Liquid Phase Exfoliation\nof Protein Parent Crystals\ninto Nanosheets and Fibrils Based on Orthogonal Supramolecular Interactions

Proteins are attractive building blocks for fabricating\ndiverse\nand precise nanomaterials. However, the facile fabrication of multidimensional\nartificial assemblies is highly challenging. Here, inspired by the\nlarge-scale production technique of inorganic nanomaterials, we demonstrate\nthe application of liquid phase exfoliation (LPE) on native protein\nConA by the design of synthetic ligands. These ligands provide distinct\nin-plane and out-of-plane supramolecular interactions, allowing the\ngeneration of multidimensional architectures based on the same protein\nby dissociating a single interaction in solution, including 3D porous\nprotein crystals, 2D sizable nanosheets, and 1D fibrils. Importantly,\nthe exfoliated 2D sheets were dozens of times larger than the self-assembled\nnanosheets, resulting in a dramatic enhancement of the intrinsic bioactivity\nof the building blocks by receptor clustering and less endocytosis.\nThese findings enable the successful application of LPE on biomacromolecules\nand open up an alternative avenue to generate advanced multidimensional\nnanomaterials, without the need for complex protein design and careful\nadjustment of self-assembly conditions.