Synergistic effects of crosslinking and chitosan molecular weight on the microstructure, molecular mobility, thermal and sorption properties of porous chitosan/gelatin/hyaluronic acid scaffolds

In this study, synergistic effects of crosslinking and chitosan molecular weight on the microstructure, molecular mobility, thermal, and sorption properties of porous chitosan/gelatin/hyaluronic acid hybrid foams are reported. Fourier transform infrared spectroscopy has been utilized to confirm the covalent attachment of hyaluronic acid to gelatin and chitosan, and covalent chemical crosslinking between gelatin and chitosan. Detailed image analysis of scanning electron microscopy images of the porous scaffold hydrids reveal that the pore size of the materials formulated using either low- or high-molecular-weight chitosan increases significantly upon crosslinking using ethyl(dimethylaminopropyl) carbodiimide/N-Hydroxysuccinimide. These microstructural changes are even more pronounced for the crosslinked hybrid scaffolds formulated using low-molecular-weight chitosan, highlighting a synergistic effect between crosslinking and the use of low-molecular-weight chitosan. Results obtained using differential scanning calorimetry demonstrate a significant reduction in molecular mobility reduction in molecular mobility for crosslinked scaffolds formed using high-molecular-weight chitosan compared to non-crosslinked hybrids and crosslinked hybrids formulated using low-molecular-weight chitosan. Correspondingly, dynamic vapor sorption evidenced significantly lower water vapor sorption for crosslinked scaffolds formulated using high-molecular-weight chitosan. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017, 134, 44772.

[1]  H. Mirzadeh,et al.  Effect of crosslinking procedure on structural, thermal, and functional performances of cellulosic nanofibers: A comparison between chemical and photochemical crosslinking , 2016 .

[2]  J. Delgado,et al.  Biocompatible scaffolds composed of chemically crosslinked chitosan and gelatin for tissue engineering , 2016 .

[3]  Jens Rumschöttel,et al.  Janus emulsion mediated porous scaffold bio-fabrication. , 2016, Colloids and surfaces. B, Biointerfaces.

[4]  B. Gupta,et al.  Understanding the in situ crosslinked gelatin hydrogel , 2016 .

[5]  Jia‐Horng Lin,et al.  Chitosan/gelatin porous bone scaffolds made by crosslinking treatment and freeze-drying technology: Effects of crosslinking durations on the porous structure, compressive strength, and in vitro cytotoxicity , 2015 .

[6]  V. Kokol,et al.  Molecular mobility of scaffolds' biopolymers influences cell growth. , 2014, ACS applied materials & interfaces.

[7]  Hanna Staroszczyk,et al.  Interactions of fish gelatin and chitosan in uncrosslinked and crosslinked with EDC films: FT-IR study. , 2014, Spectrochimica acta. Part A, Molecular and biomolecular spectroscopy.

[8]  G. Luo,et al.  Blockade of the Formation of Insoluble Ubiquitinated Protein Aggregates by EGCG3”Me in the Alloxan-Induced Diabetic Kidney , 2013, PloS one.

[9]  Cleo Choong,et al.  Three-dimensional scaffolds for tissue engineering applications: role of porosity and pore size. , 2013, Tissue engineering. Part B, Reviews.

[10]  E. Sánchez,et al.  Designing a gelatin/chitosan/hyaluronic acid biopolymer using a thermophysical approach for use in tissue engineering , 2013, Bioprocess and Biosystems Engineering.

[11]  E. Sánchez,et al.  Improvement of human skin cell growth by radiation-induced modifications of a Ge/Ch/Ha scaffold , 2013, Bioprocess and Biosystems Engineering.

[12]  T. Trindade,et al.  Effects of Au nanoparticles on thermoresponsive genipin-crosslinked gelatin hydrogels , 2013, Gold Bulletin.

[13]  Cheol-Sang Kim,et al.  Electrospun gelatin/nylon‐6 composite nanofibers for biomedical applications , 2012 .

[14]  A. Gandini,et al.  Novel materials based on chitosan and cellulose , 2011 .

[15]  Sanjay R. Mishra,et al.  Effect of molecular weight of chitosan degraded by microwave irradiation on lyophilized scaffold for bone tissue engineering applications. , 2011, Journal of biomedical materials research. Part A.

[16]  A A Schäffer,et al.  Early-onset inflammatory bowel disease caused by mutant IL10 receptor , 2010, Journal of Translational Medicine.

[17]  F. O'Brien,et al.  Substrate stiffness and contractile behaviour modulate the functional maturation of osteoblasts on a collagen-GAG scaffold. , 2010, Acta biomaterialia.

[18]  C. Acevedo,et al.  The effect of an autologous cellular gel-matrix integrated implant system on wound healing , 2010, Journal of Translational Medicine.

[19]  A. Shelton,et al.  Changes in neuronal activation patterns in response to androgen deprivation therapy: a pilot study , 2010, BMC Cancer.

[20]  R. Misra,et al.  Chitosan-gelatin scaffolds for tissue engineering: physico-chemical properties and biological response of buffalo embryonic stem cells and transfectant of GFP-buffalo embryonic stem cells. , 2009, Acta biomaterialia.

[21]  C. Pillai,et al.  Chitin and chitosan polymers: Chemistry, solubility and fiber formation , 2009 .

[22]  R. Misra,et al.  Biomimetic chitosan-nanohydroxyapatite composite scaffolds for bone tissue engineering. , 2009, Acta biomaterialia.

[23]  S. Gunasekaran,et al.  Spectral investigation and normal coordinate analysis of piperazine , 2008 .

[24]  Maria J. Sousa-Gallagher,et al.  Mathematical modelling of the kinetic of quality deterioration of intermediate moisture content banana during storage , 2008 .

[25]  S. Hill,et al.  Sorption behavior of mixtures of glycerol and starch. , 2007, Journal of agricultural and food chemistry.

[26]  Yilin Cao,et al.  Influence of the concentrations of hyaluronic acid on the properties and biocompatibility of Cs-Gel-HA membranes. , 2004, Biomaterials.

[27]  Kangde Yao,et al.  A study on a chitosan-gelatin-hyaluronic acid scaffold as artificial skin in vitro and its tissue engineering applications , 2004, Journal of biomaterials science. Polymer edition.

[28]  Xiu-lan Li,et al.  Preparation and characterization of macroporous chitosan-gelatin/beta-tricalcium phosphate composite scaffolds for bone tissue engineering. , 2003, Journal of biomedical materials research. Part A.

[29]  W. J. Wang,et al.  Crosslinked collagen/chitosan matrix for artificial livers. , 2003, Biomaterials.

[30]  J. Mao,et al.  The properties of chitosan-gelatin membranes and scaffolds modified with hyaluronic acid by different methods. , 2003, Biomaterials.

[31]  S. Guilbert,et al.  Distribution of Water between Wheat Flour Components: A Dynamic Water Vapour Adsorption Study , 2002 .

[32]  T. Ma,et al.  Effects of pore size in 3-D fibrous matrix on human trophoblast tissue development. , 2000, Biotechnology and bioengineering.

[33]  M. N. R. Kumar.  A review of chitin and chitosan applications , 2000 .

[34]  S. Hirano.  Chitin and chitosan as novel biotechnological materials , 1999 .

[35]  G. W. Small.  Spectrometric Identification of Organic Compounds , 1992 .

[36]  G. Poncelet,et al.  Influence of the Van der Waals force on the infrared spectra of short aliphatic alkylammonium cations held on montmorillonite , 1969, Clay Minerals.

[37]  L. Segal'.  SPECTROPHOTOMETRIC EVIDENCE FOR INTERACTION BETWEEN CHLOROFORM AND MONOETHYLAMINE , 1961 .

[38]  Yuan Lu,et al.  Effects of chitosan molecular weight and degree of deacetylation on the properties of gelatine-based films , 2012 .

[39]  Changyou Gao,et al.  Gelatin/chitosan/hyaluronan scaffold integrated with PLGA microspheres for cartilage tissue engineering. , 2009, Acta biomaterialia.

[40]  J. V. García-Pérez,et al.  Water sorption isotherms for lemon peel at different temperatures and isosteric heats , 2008 .

[41]  M. Diem,et al.  Infrared spectroscopy of human tissue. III. Spectral differences between squamous and columnar tissue and cells from the human cervix , 1997 .

[42]  J. H. de Boer,et al.  The dynamical character of adsorption , 1968 .

[43]  E. A. Guggenheim.  Applications of Statistical Mechanics , 1966 .