Application of response surface methodology to tailor the surface chemistry of electrospun chitosan-poly(ethylene oxide) fibers.

Chitosan is a promising biocompatible polymer for regenerative engineering applications, but its processing remains challenging due to limited solubility and rigid crystalline structure. This work represents the development of electrospun chitosan/poly(ethylene oxide) blend nanofibrous membranes by means of a numerical analysis in order to identify and tailor the main influencing parameters with respect to accessible surface nitrogen functionalities which are of importance for the biological activity as well as for further functionalization. Depending on the solution composition, both gradient fibers and homogenous blended fiber structures could be obtained with surface nitrogen concentrations varying between 0 and 6.4%. Response surface methodology (RSM) revealed chitosan/poly(ethylene oxide) ratio and chitosan molecular weight as the main influencing factors with respect to accessible nitrogen surface atoms and respective concentrations. The model showed good adequacy hence providing a tool to tailor the surface properties of chitosan/poly(ethylene oxide) blends by addressing the amount of accessible chitosan.

[1]  Xiguang Chen,et al.  Investigation of acetylated chitosan microspheres as potential chemoembolic agents. , 2014, Colloids and surfaces. B, Biointerfaces.

[2]  H. Park,et al.  Preparation and biocompatibility of chitosan microcarriers as biomaterial , 2006 .

[3]  L. Carvalho,et al.  Application of Infrared Spectroscopy to Analysis of Chitosan/Clay Nanocomposites , 2012 .

[4]  Thierry Delair,et al.  Typical physicochemical behaviors of chitosan in aqueous solution. , 2003, Biomacromolecules.

[5]  P. Agarwal,et al.  Statistical optimization of the electrospinning process for chitosan/polylactide nanofabrication using response surface methodology , 2012, Journal of Materials Science.

[6]  M. Mucha.  Rheological properties of chitosan blends with poly(ethylene oxide) and poly(vinyl alcohol) in solution , 1998 .

[7]  M. Heuzey,et al.  Core-shell structured PEO-chitosan nanofibers by coaxial electrospinning. , 2012, Biomacromolecules.

[8]  Xiguang Chen,et al.  Optimization and characteristics of preparing chitosan microspheres using response surface methodology , 2013 .

[9]  Derek J. Pike,et al.  Empirical Model‐building and Response Surfaces. , 1988 .

[10]  S. Jeyamkonda,et al.  Microbial growth modelling with artificial neural networks. , 2001, International journal of food microbiology.

[11]  S. Honary,et al.  Effect of Zeta Potential on the Properties of Nano-Drug Delivery Systems - A Review (Part 2) , 2013 .

[12]  M. Buschmann,et al.  High efficiency gene transfer using chitosan/DNA nanoparticles with specific combinations of molecular weight and degree of deacetylation. , 2006, Biomaterials.

[13]  L. Matienzo,et al.  Dry Processes for Surface Modification of a Biopolymer: Chitosan , 2002 .

[14]  S. Ramakrishna,et al.  Chitosan nanofibers from an easily electrospinnable UHMWPEO-doped chitosan solution system. , 2008, Biomacromolecules.

[15]  O. Damour,et al.  Influence of the degree of acetylation on some biological properties of chitosan films. , 2001, Biomaterials.

[16]  D. Liang,et al.  Memory effect on solution crystallization of high molecular weight poly(ethylene oxide) , 2012 .

[17]  Y. Hsieh,et al.  Chitosan bicomponent nanofibers and nanoporous fibers. , 2006, Carbohydrate research.

[18]  V. Sutariya,et al.  Reversed chitosan-alginate polyelectrolyte complex for stability improvement of alpha-amylase: optimization and physicochemical characterization. , 2007, European journal of pharmaceutics and biopharmaceutics : official journal of Arbeitsgemeinschaft fur Pharmazeutische Verfahrenstechnik e.V.

[19]  Michael W. Peck,et al.  Predictive Model Describing the Effect of Prolonged Heating at 70 to 80°C and Incubation at Refrigeration Temperatures on Growth and Toxigenesis by Nonproteolylic Clostridium botulinum. , 1997, Journal of food protection.

[20]  A. Domard,et al.  Physicochemical behavior of homogeneous series of acetylated chitosans in aqueous solution: role of various structural parameters. , 2005, Biomacromolecules.

[21]  J. Nie,et al.  Fabrication of core–shell nanofibers by single capillary electrospinning combined with vapor induced phase separation , 2013 .

[22]  K. Leong,et al.  The effect of the degree of chitosan deacetylation on the efficiency of gene transfection. , 2004, Biomaterials.

[23]  R. Rossi,et al.  Molecular weight driven structure formation of PEG based e-spun polymer blend fibres , 2014 .

[24]  F. Zhao,et al.  Regulation of vascular smooth muscle cells on poly(ethylene terephthalate) film by O-carboxymethylchitosan surface immobilization. , 2008, Journal of biomedical materials research. Part A.

[25]  Xianqun Fan,et al.  Electrospun chitosan-graft-poly (ɛ-caprolactone)/poly (ɛ-caprolactone) nanofibrous scaffolds for retinal tissue engineering , 2011, International journal of nanomedicine.

[26]  S. Küçükbayrak,et al.  Evaluation of the factors influencing the resultant diameter of the electrospun gelatin/sodium alginate nanofibers via Box-Behnken design. , 2016, Materials science & engineering. C, Materials for biological applications.

[27]  Douglas C. Montgomery,et al.  Response Surface Methodology: Process and Product Optimization Using Designed Experiments , 1995 .

[28]  Miqin Zhang,et al.  Electrospun chitosan-based nanofibers and their cellular compatibility. , 2005, Biomaterials.

[29]  R. Rossi,et al.  Tunable release of hydrophilic compounds from hydrophobic nanostructured fibers prepared by emulsion electrospinning , 2015 .

[30]  M. Abraham,et al.  Solubility characteristics of poly(ethylene oxide): Effect of molecular weight, end groups and temperature , 1994 .

[31]  M N Hajmeer,et al.  Computational neural networks for predictive microbiology. II. Application to microbial growth. , 1997, International journal of food microbiology.

[32]  Senentxu Lanceros-Méndez,et al.  Role of Nanoparticle Surface Charge on the Nucleation of the Electroactive β-Poly(vinylidene fluoride) Nanocomposites for Sensor and Actuator Applications , 2012 .

[33]  Christine Jérôme,et al.  Development of a chitosan nanofibrillar scaffold for skin repair and regeneration. , 2011, Biomacromolecules.

[34]  K. Kit,et al.  Nanofibrous chitosan non-wovens for filtration applications , 2009 .

[35]  Saied Nouri Khorasani,et al.  Characterization of gelatin/cellulose acetate nanofibrous scaffolds: Prediction and optimization by response surface methodology and artificial neural networks , 2016, Polymer Science Series A.

[36]  Xiguang Chen,et al.  Protonation constants of chitosan with different molecular weight and degree of deacetylation , 2006 .

[37]  Derek L. Ho,et al.  Unusual phase behavior in mixtures of poly(ethylene oxide) and ethyl alcohol , 2006 .

[38]  M. Hasik,et al.  FT-IR study of montmorillonite-chitosan nanocomposite materials. , 2011, Spectrochimica acta. Part A, Molecular and biomolecular spectroscopy.

[39]  M. Mucha.  Rheological characteristics of semi‐dilute chitosan solutions , 1997 .

[40]  M. Yılmaz,et al.  A Novel Approach to Limit Chemical Deterioration of Gilthead Sea Bream (Sparus aurata) Fillets: Coating with Electrospun Nanofibers as Characterized by Molecular, Thermal, and Microstructural Properties. , 2017, Journal of food science.

[41]  Thomas E Oscar,et al.  Validation of Lag Time and Growth Rate Models for Salmonella Typhimurium: Acceptable Prediction Zone Method , 2005 .

[42]  X. D. Wang,et al.  The controlling biodegradation of chitosan fibers by N-acetylation in vitro and in vivo , 2007, Journal of materials science. Materials in medicine.

[43]  J. Hilborn,et al.  Emulsion Electrospinning as an Approach to Fabricate PLGA/Chitosan Nanofibers for Biomedical Applications , 2014, BioMed research international.

[44]  N. Wagner,et al.  Theory and kinematic measurements of the mechanics of stable electrospun polymer jets , 2008 .

[45]  V. Sivakumar,et al.  Preparation of Chitosan based Nanofibers: Optimization and Modeling , 2015 .

[46]  S. Bo,et al.  Determination of the Mark-Houwink equation for chitosans with different degrees of deacetylation. , 1991, International journal of biological macromolecules.

[47]  D. Reneker,et al.  Dynamics of Hollow Nanofiber Formation During Solidification Subjected to Solvent Evaporation , 2006 .

[48]  Jack L. Koenig,et al.  A review of polymer dissolution , 2003 .

[49]  J. Nie,et al.  Electrospun Core−Shell Structure Nanofibers from Homogeneous Solution of Poly(ethylene oxide)/Chitosan , 2009 .

[50]  J Baranyi,et al.  Mathematics of predictive food microbiology. , 1995, International journal of food microbiology.

[51]  Jun Kameoka,et al.  Polymeric Nanowire Chemical Sensor , 2004 .

[52]  A. A. Gharehaghaji,et al.  Fabrication of Electrospun Polyamide-6/Chitosan Nanofibrous Membrane toward Anionic Dyes Removal , 2014 .

[53]  Xiaoyan Yuan,et al.  Electrospinning of chitosan solutions in acetic acid with poly(ethylene oxide) , 2004, Journal of biomaterials science. Polymer edition.

[54]  C. Jérôme,et al.  Polysaccharide‐Coated PCL Nanofibers for Wound Dressing Applications , 2014, Advanced healthcare materials.

[55]  P. Kocbek,et al.  Development and bioevaluation of nanofibers with blood-derived growth factors for dermal wound healing. , 2014, European journal of pharmaceutics and biopharmaceutics : official journal of Arbeitsgemeinschaft fur Pharmazeutische Verfahrenstechnik e.V.

[56]  Xingyou Hu,et al.  Composite chitosan/poly(ethylene oxide) electrospun nanofibrous mats as novel wound dressing matrixes for the controlled release of drugs , 2015 .

[57]  Abdellah Ajji,et al.  A fundamental study of chitosan/PEO electrospinning , 2011 .

[58]  F. Besenbacher,et al.  Electrospinning of uniform polystyrene fibers : The effect of solvent conductivity , 2008 .

[59]  Won Il Kim,et al.  Nanofiber mats composed of a chitosan-poly(d,l-lactic-co-glycolic acid)-poly(ethylene oxide) blend as a postoperative anti-adhesion agent. , 2017, Journal of biomedical materials research. Part B, Applied biomaterials.

[60]  Gary E. Wnek,et al.  Role of chain entanglements on fiber formation during electrospinning of polymer solutions: Good solvent, non-specific polymer-polymer interaction limit , 2005 .

[61]  F. Bossard,et al.  Preparation of Pure and Stable Chitosan Nanofibers by Electrospinning in the Presence of Poly(ethylene oxide) , 2016, International journal of molecular sciences.

[62]  C. Sung,et al.  Core‐Sheath Structure in Electrospun Nanofibers from Polymer Blends , 2006 .

[63]  G. Sánchez,et al.  Impact of molecular weight on the formation of electrosprayed chitosan microcapsules as delivery vehicles for bioactive compounds. , 2016, Carbohydrate polymers.

[64]  M. Horne,et al.  Review Paper: A Review of the Cellular Response on Electrospun Nanofibers for Tissue Engineering , 2009, Journal of biomaterials applications.

[65]  D. Paneva,et al.  Preparation of chitosan-containing nanofibres by electrospinning of chitosan/poly(ethylene oxide) blend solutions , 2004 .

[66]  A. M. Shoushtari,et al.  Fabrication of high performance chitosan/polyvinyl alcohol nanofibrous mat with controlled morphology and optimised diameter , 2014 .

[67]  B. Marí,et al.  Determining the influence of N-acetylation on water sorption in chitosan films. , 2015, Carbohydrate polymers.

[68]  M. Heuzey,et al.  Determination of Phase Behavior of Poly(ethylene oxide) and Chitosan Solution Blends Using Rheometry , 2012 .

[69]  A. Kishan,et al.  In situ crosslinking of electrospun gelatin for improved fiber morphology retention and tunable degradation. , 2015, Journal of materials chemistry. B.

[70]  R. Rossi,et al.  Encapsulation of polyphenols into pHEMA e-spun fibers and determination of their antioxidant activities. , 2015, International journal of pharmaceutics.

[71]  F. Besenbacher,et al.  Thermo-responsive core-sheath electrospun nanofibers from poly (N-isopropylacrylamide)/polycaprolactone blends , 2010 .

[72]  M. Irani,et al.  Electrospun nanofiber membrane of PEO/Chitosan for the adsorption of nickel, cadmium, lead and copper ions from aqueous solution , 2013 .

[73]  H. Tadokoro,et al.  Normal Vibrations of the Polymer Molecules of Helical Conformation. IV. Polyethylene Oxide and Polyethylene‐d4 Oxide , 1964 .

[74]  Gary E. Wnek,et al.  Electrospinning and Stabilization of Fully Hydrolyzed Poly(Vinyl Alcohol) Fibers , 2003 .

[75]  O. Kwon,et al.  Electrospinning of chitosan dissolved in concentrated acetic acid solution. , 2005, Biomaterials.

[76]  Piotr Stepnowski,et al.  Application of Spectroscopic Methods for Structural Analysis of Chitin and Chitosan , 2010, Marine drugs.

[77]  Young-Jin Kim,et al.  Fabrication of poly(vinyl acetate)/polysaccharide biocomposite nanofibrous membranes for tissue engineering , 2013, Macromolecular Research.

[78]  Jessica D. Schiffman,et al.  Electrospinning chitosan/poly(ethylene oxide) solutions with essential oils: Correlating solution rheology to nanofiber formation. , 2016, Carbohydrate polymers.

[79]  W. Krause,et al.  Correlation of chitosan's rheological properties and its ability to electrospin. , 2007, Biomacromolecules.

[80]  A. Muffler,et al.  The use of a radial basis neural network and genetic algorithm for improving the efficiency of laccase-mediated dye decolourization. , 2012, Journal of biotechnology.

[81]  Thomas Kissel,et al.  In vitro cytotoxicity testing of polycations: influence of polymer structure on cell viability and hemolysis. , 2003, Biomaterials.

[82]  G. Patzke,et al.  Synthesis and screening of N-acyl thiolated chitosans for antibacterial applications. , 2016, Carbohydrate polymers.

[83]  George E. P. Box,et al.  Empirical Model‐Building and Response Surfaces , 1988 .

[84]  Eleonore Fröhlich,et al.  The role of surface charge in cellular uptake and cytotoxicity of medical nanoparticles , 2012, International journal of nanomedicine.

[85]  Shun-Hsien Chang,et al.  pH Effects on solubility, zeta potential, and correlation between antibacterial activity and molecular weight of chitosan. , 2015, Carbohydrate polymers.

[86]  D. Mcclements,et al.  Electrospinning of chitosan–poly(ethylene oxide) blend nanofibers in the presence of micellar surfactant solutions , 2009 .

[87]  G. Guebitz,et al.  Antimicrobial Cellobiose Dehydrogenase-Chitosan Particles. , 2016, ACS applied materials & interfaces.

[88]  T. Carrel,et al.  Fine-tuning of substrate architecture and surface chemistry promotes muscle tissue development. , 2012, Acta biomaterialia.

[89]  Yan Huang,et al.  In vitro characterization of chitosan-gelatin scaffolds for tissue engineering. , 2005, Biomaterials.

[90]  R. Bellamkonda,et al.  The polarity and magnitude of ambient charge influences three-dimensional neurite extension from DRGs. , 2000, Journal of biomedical materials research.

[91]  F. Besenbacher,et al.  Ultraporous interweaving electrospun microfibers from PCL-PEO binary blends and their inflammatory responses. , 2014, Nanoscale.

[92]  Jessica D. Schiffman,et al.  Cross-linking chitosan nanofibers. , 2007, Biomacromolecules.

[93]  Ming Kong,et al.  Preparation of biocompatible chitosan grafted poly(lactic acid) nanoparticles. , 2012, International journal of biological macromolecules.

[94]  Ming Kong,et al.  In vitro and in vivo evaluation of chitosan microspheres with different deacetylation degree as potential embolic agent. , 2014, Carbohydrate polymers.

[95]  O. Smidsrod,et al.  Solution properties of chitosans: conformation and chain stiffness of chitosans with different degrees of N-acetylation , 1993 .

[96]  M. Maaza,et al.  Optimization of Electrospinning Parameters for Chitosan Nanofibres , 2011 .

[97]  Federica Chiellini,et al.  Chitosan—A versatile semi-synthetic polymer in biomedical applications , 2011 .

[98]  M. Nouri,et al.  Optimization of chitosan-polyvinylalcohol electrospinning process by response surface methodology (RSM) , 2010 .

[99]  M. Dilamian,et al.  Nanofibrous Chitosan-Polyethylene Oxide Engineered Scaffolds: A Comparative Study between Simulated Structural Characteristics and Cells Viability , 2014, BioMed research international.

[100]  K. Kit,et al.  Morphological and surface properties of electrospun chitosan nanofibers. , 2008, Biomacromolecules.

[101]  R. García-Gimeno,et al.  Predictive Model of Listeria Monocytogenes’ Growth Rate Under Different Temperatures and Acids , 2006 .

[102]  J. Desbrières,et al.  Influence of acetic acid concentration on the solubilization of chitosan , 1999 .

[103]  M. A. d’Ávila,et al.  Non-woven nanofiber chitosan/peo membranes obtained by electrospinning , 2014 .

[104]  Digvir S. Jayas,et al.  Microbial growth modelling with artificial neural networks. , 2001 .

[105]  Wilfried Weigel,et al.  XPS and NEXAFS studies of aliphatic and aromatic amine species on functionalized surfaces , 2009 .

[106]  Xiaoyuan Wang,et al.  Controlled release of protein from core–shell nanofibers prepared by emulsion electrospinning based on green chemical , 2015 .

[107]  C. Fong,et al.  Transfection efficiency of chitosan vectors: effect of polymer molecular weight and degree of deacetylation. , 2005, Journal of controlled release : official journal of the Controlled Release Society.