Zipping and Unzipping of a Paddlewheel Metal–Organic Framework to Enable Two‐Step Synthetic and Structural Transformation

MOF zipper: Thermal removal of axial pyridine ligands from the non-covalently pillared metal–organic framework [Zn2(camph)2(py)2]⋅2EtOH prompts migration of alternate camphorate ligands to zip Zn centers from adjacent layers into continuous chains within the nonporous material [Zn2(camph)2] (see scheme). Unzipping to generate new pillared, layered MOFs occurs on exposure to new axial ligands.