Molecular Flytraps Held Together by Platinum–Platinum Intermetallic Bonds

Metal‐metal bonds have rarely been explored as active elements in supramolecular assemblies despite their unique potential to introduce responsive behavior. In this report, a dynamic molecular container composed of two cyclometalated Pt units is constructed using Pt−Pt bonds. This molecule—the flytrap—has a flexible jaw composed of two [18]crown‐6 ethers that can adapt their shape to bind large inorganic cations with sub‐micromolar affinity. Along with the spectroscopic and crystallographic characterization of the flytrap, we report its photochemical assembly, which allows the capture of ions and their transport from solution to the solid state. In addition, we have been able to recycle the flytrap to regenerate its starting material due to the reversible nature of the Pt−Pt bond. We believe that other molecular containers and materials for harvesting valuable substrates from solution could be assembled using the advances presented here. Metal‐metal bonds have rarely been sighted in the supramolecular realm, yet they can provide a number of features from which to harvest dynamic behavior and responsiveness. Here, a single Pt−Pt bond was used to glue two cyclometalated hosts together and generate a flytrap‐like molecule. This compound traps inorganic ions in its jaw, assembles and disassembles photochemically, and irreversibly transports guests from solution to the solid state.