Inkjet printed drug-releasing polyelectrolyte multilayers for wound dressings

Huilin Yang; Amy M. Peterson; Huilin Yang; Amy M. Peterson

doi:10.3934/matersci.2017.2.452

AIMS Materials Science

2017, Volume 4, Issue 2: 452-469. doi: 10.3934/matersci.2017.2.452

Previous Article Next Article

Research article Topical Sections

Inkjet printed drug-releasing polyelectrolyte multilayers for wound dressings

Huilin Yang ,
Amy M. Peterson ^,

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

Received: 20 December 2016 Accepted: 27 February 2017 Published: 03 March 2017

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.
- 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[J]. AIMS Materials Science, 2017, 4(2): 452-469. doi: 10.3934/matersci.2017.2.452

Related Papers:

Abstract

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.

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. doi: 10.1111/j.1524-475X.2009.00543.x
[2]	Mangoni ML, Mcdermott AM, Zasloff M (2016) Antimicrobial peptides and wound healing: Biological and therapeutic considerations. Exp Dermatol 25: 167–173. doi: 10.1111/exd.12929
[3]	Fahs F, Bi X, Yu FS, et al. (2015) New insights into microRNAs in skin wound healing. IUBMB Life 67: 889–896. doi: 10.1002/iub.1449
[4]	You HJ, Han SK (2014) Cell therapy for wound healing. J Korean Med Sci 29: 311–319. doi: 10.3346/jkms.2014.29.3.311
[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. doi: 10.1002/jps.21210
[6]	Zelikin AN (2010) Drug Releasing Polymer Thin Films: New Era of Surface-Mediated Drug Delivery. ACS Nano 4: 2494–2509. doi: 10.1021/nn100634r
[7]	Delcea M, Möhwald H, Skirtach AG (2011) Stimuli-responsive LbL capsules and nanoshells for drug delivery. Adv Drug Deliver Rev 63: 730–747. doi: 10.1016/j.addr.2011.03.010
[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. doi: 10.1016/S0169-409X(00)00124-1
[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. doi: 10.1016/j.addr.2008.04.016
[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. doi: 10.1016/S0168-3659(01)00248-6
[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. doi: 10.1016/j.biomaterials.2007.10.027
[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. doi: 10.1021/am503750w
[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. doi: 10.1039/c2cs15264a
[17]	Fakhrullin RF, Lvov YM (2012) "Face-Lifting" and "Make-Up" for Microorganisms: Layer-by-Layer Polyelectrolyte Nanocoating. ACS Nano 6: 4557–4564. doi: 10.1021/nn301776y
[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. doi: 10.1016/j.colsurfa.2016.09.052
[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. doi: 10.1002/advs.201600206
[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. doi: 10.1016/j.biomaterials.2010.04.011
[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. doi: 10.1016/j.jconrel.2011.09.062
[22]	Shukla A, Fuller RC, Hammond PT (2011) Design of multi-drug release coatings targeting infection and inflammation. J Control Release 155: 159–166. doi: 10.1016/j.jconrel.2011.06.011
[23]	Teng XR, Shchukin DG, Möhwald H (2008) A Novel Drug Carrier: Lipophilic Drug-Loaded Polyglutamate/Polyelectrolyte Nanocontainers. Langmuir 24: 383–389. doi: 10.1021/la702370k
[24]	Shchukina EM, Shchukin DG (2011) LbL coated microcapsules for delivering lipid-based drugs. Adv Drug Deliver Rev 63: 837–846. doi: 10.1016/j.addr.2011.03.009
[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. doi: 10.1021/ja3019143
[26]	Shukla A, Fleming KE, Chuang HF, et al. (2010) Controlling the release of peptide antimicrobial agents from surfaces. Biomaterials 31: 2348–2357. doi: 10.1016/j.biomaterials.2009.11.082
[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. doi: 10.1016/j.actbio.2011.10.020
[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. doi: 10.1021/la048888i
[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. doi: 10.1016/j.jconrel.2008.03.008
[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. doi: 10.1007/s11095-011-0642-z
[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. doi: 10.1016/j.biomaterials.2011.04.036
[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. doi: 10.1002/smll.200800804
[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. doi: 10.4161/biom.28823
[37]	Seon L, Lavalle P, Schaaf P, et al. (2015) Polyelectrolyte Multilayers: A Versatile Tool for Preparing Antimicrobial Coatings. Langmuir 31: 12856–12872. doi: 10.1021/acs.langmuir.5b02768
[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. doi: 10.1021/ma901356s
[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. doi: 10.1007/s10924-012-0507-5
[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. doi: 10.1016/j.biomaterials.2012.05.068
[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. doi: 10.1016/j.msec.2013.09.001
[43]	Dai J, Bruening ML (2002) Catalytic Nanoparticles Formed by Reduction of Metal Ions in Multilayered Polyelectrolyte Films. Nano Lett 2: 497–501. doi: 10.1021/nl025547l
[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. doi: 10.1073/pnas.0602884103
[46]	Kiryukhin MV, Man SM, Tonoyan A, et al. (2012) Adhesion of polyelectrolyte multilayers: Sealing and transfer of microchamber arrays. Langmuir 28: 5678–5686. doi: 10.1021/la3003004
[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. doi: 10.1002/marc.201200564
[48]	Schlenoff JB, Dubas ST, Farhat T (2000) Sprayed Polyelectrolyte Multilayers. Langmuir 16: 9968–9969. doi: 10.1021/la001312i
[49]	Patel PA, Dobrynin AV, Mather PT (2007) Combined effect of spin speed and ionic strength on polyelectrolyte spin assembly. Langmuir 23: 12589–12597. doi: 10.1021/la7020676
[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. doi: 10.1021/la103609f
[51]	Andres CM, Kotov NA (2010) Inkjet deposition of layer-by-layer assembled films. J Am Chem Soc 132: 14496–14502. doi: 10.1021/ja104735a
[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. doi: 10.1002/app.1969.070130815
[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. doi: 10.1016/S0378-5173(00)00520-2
[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. doi: 10.1016/j.biomaterials.2011.09.084
[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. doi: 10.1039/c3tb21757d
[57]	Liu TY, Lin YL (2010) Novel pH-sensitive chitosan-based hydrogel for encapsulating poorly water-soluble drugs. Acta Biomater 6: 1423–1429. doi: 10.1016/j.actbio.2009.10.010
[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. doi: 10.1016/S0169-409X(01)00112-0
[59]	von Klitzing R (2006) Internal structure of polyelectrolyte multilayer assemblies. Phys Chem Chem Phys 8: 5012–5033. doi: 10.1039/b607760a
[60]	Ghostine RA, Markarian MZ, Schlenoff JB (2013) Asymmetric growth in polyelectrolyte multilayers. J Am Chem Soc 135: 7636–7646. doi: 10.1021/ja401318m
[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. doi: 10.1021/la035909k
[62]	Armstrong G, Buggy M (2005) Hydrogen-bonded supramolecular polymers: A literature review. J Mater Sci 40: 547–559. doi: 10.1007/s10853-005-6288-7
[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. doi: 10.1021/acs.biomac.5b01730
[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. doi: 10.1021/bm050174e
[70]	Siepmann J, Peppas NA (2011) Higuchi equation: derivation, applications, use and misuse. Int J Pharmaceut 418: 6–12. doi: 10.1016/j.ijpharm.2011.03.051

Reader Comments

Your name:*

Email:*
© 2017 the Author(s), licensee AIMS Press. This is an open access article distributed under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/4.0)