Bioinspired Metal-Ligand Networks with Enhanced Stability and Performance: Facile Preparation of Hydroxypyridinone (HOPO)-Functionalized Materials.

Bioinspired hydroxypyridinone (HOPO)functionalized materials are shown to display a remarkable capacity for stability and for chelating a wide array of metal ions. This allows for the synthesis of multifunctional networks with diverse physical properties when compared to traditional catechol systems. In the present study, we report a facile, one-pot synthesis of an amino HOPO ligand and simple, scalable incorporation into PEG-acrylate based networks via active ester chemistry. This modular network approach allows for fabrication of patterned HOPO containing networks which can chelate a range of metal ions, such as transition metals (Fe) and lanthanides (Ho, Tb), leading to modulation of mechanical, magnetic, and fluorescent properties. Moreover, networks with tailored, heterogeneous properties can be prepared through localization of metal ion incorporation in 3-dimensions via masking techniques, creating distinctly soft, hard, magnetic, and fluorescent domains.