Chemical modification of wheat-protein-based natural polymers: formation of polymer networks with alkoxysilanes to modify molecular motions and enhance the material performance.

The mechanical performance of plasticized wheat gluten (WG) materials was significantly modified through the formation of different chemical and network structures with alkoxysilanes. The epoxy-functionalized alkoxysilanes were grafted to segments of WG, and then the condensation reactions between alkoxysilane segments occurred during thermal processing to form WG-siloxane networks. The mechanical properties and molecular motions of the networks were dependent on the amount and type of alkoxysilanes applied. A lower amount of alkoxysilanes caused the alkoxysilane molecules to predominately graft onto WG chains without forming linkages between WG segments, which produced an additional plasticizing effect on the WG systems with a longer elongation value and weaker tensile strength at relative humidity (RH) = 50% as compared to the WG system. However, such grafting improved the hydrostability of the materials and generated an improvement in tensile strength at RH = 85%. Increasing the amount of alkoxysilanes in the systems led to the formation of cross-linked WG-siloxane networks via linkages between alkoxysilane segments. Remarkable strength improvement was obtained for the networks with elongation values still higher than the original plasticized WG due to the flexible nature of the siloxane components. A more significant strength improvement was obtained for the WG-SiA systems at both RH = 50% and 85%, where SiA could form three-dimensional networks from siloxane condensation and generate highly cross-linked network structures with relatively low mobility. For WG-SiB systems, SiB could only form linear linkages, and the higher mobility of the SiB phase caused the systems to display a lower strength improvement with a longer elongation value.