Theoretical study on the interactions between cellulose and different methyltriethoxysilane hydrolysis products

Silylation is an effective means of cellulose modification. However, the condensation reaction process between the hydrolysis products of the silane coupling agent and cellulose, as well as the structure of the coating, which both have a strong influence on the wettability, are still controversial. In this paper, the reactions of different methyltriethoxysilane hydrolysis products with cellulose were simulated via the density functional theory method. The reaction activity centers of the different methyltriethoxysilane hydrolysis products in an ethanol solution were analyzed via the front-line orbital theory and the Fukui function. The silylation reaction of different methyltriethoxysilane hydrolysis products in an ethanol solution on the cellulose surface were investigated via the transition state theory. The results show that although the initial hydrolysis product has the lowest grafting energy barrier, considering the whole process of grafting and condensation on the cellulose surface, the hydrolysis product with two hydroxyl groups is more favorable for the growth of organosilicon on the cellulose surface, so it is desirable to control the reaction where this product is dominant. In addition, the silylation process on the cellulose surface is more inclined to a multilayer coating mechanism.