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Synergetic Extreme Condition High-Pressure Science Center, State Key Laboratory of Superhard Materials, College of Physics, Jilin University, Changchun 130012, China.

Covalent-organic frameworks (COFs) are dynamic covalent porous organic materials constructed from emissive molecular organic building blocks. However, most two-dimensional (2D) COFs are nonemissive or weakly emissive in the solid state owing to the intramolecular rotation and vibration together with strong π-π interactions. Herein, we report a pressure strategy to achieve the bright multicolor emission from yellow to red in the 2D triazine triphenyl imine COF (TTI-COF).

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