Self-Assembly of Nano- to Macroscopic Metal-Phenolic Materials

The self-assembly of molecular building blocks into well-defined macroscopic materials is desirable for developing emergent functional materials. However, the self assembly of molecules into macroscopic materials remains challenging, in part because of limitations in controlling the growth and robustness of the materials. Herein, we report the molecular self-assembly of nano- to macroscopic free-standing materials through the coordination of metals with natural phenolic molecules. Our method involves a simple and scalable solution-based template dipping process in precomplexed metal phenolic solutions, enabling the fabrication of free-standing macroscopic materials of customized architectures (2D and 3D geometries), thickness (about 10 nm to 5 mu m), and chemical composition (different metals and phenolic ligands). Our macroscopic free-standing materials can be physically folded and unfolded like origami, yet are selectively degradable. Furthermore, metal nanoparticles can be grown in the macroscopic free-standing films, indicating their potential for future applications in biotechnology and catalysis.