Covalent organic frameworks (COFs) possess high stability due to the covalent backbones and are promising platforms for electrocatalyst, sensors, energy storage as well as quantum information systems1-5. These mechanically robust COFs provide exciting opportunities to probe the electronic states of porous materials under high pressure. In this work, we investigate a two-dimensional conjugated COF known as sp2-c-COF6. Raman spectroscopy and X-ray diffraction show that the 2D COF is stable up to 15 GPa. Interestingly, in situ electrical transport reveals an insulator-to-metal transition in tetracyanoquinodimethane (TCNQ) - doped sp2-c-COF at 9 GPa, representing the first porous crystalline material with true metallic transport. Density-functional tight binding (DFTB) modeling show pressure-induced coplanarity as the main structural driving force for the evolution of electron states. These results pave the way for further investigation of COFs as a new class of electronic materials under extreme conditions.

Two-dimensional conjugated covalent organic frameworks under high-pressure

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