Shannon Declan P, Cerdan Kenneth, Kim Minseong, Mecklenburg Matthew, Su Judy, Chen Yueyun, Helgeson Matthew E, Valentine Megan T, Hawker Craig J
Materials Department, University of California Santa Barbara, Santa Barbara, California 93106-5050, United States.
Materials Research Laboratory, University of California Santa Barbara, Santa Barbara, California 93106-5121, United States.
Macromolecules. 2024 Dec 6;57(24):11339-11349. doi: 10.1021/acs.macromol.4c02250. eCollection 2024 Dec 24.
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.
受生物启发的羟基吡啶酮（HOPO）功能化材料显示出卓越的稳定性以及螯合多种金属离子的能力。与传统的儿茶酚体系相比，这使得合成具有多样物理性质的多功能网络成为可能。在本研究中，我们报道了一种简便的一锅法合成氨基HOPO配体，并通过活性酯化学方法将其简单、可扩展地引入基于聚乙二醇丙烯酸酯的网络中。这种模块化网络方法能够制造出含HOPO的图案化网络，该网络可以螯合一系列金属离子，如过渡金属（铁）和镧系元素（钬、铽），从而实现对机械、磁性和荧光性质的调控。此外，通过掩蔽技术在三维空间中定位金属离子掺入，可以制备具有定制的、异质性质的网络，从而形成明显的软、硬、磁性和荧光区域。
