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As a subseries of the covalent organic framework (COF) material family, polyimide-based covalent organic framework (PI-COF) material, which has the advantages of high stability of polyimide, high specific surface area, and controllable pores of COF material, is expected to be a new type of porous material with potential applications. Although the development of PI-COF is in the early stages during the past decade, it has attracted extensive attention and is widely used in heterogeneous catalysis, gas separation, and storage fields. Therefore, this review is aiming to give a comprehensive understanding of the recent progress of PI-COFs. This article summarizes the progress of PI-COF from three aspects: controllable structure design, synthesis method, and application. First of all, under the guidance of network chemical design principles, the topology type of PI-COF and the size and shape of the formed pores are summarized in terms of different organic monomers. Then the five synthetic strategies for the synthesis of PI-COF are analyzed. Finally, the applications of PI-COF in adsorption and separation, drug delivery, solar-to-electrochemical energy storage, photocatalysis, and electrocatalyst are introduced.

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