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Abstract Sp2-carbon-conjugated covalent organic frameworks (sp2C-COFs) hold exceptional potential as π-conjugated semiconductors for optoelectronics and photocatalysis, yet their thin-film fabrication suffers from irreversible C = C linkages that impede crystallinity and morphology control. Herein, we report a polymer brush-mediated surface-initiated polycondensation (PB-SIP) strategy to synthesize the sp2C-COF films with controlled crystallinity and morphology.
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