Characterization of Chitosan/Hyaluronan Complex Coacervates Assembled by Varying Polymers Weight Ratio and Chitosan Physical-Chemical Composition

Herein, we synthetized and characterized polysaccharide-based complex coacervates starting from two water-soluble biopolymers, i.e., hydrochloride chitosans and sodium hyaluronan. We used chitosans encompassing a range of molecular weights from 30,000 to 400,000 and showing different fraction of acetylated units (i.e., FA = 0.16, 0.46, and 0.63). This set of chitosans was mixed with a low molecular weight hyaluronan to promote electrostatic interactions. Resulting colloids were analyzed in terms of size, polydispersity and surface charge by Dynamic Light Scattering. The weight ratio between the two polyelectrolytes was studied as additional parameter influencing the liquid-liquid phase separation. Main results include the following: the polymers weight ratio was fundamental in dictating the colloids surface charge, whereas chitosan physical-chemical features influenced the dimension and homogeneity of colloids. This contribution presents additional understanding of the complex coacervation between these two oppositely charged polysaccharides, with the potential translation of present system in food and biomedical sectors.

[1]  I. Donati,et al.  N-isopropyl chitosan. A pH- and thermo-responsive polysaccharide for gel formation. , 2020, Carbohydrate polymers.

[2]  K. K. Asha,et al.  Chitosan - Whey protein as efficient delivery system for squalene: Characterization and functional food application. , 2019, International journal of biological macromolecules.

[3]  I. Donati,et al.  Chitosan Acetylation Degree Influences the Physical Properties of Polysaccharide Nanoparticles: Implication for the Innate Immune Cells Response. , 2019, ACS applied materials & interfaces.

[4]  B. S. de Farias,et al.  Chitosan-functionalized nanofibers: A comprehensive review on challenges and prospects for food applications. , 2019, International journal of biological macromolecules.

[5]  J. Spadavecchia,et al.  Lactose-Modified Chitosan Gold(III)-PEGylated Complex-Bioconjugates: From Synthesis to Interaction with Targeted Galectin-1 Protein. , 2018, Bioconjugate chemistry.

[6]  G. Turco,et al.  Complex Coacervates between a Lactose-Modified Chitosan and Hyaluronic Acid as Radical-Scavenging Drug Carriers. , 2018, Biomacromolecules.

[7]  I. Donati,et al.  The role played by the molecular weight and acetylation degree in modulating the stiffness and elasticity of chitosan gels. , 2018, Carbohydrate polymers.

[8]  I. Donati,et al.  Concepts for Developing Physical Gels of Chitosan and of Chitosan Derivatives , 2018, Gels.

[9]  Francesca Cuomo,et al.  Effect of the coexistence of sodium caseinate and Tween 20 as stabilizers of food emulsions at acidic pH. , 2018, Colloids and surfaces. B, Biointerfaces.

[10]  M. Guo,et al.  Antimicrobial edible coatings and films from micro-emulsions and their food applications. , 2017, International journal of food microbiology.

[11]  B. Lindman,et al.  In-vitro digestion of curcumin loaded chitosan-coated liposomes. , 2017, Colloids and surfaces. B, Biointerfaces.

[12]  I. Donati,et al.  Highly monodisperse colloidal coacervates based on a bioactive lactose-modified chitosan: From synthesis to characterization. , 2017, Carbohydrate polymers.

[13]  E. Dickinson.  On the road to understanding and control of creaminess perception in food colloids , 2017 .

[14]  K. Vårum,et al.  Butyrate-Loaded Chitosan/Hyaluronan Nanoparticles: A Suitable Tool for Sustained Inhibition of ROS Release by Activated Neutrophils. , 2017, Macromolecular bioscience.

[15]  Shakeel Ahmed,et al.  Chitosan: Derivatives, Composites and Applications , 2017 .

[16]  I. Stratford,et al.  Chitosan/Hyaluronic Acid Nanoparticles: Rational Design Revisited for RNA Delivery. , 2017, Molecular pharmaceutics.

[17]  D. Mcclements.  The future of food colloids: Next-generation nanoparticle delivery systems , 2017 .

[18]  Ji-bao Cai,et al.  Polysaccharide-based nanoparticles by chitosan and gum arabic polyelectrolyte complexation as carriers for curcumin , 2016 .

[19]  P. Aramwit,et al.  The development of non-toxic ionic-crosslinked chitosan-based microspheres as carriers for the controlled release of silk sericin , 2015, Biomedical microdevices.

[20]  Eric Dickinson,et al.  Colloids in food: ingredients, structure, and stability. , 2015, Annual review of food science and technology.

[21]  K. Draget,et al.  Chitosan: Gels and Interfacial Properties , 2015 .

[22]  Yangchao Luo,et al.  Recent development of chitosan-based polyelectrolyte complexes with natural polysaccharides for drug delivery. , 2014, International journal of biological macromolecules.

[23]  Philip J Day,et al.  Hyaluronic acid-coated chitosan nanoparticles: molecular weight-dependent effects on morphology and hyaluronic acid presentation. , 2013, Journal of controlled release : official journal of the Controlled Release Society.

[24]  Y. Zambito,et al.  Mucoadhesive nanoparticles made of thiolated quaternary chitosan crosslinked with hyaluronan. , 2013, Carbohydrate polymers.

[25]  M. Santos-Martinez,et al.  Exploring the assembly process and properties of novel crosslinker-free hyaluronate-based polyelectrolyte complex nanocarriers. , 2012, International journal of pharmaceutics.

[26]  J. Dutta,et al.  Progress in antimicrobial activities of chitin, chitosan and its oligosaccharides: a systematic study needs for food applications , 2012, Food science and technology international = Ciencia y tecnologia de los alimentos internacional.

[27]  A. B. Kayitmazer,et al.  Complexation and coacervation of polyelectrolytes with oppositely charged colloids. , 2011, Advances in colloid and interface science.

[28]  P. Dubin,et al.  Entering and exiting the protein-polyelectrolyte coacervate phase via nonmonotonic salt dependence of critical conditions. , 2010, Biomacromolecules.

[29]  M. Loza,et al.  Chitosan-hyaluronic acid nanoparticles loaded with heparin for the treatment of asthma. , 2009, International journal of pharmaceutics.

[30]  J. Mano,et al.  hitosan derivatives obtained by chemical modifications for biomedical nd environmental applications , 2022 .

[31]  M. de la Fuente,et al.  Novel hyaluronan-based nanocarriers for transmucosal delivery of macromolecules. , 2008, Macromolecular bioscience.

[32]  M. de la Fuente,et al.  Novel hyaluronic acid-chitosan nanoparticles for ocular gene therapy. , 2008, Investigative ophthalmology & visual science.

[33]  M. de la Fuente,et al.  Design of novel polysaccharidic nanostructures for gene delivery , 2008, Nanotechnology.

[34]  G. Ya. Wiederschain,et al.  Polysaccharides. Structural diversity and functional versatility , 2007, Biochemistry (Moscow).

[35]  M. Rinaudo,et al.  Chitin and chitosan: Properties and applications , 2006 .

[36]  O. Smidsrod,et al.  Structure–Property Relationship in Chitosans , 2004 .

[37]  Tejraj M Aminabhavi,et al.  Recent advances on chitosan-based micro- and nanoparticles in drug delivery. , 2004, Journal of controlled release : official journal of the Controlled Release Society.

[38]  S. Hudson,et al.  Synthesis and antimicrobial activity of a water-soluble chitosan derivative with a fiber-reactive group. , 2004, Carbohydrate research.

[39]  I. Donati,et al.  Mimicking mechanical response of natural tissues. Strain hardening induced by transient reticulation in lactose-modified chitosan (chitlac). , 2018, International journal of biological macromolecules.

[40]  R. Auzély-Velty,et al.  Chitosan‐based hydrogels: recent design concepts to tailor properties and functions , 2017 .

[41]  E. Dickinson,et al.  Food Colloids, Proteins, Lipids and Polysaccharides , 1997 .