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Inkjet printed drug-releasing polyelectrolyte multilayers for wound dressings

Department of Chemical Engineering, Worcester Polytechnic Institute, 100 Institute Road, Worcester, Massachusetts 01609, USA

Topical Section: Biological and biomimetic materials

Inkjet printing was used as a novel processing method for the preparation of polyelectrolyte multilayers. Conformal, consistent coatings were formed on a cotton substrate. As a demonstration of a potential application of this processing method, polyelectrolyte multilayers were assembled on cotton for wound dressing. When loaded with gentamicin, these coatings demonstrated burst release of 50% of the loaded gentamicin over the first five hours, followed by consistent release of 0.15 µg/(cm2-h) for at least four days. Significant antimicrobial activity of the gentamicin-releasing polyelectrolyte multilayer-coated cotton was observed, with a zone of inhibition of 1.575 ± 0.03 cm. This result is comparable to the zone of inhibition for cotton soaked in gentamicin (1.75 ± 0.04 cm), indicating that the inkjet printing processing method does not degrade gentamicin. Inkjet printing shows promise as a low cost, versatile option for polyelectrolyte multilayer fabrication. Additionally, as a scalable process, inkjet printed samples exhibited consistent antibacterial function for over three months after preparation.
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Keywords polyelectrolyte multilayers; polyelectrolyte complexes; inkjet printing; Escheria coli; gentamicin; surface properties

Citation: Huilin Yang, Amy M. Peterson. Inkjet printed drug-releasing polyelectrolyte multilayers for wound dressings. AIMS Materials Science, 2017, 4(2): 452-469. doi: 10.3934/matersci.2017.2.452

References

  • 1. Sen CK, Gordillo GM, Roy S, et al. (2009) Human skin wounds: A major and snowballing threat to public health and the economy. Wound Repair Regen 17: 763–771.    
  • 2. Mangoni ML, Mcdermott AM, Zasloff M (2016) Antimicrobial peptides and wound healing: Biological and therapeutic considerations. Exp Dermatol 25: 167–173.    
  • 3. Fahs F, Bi X, Yu FS, et al. (2015) New insights into microRNAs in skin wound healing. IUBMB Life 67: 889–896.    
  • 4. You HJ, Han SK (2014) Cell therapy for wound healing. J Korean Med Sci 29: 311–319.    
  • 5. Boateng JS, Matthews KH, Stevens HNE, et al. (2008) Wound healing dressings and drug delivery systems: A review. J Pharm Sci 97: 2892–2923.    
  • 6. Zelikin AN (2010) Drug Releasing Polymer Thin Films: New Era of Surface-Mediated Drug Delivery. ACS Nano 4: 2494–2509.    
  • 7. Delcea M, Möhwald H, Skirtach AG (2011) Stimuli-responsive LbL capsules and nanoshells for drug delivery. Adv Drug Deliver Rev 63: 730–747.    
  • 8. Kataoka K, Harada A, Nagasaki Y (2001) Block copolymer micelles for drug delivery: design, characterization and biological significance. Adv Drug Deliver Rev 47: 113–131.    
  • 9. Qiu Y, Park K (2001) Environment-sensitive hydrogels for drug delivery. Adv Drug Deliver Rev 53: 321–339.
  • 10. Yamada Y, Harashima H (2008) Mitochondrial drug delivery systems for macromolecule and their therapeutic application to mitochondrial diseases. Adv Drug Deliver Rev 60: 1439–1462.    
  • 11. Huang X, Brazel CS (2001) On the importance and mechanisms of burst release in matrix-controlled drug delivery systems. J Control Release 73: 121–136.    
  • 12. Kost J, Langer R (2001) Responsive polymeric delivery systems. Adv Drug Deliver Rev 46: 125–148.
  • 13. Wohl BM, Engbersen JFJ (2012) Responsive layer-by-layer materials for drug delivery. J Control Release 158: 2–14.
  • 14. Meyer F, Dimitrova M, Jedrzejenska J, et al. (2008) Relevance of bi-functionalized polyelectrolyte multilayers for cell transfection. Biomaterials 29: 618–624.    
  • 15. Lee IC, Wu YC (2014) Assembly of Polyelectrolyte Multilayer Films on Supported Lipid Bilayers To Induce Neural Stem/Progenitor Cell Differentiation into Functional Neurons. ACS Appl Mater Inter 6: 14439–14450.    
  • 16. Fakhrullin RF, Zamaleeva AI, Minullina RT, et al. (2012) Cyborg cells: functionalisation of living cells with polymers and nanomaterials. Chem Soc Rev 41: 4189–4206.    
  • 17. Fakhrullin RF, Lvov YM (2012) "Face-Lifting" and "Make-Up" for Microorganisms: Layer-by-Layer Polyelectrolyte Nanocoating. ACS Nano 6: 4557–4564.    
  • 18. He W, Frueh J, Shao J, et al. (2016) Guidable GNR-Fe3O4-PEM@SiO2 composite particles containing near infrared active nanocalorifiers for laser assisted tissue welding. Colloid Surface A 511: 73–81.    
  • 19. He W, Frueh J, Hu N, et al. (2016) Guidable Thermophoretic Janus Micromotors Containing Gold Nanocolorifiers for Infrared Laser Assisted Tissue Welding. Adv Sci 3: 1600206.    
  • 20. Moskowitz JS, Blaisse MR, Samuel RE, et al. (2010) The effectiveness of the controlled release of gentamicin from polyelectrolyte multilayers in the treatment of Staphylococcus aureus infection in a rabbit bone model. Biomaterials 31: 6019–6030.    
  • 21. Shukla A, Fang JC, Puranam S, et al. (2012) Release of vancomycin from multilayer coated absorbent gelatin sponges. J Control Release 157: 64–71.    
  • 22. Shukla A, Fuller RC, Hammond PT (2011) Design of multi-drug release coatings targeting infection and inflammation. J Control Release 155: 159–166.    
  • 23. Teng XR, Shchukin DG, Möhwald H (2008) A Novel Drug Carrier: Lipophilic Drug-Loaded Polyglutamate/Polyelectrolyte Nanocontainers. Langmuir 24: 383–389.    
  • 24. Shchukina EM, Shchukin DG (2011) LbL coated microcapsules for delivering lipid-based drugs. Adv Drug Deliver Rev 63: 837–846.    
  • 25. González-Toro DC, Ryu JH, Chacko RT, et al. (2012) Concurrent binding and delivery of proteins and lipophilic small molecules using polymeric nanogels. J Am Chem Soc 134: 6964–6967.    
  • 26. Shukla A, Fleming KE, Chuang HF, et al. (2010) Controlling the release of peptide antimicrobial agents from surfaces. Biomaterials 31: 2348–2357.    
  • 27. Huang Y, Luo Q, Li X, et al. (2012) Fabrication and in vitro evaluation of the collagen/hyaluronic acid PEM coating crosslinked with functionalized RGD peptide on titanium. Acta Biomater 8: 866–877.    
  • 28. Palankar R, Skirtach AG, Kreft O, et al. (2009) Controlled intracellular release of peptides from microcapsules enhances antigen presentation on MHC class I molecules. Small 5: 2168–2176.
  • 29. Zhang J, Chua LS, Lynn DM (2004) Multilayered thin films that sustain the release of functional DNA under physiological conditions. Langmuir 20: 8015–8021.    
  • 30. Kim SH, Jeong JH, Lee SH, et al. (2008) Local and systemic delivery of VEGF siRNA using polyelectrolyte complex micelles for effective treatment of cancer. J Control Release 129: 107–116.    
  • 31. Cho HJ, Chong S, Chung SJ, et al. (2012) Poly-L-arginine and dextran sulfate-based nanocomplex for epidermal growth factor receptor (EGFR) siRNA delivery: its application for head and neck cancer treatment. Pharm Res 29: 1007–1019.    
  • 32. Magboo R, Peterson AM (2016) Polyelectrolyte multilayers for controlled release of biologically relevant molecules. In: Somasundaran P, Encyclopedia of Surface and Colloid Science, Taylor and Francis, 1519–1533.
  • 33. Shah NJ, Macdonald ML, Beben YM, et al. (2011) Tunable dual growth factor delivery from polyelectrolyte multilayer films. Biomaterials 32: 6183–6193.    
  • 34. Crouzier T, Ren K, Nicolas C, et al. (2009) Layer-by-layer films as a biomimetic reservoir for rhBMP-2 delivery: Controlled differentiation of myoblasts to osteoblasts. Small 5: 598–608.    
  • 35. Peterson AM, Pilz-Allen C, Kolesnikova T, et al. (2014) Growth factor release from polyelectrolyte-coated titanium for implant applications. ACS Appl Mater Inter 6: 1866–1871.
  • 36. Gand A, Hindié M, Chacon D, et al. (2014) Nanotemplated polyelectrolyte films as porous biomolecular delivery systems: Application to the growth factor BMP-2. Biomatter 4: e28823.    
  • 37. Seon L, Lavalle P, Schaaf P, et al. (2015) Polyelectrolyte Multilayers: A Versatile Tool for Preparing Antimicrobial Coatings. Langmuir 31: 12856–12872.    
  • 38. Grunlan JC, Choi JK, Lin A (2005) Antimicrobial behavior of polyelectrolyte multilayer films containing cetrimide and silver. Biomacromolecules 6: 1149–1153.
  • 39. Lichter JA, Van Vliet KJ, Rubner MF (2009) Design of Antibacterial Surfaces and Interfaces: Polyelectrolyte Multilayers as a Multifunctional Platform. Macromolecules 42: 8573–8586.    
  • 40. Gomes AP, Mano JF, Queiroz JA, et al. (2012) Layer-by-Layer Deposition of Antibacterial Polyelectrolytes on Cotton Fibres. J Polym Environ 20: 1084–1094.    
  • 41. Agarwal A, Nelson TB, Kierski PR, et al. (2012) Polymeric multilayers that localize the release of chlorhexidine from biologic wound dressings. Biomaterials 33: 6783–6792.    
  • 42. Yang JM, Yang JH, Huang HT (2014) Chitosan/polyanion surface modification of styrene-butadiene-styrene block copolymer membrane for wound dressing. Mater Sci Eng C 34: 140–148.    
  • 43. Dai J, Bruening ML (2002) Catalytic Nanoparticles Formed by Reduction of Metal Ions in Multilayered Polyelectrolyte Films. Nano Lett 2: 497–501.    
  • 44. Rieger KA, Birch NP, Schiffman JD (2013) Designing electrospun nanofiber mats to promote wound healing-a review. J Mater Chem B 1: 4531.
  • 45. Wood KC, Chuang HF, Batten RD, et al. (2006) Controlling interlayer diffusion to achieve sustained, multiagent delivery from layer-by-layer thin films. Proceedings of the National Academy of Sciences, 103: 10207–10212.    
  • 46. Kiryukhin MV, Man SM, Tonoyan A, et al. (2012) Adhesion of polyelectrolyte multilayers: Sealing and transfer of microchamber arrays. Langmuir 28: 5678–5686.    
  • 47. Kiryukhin MV, Gorelik SR, Man SM, et al. (2013) Individually addressable patterned multilayer microchambers for site-specific release-on-demand. Macromol Rapid Comm 34: 87–93.    
  • 48. Schlenoff JB, Dubas ST, Farhat T (2000) Sprayed Polyelectrolyte Multilayers. Langmuir 16: 9968–9969.    
  • 49. Patel PA, Dobrynin AV, Mather PT (2007) Combined effect of spin speed and ionic strength on polyelectrolyte spin assembly. Langmuir 23: 12589–12597.    
  • 50. Kiel M, Mitzscherling S, Leitenberger W, et al. (2010) Structural characterization of a spin-assisted colloid-polyelectrolyte assembly: stratified multilayer thin films. Langmuir 26: 18499–18502.    
  • 51. Andres CM, Kotov NA (2010) Inkjet deposition of layer-by-layer assembled films. J Am Chem Soc 132: 14496–14502.    
  • 52. Schmidt DJ, Moskowitz JS, Hammond PT (2011) Electrically Triggered Release of a Small Molecule Drug from a Polyelectrolyte Multilayer Coating. Chem Mater 22: 6416–6425.
  • 53. Owens DK, Wendt RC (1969) Estimation of the surface free energy of polymers. J Appl Polym Sci 13: 1741–1747.    
  • 54. Frutos Cabanillas P, Diez Pena E, Barrales-Rienda JM, et al. (2000) Validation and in vitro characterization of antibiotic-loaded bone cement release. Int J Pharmaceut 209: 15–26.    
  • 55. Tan H, Peng Z, Li Q, et al. (2012) The use of quaternised chitosan-loaded PMMA to inhibit biofilm formation and downregulate the virulence-associated gene expression of antibiotic-resistant staphylococcus. Biomaterials 33: 365–377.    
  • 56. Peterson AM, Pilz-Allen C, Möhwald H, et al. (2014) Evaluation of the role of polyelectrolyte deposition conditions on growth factor release. J Mater Chem B 2: 2680–2687.    
  • 57. Liu TY, Lin YL (2010) Novel pH-sensitive chitosan-based hydrogel for encapsulating poorly water-soluble drugs. Acta Biomater 6: 1423–1429.    
  • 58. Siepmann J, Peppas NA (2001) Modeling of drug release from delivery systems based on hydroxypropyl methylcellulose (HPMC). Adv Drug Deliver Rev 48: 139–157.    
  • 59. von Klitzing R (2006) Internal structure of polyelectrolyte multilayer assemblies. Phys Chem Chem Phys 8: 5012–5033.    
  • 60. Ghostine RA, Markarian MZ, Schlenoff JB (2013) Asymmetric growth in polyelectrolyte multilayers. J Am Chem Soc 135: 7636–7646.    
  • 61. Schoeler B, Sharpe S, Hatton TA, et al. (2004) Polyelectrolyte multilayer films of different charge density copolymers with synergistic nonelectrostatic interactions prepared by the layer-by-layer technique. Langmuir 20: 2730–2738.    
  • 62. Armstrong G, Buggy M (2005) Hydrogen-bonded supramolecular polymers: A literature review. J Mater Sci 40: 547–559.    
  • 63. Abidi N, Hequet E, Cabrales L (2011) Applications of Fourier transform infrared spectroscopy to study cotton fibers, In: Nikolic G, Fourier Transforms-New Analytical Approaches and FTIR Strategies, InTech, 90–114.
  • 64. Moulds RFW, Jeyasingham MS (2010) Gentamicin: A great way to start. Aust Prescr 33: 35–37.
  • 65. Schönhoff M, Ball V, Bausch AR, et al. (2007) Hydration and internal properties of polyelectrolyte multilayers. Colloid Surface A 303: 14–29.
  • 66. Hu N, Frueh J, Zheng C, et al. (2015) Photo-crosslinked natural polyelectrolyte multilayer capsules for drug delivery. Colloid Surface A 482: 315–323.
  • 67. Salvi C, Lyu X, Peterson AM (2016) Effect of assembly pH on polyelectrolyte multilayer surface properties and BMP-2 release. Biomacromolecules 17: 1949–1958.    
  • 68. Schafer T, Pascale A, Shimonaski G, et al. (1972) Evaluation of gentamicin for use in virology and tissue culture. Appl Microbiol 23: 565–570.
  • 69. Berg MC, Zhai L, Cohen RE, et al. (2006) Controlled drug release from porous polyelectrolyte multilayers. Biomacromolecules 7: 357–364.    
  • 70. Siepmann J, Peppas NA (2011) Higuchi equation: derivation, applications, use and misuse. Int J Pharmaceut 418: 6–12.    

 

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Copyright Info: 2017, Amy M. Peterson, et al., licensee AIMS Press. This is an open access article distributed under the terms of the Creative Commons Attribution Licese (http://creativecommons.org/licenses/by/4.0)

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