The interest in the design and controlled fabrication of dendritic mesoporous silica nanospheres (DMSNs) emanates from their widespread application in drug-delivery carriers, catalysis and nanodevices owing to their unique open three-dimensional dendritic superstructures with large pore channels and highly accessible internal surface areas. A variety of synthesis strategies have been reported, but there is no basic consensus on the elucidation of the pore structure and the underlying formation mechanism of DMSNs. Although all the DMSNs show a certain degree of similarity in structure, do they follow the same synthesis mechanism? What are the exact pore structures of DMSNs? How did the bimodal pore size distributions kinetically evolve in the self-assembly? Can the relative fractions of small mesopores and dendritic large pores be precisely adjusted? In this review, by carefully analysing the structures and deeply understanding the formation mechanism of each reported DMSN and coupling this with our research results on this topic, we conclude that all the DMSNs indeed have the same mesostructures and follow the same dynamic self-assembly mechanism using microemulsion droplets as super templates in the early reaction stage, even without the oil phase.
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