0000000000827196
AUTHOR
Aline Maire Du Poset
Polygalacturonate hydrogels using Fe2+ as cross-linkers : impact of the local association mode on gelation mechanisms, control of the multiscale structure and the mechanical properties.
This pHD thesis describes the design of polygalacturonate hydrogels (polyGal) cross-linked by the Fe2+ cations, and their experimental characterization from the molecular scales up to the macroscopic scales, by combining EXAFS spectroscopy, Small Angle Neutron Scattering (SANS) and rheological measurements. We designed a robust gelling protocol that allowed to obtain reproducible cylindrical gels with controlled concentration gradients from the lower side to the upper side of the gel. The ratio [Fe]/[Gal] has a constant value all along the gel, which demonstrate that the Fe2+ cations are associated with 4 galacturonate units. The comparison of EXAFS measurements and molecular dynamics simul…
Controlled loading and release of beta-lactoglobulin in calcium-polygalacturonate hydrogels
International audience; We show here how the structure of polygalacturonate (polyGalA) hydrogels cross-linked by Ca2+ cations via external gelation controls the loading and the release rate of betalactoglobulin (BLG), a globular protein. Hydrogels prepared from a polyGalA/BLG solution are found similar to those obtained from a polyGalA solution in our previous study (Maire du Poset, et al. Biomacromolecules 2019, 20(7), 2864-2872): they exhibit similar transparencies and gradients of mechanical properties and polyGalA concentration. The nominal BLG/polyGalA ratio of the mixtures is almost recovered within the whole mixed hydrogel despite such strong concentration gradients, except in the pa…
Tuning the Structure of Galacturonate Hydrogels: External Gelation by Ca, Zn, or Fe Cationic Cross-Linkers
International audience; We show here how the nature of various divalent cations M2+ (Ca2+, Zn2+, or Fe2+) influences the structure and mechanical properties of ionotropic polygalacturonate (polyGal) hydrogels designed by the diffusion of cations along one direction (external gelation). All hydrogels exhibit strong gradients of polyGal and cation concentrations, which are similar for all studied cations with a constant ratio R = [M2+]/[Gal] equal to 0.25, showing that every M2+ cation interacts with four galacturonate (Gal) units all along the gels. The regions of the hydrogels formed in the early stages of the gelation process are also similar for all cations and are homogeneous, with the s…