Interpenetration Control in Three-Dimensional Covalent Organic Frameworks: Architectural Modulation and cis -Imine Configuration

isomerization, imparting pronounced framework flexibility and driving an exceptional ∼220% expansion of the crystal volume. This work provides the systematic experimental demonstration that interpenetration can be harnessed to govern both framework architecture and dynamic behavior, highlighting its key role in designing 3D COFs with tailored functions.