Rheological study of in-situ crosslinkable hydrogels based on hyaluronanic acid, collagen and sericin.
The elaboration of chemically crosslinked hydrogels based on collagen (C), hyaluronanic acid (HA) and sericin (S) with different polymer ratios was investigated by in-situ rheology. This reaction was performed via amide or ester bond reaction activated by carbodiimide, in pure water. Prior to molecule crosslinking, the rheological behaviour of the biopolymers (alone or in mixture) was characterized in a semi-dilute concentration regime. Both flow and dynamic measurements showed that uncrosslinked collagen alone appears to be rather elastic with yield stress properties, whereas uncrosslinked HA alone appears to be rather shear thinning and viscoelastic in agreement with entangled polymer behaviour. Sericin exhibited Newtonian low viscosity behaviour according to its very low molar mass. Before crosslinking, HA exhibited viscoelastic behaviour at concentrations above the critical entangled concentration (C*) in the mixtures, thus HA shows promise as a matrix for future crosslinked networks, whereas sericin did not significantly modify the rheology. During the reaction, followed by rheology, the kinetics were slower for pure HA systems compared with the mixtures (i.e., with added collagen and/or to a lesser extent sericin). At the same time, the final network of hydrogels (i.e., the elastic modulus) was more structured in the mixture based systems. This result is explained by ester bonds (the only possibility for pure HA systems), which are less favourable and reactive than amide bonds (possible with sericin and collagen). The presence of collagen in the HA matrix reinforced the hydrogel network. SEM studies confirmed the structure of the hydrogels, and in vitro degradability was globally consistent with the effect of the selected enzyme according to the hydrogel composition. All the elaborated hydrogels were non-cytotoxic in vitro.
"Gheorghe Asachi" Technical University, Faculty of Chemical Engineering and Environmental Protection, Department of Natural and Synthetic Polymers, 73 Prof. Dr. docent Dimitrie Mangeron Street, 700050 Iasi, Romania; Université de Rouen, Laboratoire Polymères Biopolymères Surfaces, F-76821 Mont Saint Aignan, France.
Raluca
R
Vulpe
Normandie Université, France; Université de Rouen, Laboratoire Polymères Biopolymères Surfaces, F-76821 Mont Saint Aignan, France; CNRS UMR 6270 & FR3038, F-76821 Mont Saint Aignan, France.
Didier
D
Le Cerf
Normandie Université, France; Université de Rouen, Laboratoire Polymères Biopolymères Surfaces, F-76821 Mont Saint Aignan, France; CNRS UMR 6270 & FR3038, F-76821 Mont Saint Aignan, France.
Virginie
V
Dulong
"Gheorghe Asachi" Technical University, Faculty of Chemical Engineering and Environmental Protection, Department of Natural and Synthetic Polymers, 73 Prof. Dr. docent Dimitrie Mangeron Street, 700050 Iasi, Romania; Academy of Romanian Scientists, Splaiul Independentei, 54, Sector 5, 050094, Bucuresti, Romania; "Apollonia" University of Iași, Faculty of Dental Medicine, Muzicii Avenue, 2, 700399, Iasi, Romania.
Marcel
M
Popa
"Gheorghe Asachi" Technical University, Faculty of Chemical Engineering and Environmental Protection, Department of Natural and Synthetic Polymers, 73 Prof. Dr. docent Dimitrie Mangeron Street, 700050 Iasi, Romania.
Catalina
C
Peptu
"Grigore T. Popa" University of Medicine and Pharmacy, Faculty of Medical Bioengineering, Department of Biological Sciences, 9-13 Kogalniceanu Street, 700454 Iasi, Romania.
Liliana
L
Verestiuc
Normandie Université, France; Université de Rouen, Laboratoire Polymères Biopolymères Surfaces, F-76821 Mont Saint Aignan, France; CNRS UMR 6270 & FR3038, F-76821 Mont Saint Aignan, France. Electronic address: luc.picton@univ-rouen.fr.
Luc
L
Picton
D001672:Biocompatible Materials / Q000737:chemistry / Q000494:pharmacology; D002460:Cell Line; D002470:Cell Survival / Q000187:drug effects; D003094:Collagen / Q000737:chemistry*; D006801:Humans; D006820:Hyaluronic Acid / Q000737:chemistry*; D020100:Hydrogels / Q000737:chemistry*; D008855:Microscopy, Electron, Scanning; D012212:Rheology; D047030:Sericins / Q000737:chemistry*; D014783:Viscosity; D014867:Water / Q000737:chemistry
D001672:Biocompatible Materials; D020100:Hydrogels; D047030:Sericins; D014867:Water; D006820:Hyaluronic Acid; D003094:Collagen
Collagen; Hyaluronan; Hydrogels; Rheological behaviour; Sericin