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Dimensional regulation of titanosilicates from conventional 3D to revolutionary 2D without extra additives is limited by the Ostwald ripening process together with the mismatch of hydrolysis rate between Ti and Si species. Herein, the kinetically controlled and additive‐free strategy is devised to continuously regulate the dimensionality of intergrowth titanosilicate from 3D bulk to 2D nanosheets...
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