Morphogenesis of Biogenic Phenolic Mesocrystals Mediated by Competitive Intermolecular Interactions

The size and shape of the mesocrystals directly determine their properties, making the associated morphogenesis a means to engineer advanced materials from biogenic molecules. Unfortunately, the promise of the latter has been scarcely demonstrated, given their inherent anisotropic covalent bonding and limited tendency to form ordered structures. Herein, we report a library of mesocrystals derived from 3,4,5-tri-O-galloylquinic acid, which is a naturally occurring polyphenol. The direct structural characterization uncovers the crystallization path as the initial densification of prenucleated nanoscale intermediates and the followed continuous ordering into the final morphological changes. We demonstrate the possibility of affording biogenic mesocrystals with tailorable colloidal behavior by gaining control of the competitive intermolecular interactions that direct the self-assembly process.