Oxidation Level and Glycidyl Ether Structure Determine Thermal Processability and Thermomechanical Properties of Arabinoxylan-Derived Thermoplastics.

Developing flexible, stretchable, and thermally processable materials for packaging and stretchable electronic applications from polysaccharide-based polymers contributes to the smooth transition of the fossil-based economy to the circular bioeconomy. We present arabinoxylan (AX)-based thermoplastics obtained by ring-opening oxidation and subsequent reduction (dA-AX) combined with hydrophobization with three different glycidyl ethers [-butyl (BuGE), isopropyl (PrGE), and 2-ethyl hexyl (EtHGE) glycidyl ether]. We also investigate the relationship between structural composition, thermal processing, and thermomechanical properties.

Hydrophobization of arabinoxylan with n-butyl glycidyl ether yields stretchable thermoplastic materials.

Hemicelluloses are regarded as one of the first candidates for the development of value-added materials due to their renewability, abundance, and functionality. However, because most hemicelluloses are brittle, they can only be processed as a solution and cannot be processed using industrial melt-based polymer processing techniques. In this study, arabinoxylan (AX) was hydrophobized by incorporating butyl glycidyl ether (BuGE) into the hydroxyl groups through the opening of the BuGE epoxide ring, yielding alkoxy alcohols with terminal ethers.

Controlled Loading and Release of Beta-Lactoglobulin in Calcium-Polygalacturonate Hydrogels.

We show here how the structure of polygalacturonate (polyGalA) hydrogels cross-linked by Ca cations via external gelation controls the loading and release rate of beta-lactoglobulin (BLG), a globular protein. Hydrogels prepared from a polyGalA/BLG solution are found to be similar to those obtained from a polyGalA solution in our previous study (Maire du Poset et al. , (7), 2864-2872): they exhibit similar transparencies and gradients of mechanical properties and polyGalA concentrations.

Evidence for an egg-box-like structure in iron(ii)-polygalacturonate hydrogels: a combined EXAFS and molecular dynamics simulation study.

The local structure of Fe in Fe-polygalacturonic acid (polyGalA) hydrogels has been studied by coupling Extended X-ray Absorption Fine Structure (EXAFS) spectroscopy and molecular dynamics (MD) simulation. The EXAFS fitting results reveal an octahedral coordination geometry of Fe both in aqueous solution and in the hydrogel, with similar Fe-O distances (2.09 ± 0.

Tuning the Structure of Galacturonate Hydrogels: External Gelation by Ca, Zn, or Fe Cationic Cross-Linkers.

We show here how the nature of various divalent cations M (Ca, Zn, or Fe) 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 = [M]/[Gal] equal to 0.25, showing that every M cation interacts with four galacturonate (Gal) units all along the gels.

Insights into gelation kinetics and gel front migration in cation-induced polysaccharide hydrogels by viscoelastic and turbidity measurements: Effect of the nature of divalent cations.

Polysaccharide-based hydrogels were prepared by the diffusion of various divalent cations (X) into the polygalacturonate (polyGal) solution through a dialysis membrane. The diffusion of various divalent cations (Mg, Ca, Zn and Ba) was investigated. The polyGal gel growth was studied as a function of the initial cation concentration by both viscoelastic and turbidity measurements.

Design of polygalacturonate hydrogels using iron(II) as cross-linkers: A promising route to protect bioavailable iron against oxidation.

We designed stable and highly reproducible hydrogels by external unidirectional diffusion of Fe ions into aqueous solutions of polygalacturonate (polyGal) chains. The Fe ions act as cross-linkers between the Gal units in such a way that both the molar ratio R ([Fe]/[Gal units] = 0.25) and the mesh size of the polyGal network at the local scale (ξ = 75 ± 5 Å) have constant values within the whole gel, as respectively determined by titration and Small Angle Neutron Scattering.