Materials Science and Engineering

Biography

Biography: Kimihisa Yamamoto

Abstract

We show that tin chlorides, SnCl₂ and FeCl₃ complexes to the imines groups of a spherical polyphenyl-azomethine dendrimer in a stepwise fashion according to an electron gradient, with complexation in a more peripheral generation proceeding only after complexation in generations closer to the core has been completed. The metal-assembly in a discrete molecule can be converted to a size-regulated metal cluster with a size smaller than 1nm as a molecular reactor. Due to the well-defined number of metal clusters in the sub-nanometer size region, its property is much different from that of bulk or general metal nanoparticles. Dendrimers are highly branched organic macromolecules with successive layers or “generations” of branch units surrounding a central core. Organic inorganic hybrid versions have also been produced, by trapping metal ions or metal clusters within the voids of the dendrimers. Their unusual, tree-like topology endows these nanometer-sized macromolecules with a gradient in branch density from the interior to the exterior, which can be exploited to direct the transfer of charge and energy from the dendrimer periphery to its core. Here we show that tin ions, Sn²⁺, complex to the imines groups of a spherical poly phenyl azo- methane dendrimer in a stepwise fashion according to an electron gradient, with complexation in a more peripheral generation proceeding only after complexation in generations closer to the core has been completed. By attaching an electron-withdrawing group to the dendrimer core, we are able to change the complexation pattern, so that the core imines are complexed in the last. By further extending this strategy, it should be possible to control the number and location of metal ions incorporated into dendrimer structures, which can be used as tailored catalysts, building blocks, or fine-controlled clusters for advanced materials.