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Controlled interlayer stacking, solvent processing, and long-afterglow luminescence have been challenges in the development of two-dimensional covalent organic frameworks (2D-COFs). We propose a twisted node modulation strategy to address these issues simultaneously. Consistency of node distortion types causes stacking style to become non-adjustable: eclipsed stacking (non-twisted node) and inclined stacking (twisted node). By alternating the introduction of twisted and non-twisted nodes into a 2D-COFs system, a reversible crystal transformation between eclipsed and inclined stacking is achieved. The inclined COFs can be easily exfoliated into nanosheets for solution processing. Confining isolated exfoliated nanosheets within the polymethyl methacrylate achieves programmable long-afterglow luminescence, which is for writing and printing, as well as imaging, anti-counterfeiting, and emergency lighting. This work provides a strategy for the design of 2D-COFs with different stackings to address the challenges of difficult processing for novel functional applications.
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•A structure design strategy for long-afterglow luminescence (LAL) is presented•Introducing alternately different nodes leads to a reversible crystal interconversion•The correlation between node and stacking for solution processability is determined•Confining isolated nanosheets and solution processability for programmable LAL
Two-dimensional covalent organic frameworks (2D-COFs) are seldom realized as good platforms for long-afterglow luminescence. Shao et al. report a twisted node modulation strategy to determine the correlation between node and stacking style to address three challenges: (1) reversible crystal transformation, (2) a strategy for solution processability of COFs, and (3) long-afterglow luminescence for programmable applications.