Preparation of Multiple Parallel Protein-polysaccharide Hybrid Gel Filaments Under Shear

Abstract

Fabrication of anisotropic gel with characteristic structures has been reported using a flow system with three dimensional microfluidic devices. Such gel structures are mainly achieved by design and preparation of the microchannel for flowing pre-gel solution. In this research, we propose a method for preparing multiple parallel gel filaments by controlling viscoelastic properties of polymer assembly as the fluid of microfluidic devices. To promote the formation of heterogeneous assembly of different types of macromolecules, an aqueous two-phase separation (ATPS) technique was utilized. Two layers of aqueous solutions appear when the ATPS conditions including ionic strength, temperature, and solute concentration in certain combinations of two components are satisfied. In respective phase, some solute molecules form heterogeneous assemblies because the solutes in respective phase are highly concentrated. We previously reported that the alginate (Alg) could form the assembly with polyethylene glycol (PEG) in the induced phase of Alg/PEG/NaCl system. In aqueous media, the Alg assembly has the rigid structure because diaxial linkages in a successive region of guluronic acid are stabilized by hydrogen bonds. Destruction of hydrogen bonds of Alg molecules by interaction with PEG enables deformation of Alg assembly by shear. Gel filaments were prepared with a co-axial flow device as double glass tubes, where an inner tube (inner diameter 0.7 mm) was fixed at the insert position of the outer tube. Pre-gel solution and crosslinker solution respectively were flown to inner and outer tube using syringe pumps. The morphology of the gel filaments was observed by a scanning electron microscope. A single thick gel filament was obtained from aqueous sodium alginate solution, whereas multiple thin gel filaments were obtained when a mixed solution of Alg and PEG under the ATPS condition. Appearance of shear-thinning behavior for the Alg-rich phase suggests that the complexation of Alg with PEG was responsible for destruction of the rigid assembly due to breaking hydrogen bonds. In this poster, the method will be applied to the protein containing system to fabricate the protein-polysaccharide hybrid filaments.