具有增强稳定性和性能的生物启发金属配体网络：羟基吡啶酮功能化材料的简易制备

IF 5.2 1区化学 Q1 POLYMER SCIENCE

Macromolecules Pub Date : 2024-12-06 DOI:10.1021/acs.macromol.4c0225010.1021/acs.macromol.4c02250

Declan P. Shannon, Kenneth Cerdan, Minseong Kim, Matthew Mecklenburg, Judy Su, Yueyun Chen, Matthew E. Helgeson*, Megan T. Valentine* and Craig J. Hawker*,

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引用次数: 0

摘要

生物启发羟基吡啶酮（HOPO）功能化材料显示出卓越的稳定性和螯合多种金属离子的能力。与传统的儿茶酚系统相比，这允许合成具有不同物理性质的多功能网络。在本研究中，我们报告了一个简单的，一锅合成氨基HOPO配体和简单的，可扩展的结合到peg -丙烯酸酯为基础的网络通过活性酯化学。这种模块化网络方法允许制造含有图案HOPO的网络，该网络可以螯合一系列金属离子，例如过渡金属（Fe3+）和镧系元素（Ho3+, Tb3+），从而导致机械，磁性和荧光特性的调制。此外，通过掩蔽技术在三维空间中定位金属离子，可以制备出具有定制的、异构性质的网络，从而产生明显的软、硬、磁和荧光结构域。

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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 (Fe³⁺) and lanthanides (Ho³⁺, Tb³⁺), 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.

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来源期刊

Macromolecules 工程技术-高分子科学

CiteScore

9.30

自引率

16.40%

发文量

942

审稿时长

2 months

期刊介绍： Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.