Both the pore size and particle diameter of aqueous colloidal mesostructured/mesoporous silica nanoparticles (CMSS/CMPS) derived from tetrapropoxysilane were effectively and easily controlled by the addition of trialkylbenzenes (TAB). Aqueous highly dispersed CMPS with large pores were successfully obtained through removal of surfactants and TAB by a dialysis process. The pore size (from 4 nm to 8 nm) and particle diameter (from 50 nm to 380 nm) were more effectively enlarged by the addition of 1,3,5-triisopropylbenzene (TIPB) than 1,3,5-trimethylbenzene (TMB), and the enlargement did not cause the variation of the mesostructure and particle morphology. The larger molecular size and higher hydrophobicity of TIPB than TMB induce the incorporation of TIPB into micelles without the structural change. When TMB was used as TAB, the pore size of CMSS was also enlarged while the mesostructure and particle morphology were varied. Interestingly, when tetramethoxysilane and TIPB were used, CMSS with a very small particle diameter (20 nm) with concave surfaces and large mesopores were obtained, which may strongly be related to the initial nucleation of CMSS. A judicious choice of TAB and Si sources is quite important to control the mesostructure, size of mesopores, particle diameter, and morphology.
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