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Sugarsilanes, alkoxysilanes derived from sugars and sugar alcohols including glycerol, sorbitol, maltose and dextran, were hydrolyzed to prepare monolithic, mesoporous silicas. Unlike conventional alkoxysilanes such as tetramethylorthosilicate (TMOS) and tetraethylorthosilicate (TEOS), the sol–gel hydrolysis and cure rates of sugarsilanes were very sensitive to ionic strength, but not to pH: comparable rates of gelation were observed for any specific compound at constant ionic strength over a pH range of about 5.5–11. Reduced levels of shrinkage when compared to TEOS (65% for diglycerylsilane (DGS)-derived silica; 50% for monosorbitylsilane (MSS)-derived silica) were also observed provided that the residual sugars were not washed or pyrolyzed from the silica monolith. Pore sizes in the dried silica monoliths (∼2–3 nm diameter) were marginally increased by the addition of non-functional polyethylene …