Direct Observation of the Labile Imine Formation through Single-Crystal-to-Single-Crystal Reactions in the Pores of a Porous Coordination Network

We report an approach to in situ observation of unstable species produced by a single-crystal-to-single-crystal chemical reaction. We succeeded in uniform formation and the direct observation of unstable imines in pores of a 3-D porous coordination network with aldehydes provided by guest exchange. Moreover, we found the remarkable dynamic motion of a part of the host framework by changing aldehydes.