulosic wood-fibres. To increase the amount of PVAm, polyelectrolyte multilayers were prepared using polyacrylic acid as the anionic polyelectrolyte. The modified fibres were characterised for PVAm content, water retention and antibacterial properties. The use of multilayers increased the total polymer content without notably reducing the water swelling. The fibres were shown to have excellent bioactive properties and reduced waterborne Escherichia coli and Bacillus subtilis by more than 99.9 %, which is a generally accepted definition of an antibacterial material. A large reduction in bacterial growth was observed upon addition of nutrients, although minor growth was detected after 24 h. The results further show that one adsorbed polymer layer was sufficient to obtain a contact-active surface, which makes the PVAm multilayer system seemingly unique. No polymer leaching from any of the samples was detected, indicating that the fibres work via a contact-active antibacterial mechanism. The results show the feasibility of constructing a sustainable antibacterial material using a renewable substrate and water-based solutions in the material construction process.

Keywords

Antibacterial Fibre modification Contact-active Polyelectrolyte adsorption Polyelectrolyte multilayers Cellulose fibres 

Notes

Acknowledgments

BASF SE, SCA Hygiene Products AB and VINNOVA are acknowledged for financing the study. The authors would also like to acknowledge Innventia AB for allowing access to their microbiology lab.

References

  1. Bieser AM, Tiller JC (2011) Mechanistic considerations on contact-active antimicrobial surfaces with controlled functional group densities. Macromol Biosci 11(4):526–534CrossRefGoogle Scholar
  2. Boulmedais F, Frisch B, Etienne O, Lavalle P, Picart C, Ogier J, Voegel JC, Schaaf P, Egles C (2004) Polyelectrolyte multilayer films with pegylated polypeptides as a new type of anti-microbial protection for biomaterials. Biomaterials 25(11):2003–2011CrossRefGoogle Scholar
  3. Bromberg L, Hatton TA (2007) Poly(N-vinylguanidine): characterization, and catalytic and bactericidal properties. Polymer 48(26):7490–7498CrossRefGoogle Scholar
  4. Champ S, Koch O, Ek M, Westman E, Wagberg L, Feuerhake R, Haehnle H (2008) Biocidal coatings, Basf SeGoogle Scholar
  5. Dankovich TA, Gray DG (2011) Bactericidal paper impregnated with silver nanoparticles for point-of-use water treatment. Environ Sci Technol 45(5):1992–1998CrossRefGoogle Scholar
  6. Daoud WA, Xin JH, Zhang Y-H (2005) Surface functionalization of cellulose fibers with titanium dioxide nanoparticles and their combined bactericidal activities. Surf Sci 599(1–3):69–75CrossRefGoogle Scholar
  7. Decher G (1997) Fuzzy nanoassemblies: toward layered polymeric multicomposites. Science 277(5330):1232–1237CrossRefGoogle Scholar
  8. DiFlavio JL, Bertoia R, Pelton R, Leduc M (2005) The mechanism of polyvinylamine wet-strengthening. In: Advances in paper science and technology: transactions of the 13th fundamental research symposium, vols 1–3. pp 1293–1316Google Scholar
  9. Flemming HC (2002) Biofouling in water systems—cases, causes and countermeasures. Appl Microbiol Biotechnol 59(6):629–640CrossRefGoogle Scholar
  10. Hong J, Pelton R (2002) The surface tension of aqueous polyvinylamine and copolymers with < i > N </i > -vinylformamide. Colloid Polym Sci 280(2):203–205CrossRefGoogle Scholar
  11. Hou A, Zhou M, Wang X (2009) Preparation and characterization of durable antibacterial cellulose biomaterials modified with triazine derivatives. Carbohydr Polym 75(2):328–332CrossRefGoogle Scholar
  12. Hsu BB, Ouyang J, Wong SY, Hammond PT, Klibanov AM (2011a) On structural damage incurred by bacteria upon exposure to hydrophobic polycationic coatings. Biotechnol Lett 33(2):411–416CrossRefGoogle Scholar
  13. Hsu BB, Wong SY, Hammond PT, Chen JZ, Klibanov AM (2011b) Mechanism of inactivation of influenza viruses by immobilized hydrophobic polycations. Proc Nat Acad Sci USA 108(1):61–66CrossRefGoogle Scholar
  14. Huang J, Murata H, Koepsel RR, Russell AJ, Matyjaszewski K (2007) Antibacterial polypropylene via surface-initiated atom transfer radical polymerization. Biomacromolecules 8(5):1396–1399CrossRefGoogle Scholar
  15. Huang J, Koepsel RR, Murata H, Wu W, Lee SB, Kowalewski T, Russell AJ, Matyjaszewski K (2008) Nonleaching antibacterial glass surfaces via “grafting onto”: the effect of the number of quaternary ammonium groups on biocidal activity. Langmuir 24(13):6785–6795CrossRefGoogle Scholar
  16. Illergård J, Enarsson LE, Wågberg L, Ek M (2010) Interactions of hydrophobically modified polyvinylamines: adsorption behavior at charged surfaces and the formation of polyelectrolyte multilayers with polyacrylic acid. Acs Appl Mater Interfaces 2(2):425–433CrossRefGoogle Scholar
  17. Illergård J, Wågberg L, Ek M (2011) Bacterial-growth inhibiting properties of multilayers formed with modified polyvinylamine. Colloids Surf B 88(1):115–120CrossRefGoogle Scholar
  18. Isquith AJ, Abbott EA, Walters PA (1972) Surface-bonded antimicrobial activity of an organosilicon quaternary ammonium chloride. Appl Environ Microbiol 24(6):859–863Google Scholar
  19. Klahre J, Flemming HC (2000) Monitoring of biofouling in papermill process waters. Water Res 34(14):3657–3665CrossRefGoogle Scholar
  20. Kügler R, Bouloussa O, Rondelez F (2005) Evidence of a charge-density threshold for optimum efficiency of biocidal cationic surfaces. Microbiology 151(5):1341–1348CrossRefGoogle Scholar
  21. Larsson P, Wågberg L (2010) Diffusion-induced dimensional changes in papers and fibrillar films: influence of hydrophobicity and fibre-wall cross-linking. Cellulose 17(5):891–901CrossRefGoogle Scholar
  22. Lewis K, Klibanov AM (2005) Surpassing nature: rational design of sterile-surface materials. Trend Biotechnol 23(7):343–348CrossRefGoogle Scholar
  23. Lichter JA, Rubner MF (2009) Polyelectrolyte multilayers with intrinsic antimicrobial functionality: the importance of mobile polycations. Langmuir 25(13):7686–7694CrossRefGoogle Scholar
  24. Lichter JA, Van Vliet KJ, Rubner MF (2009) Design of antibacterial surfaces and interfaces: polyelectrolyte multilayers as a multifunctional platform. Macromolecules 42(22):8573–8586CrossRefGoogle Scholar
  25. Lin J, Tiller JC, Lee SB, Lewis K, Klibanov AM (2002) Insights into bactericidal action of surface-attached poly(vinyl-N-hexylpyridinium) chains. Biotechnol Lett 24(10):801–805CrossRefGoogle Scholar
  26. Lindström T, Carlsson G (1982) The effect of chemical environment on fiber swelling. Svensk Papperstidning 85(3):R14–R20Google Scholar
  27. Milović NM, Wang J, Lewis K, Klibanov AM (2005) Immobilized N-alkylated polyethylenimine avidly kills bacteria by rupturing cell membranes with no resistance developed. Biotechnol Bioeng 90(6):715–722CrossRefGoogle Scholar
  28. Murata H, Koepsel RR, Matyjaszewski K, Russell AJ (2007) Permanent, non-leaching antibacterial surfaces-2: how high density cationic surfaces kill bacterial cells. Biomaterials 28(32):4870–4879CrossRefGoogle Scholar
  29. Park D, Wang J, Klibanov AM (2006) One-step, painting-like coating procedures to make surfaces highly and permanently bactericidal. Biotechnol Prog 22:584–589CrossRefGoogle Scholar
  30. Patel M (2009) Developments in Antibacterial Paper, Pira InternationalGoogle Scholar
  31. Ravikumar T, Murata H, Koepsel RR, Russell AJ (2006) Surface-active antifungal polyquaternary amine. Biomacromolecules 7(10):2762–2769CrossRefGoogle Scholar
  32. Roy D, Knapp JS, Guthrie JT, Perrier S (2007) Antibacterial cellulose fiber via RAFT surface graft polymerization. Biomacromolecules 9(1):91–99CrossRefGoogle Scholar
  33. Russell AD (2003) Biocide use and antibiotic resistance: the relevance of laboratory findings to clinical and environmental situations. Lancet Infect Dis 3(12):794–803CrossRefGoogle Scholar
  34. Scientific Committee on Emerging and Newly Identified Health Risks (2009) Assessment of the Antibiotic Resistance Effects of Biocides. European CommissionGoogle Scholar
  35. Silver S, Phung L, Silver G (2006) Silver as biocides in burn and wound dressings and bacterial resistance to silver compounds. J Ind Microbiol Biotechnol 33(7):627–634CrossRefGoogle Scholar
  36. Tiller J (2010) Antimicrobial surfaces. Bioactive surfaces. Börner, H. G. L., Jean-Francois, Springer Berlin/Heidelberg. 240/2011:193–217Google Scholar
  37. Tiller JC, Liao CJ, Lewis K, Klibanov AM (2001) Designing surfaces that kill bacteria on contact. Proc Nat Acad Sci USA 98(11):5981–5985CrossRefGoogle Scholar
  38. Tsien RY (1998) The green fluorescent protein. Annu Rev Biochem 67(1):509–544CrossRefGoogle Scholar
  39. Wågberg L, Forsberg S, Johansson A, Juntti P (2002) Engineering of fibre surface properties by application of the polyelectrolyte multilayer concept. Part I: modification of paper strength. J Pulp Pap Sci 28(7):222–228Google Scholar
  40. Westman EH, Ek M, Enarsson LE, Wågberg L (2009a) Assessment of antibacterial properties of polyvinylamine (PVAm) with different charge densities and hydrophobic modifications. Biomacromolecules 10(6):1478–1483CrossRefGoogle Scholar
  41. Westman EH, Ek M, Wågberg L (2009b) Antimicrobial activity of polyelectrolyte multilayer-treated cellulose films. Holzforschung 63(1):33–39CrossRefGoogle Scholar
  42. Wong SY, Li Q, Veselinovic J, Kim B-S, Klibanov AM, Hammond PT (2010) Bactericidal and virucidal ultrathin films assembled layer by layer from polycationic N-alkylated polyethylenimines and polyanions. Biomaterials 31(14):4079–4087CrossRefGoogle Scholar

Copyright information

© Springer Science+Business Media B.V. 2012

Authors and Affiliations

  • Josefin Illergård
    • 1
  • Ute Römling
    • 2
  • Lars Wågberg
    • 1
  • Monica Ek
    • 1
    Email author
  1. 1.Department of Fibre and Polymer TechnologyKTH Royal Institute of TechnologyStockholmSweden
  2. 2.Department of Microbiology, Tumor and Cell BiologyKarolinska InstitutetStockholmSweden

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