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Inspired by the 2D bilayer lipid membranes in nature, a unique supramolecular “push–pull” synergetic strategy toward self‐assembled 2D organic crystals (2DOCs) is proposed in this work, which can effectively suppress the interlayer 3D stacking while maintaining the assembly of the intralayer for 2D growth. For this purpose, a model molecule PF‐Py consisting of a planar supramolecular “attractor” and...
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