Sonogelation by supramolecular gelators is highlighted as a paradigm shift for their potential applications in material and biomedical sciences. Yet, these materials require organic solvents and low‐frequency ultrasound, limiting their utility. Here, a comb‐like polymethacrylate copolymer is synthesized with 2,6‐bis(1‐methylbenzimidazolyl)‐4‐oxypyridine tridentate ligand randomly distributed on poly(ethylene glycol) side chains. Upon addition of zinc perchlorate salt, this copolymer rapidly forms a hydrogel after exposure to either mechanical (i.e., ultrasound) or thermal stimuli. Spectroscopic analysis, to elucidate the mechanism, indicates metal ion coordination to ligand as well as the carbonyl and ethylene glycol units; interestingly, ¹H‐NMR suggests that the coordination between tridentate ligand moiety and Zn²⁺ is unexpectedly weaker in water than in acetonitrile. Investigations by dynamic light scattering indicates that the copolymer forms nanodispersions in excess salt, which coalesces to form a hydrogel by either heating or high intensity focused ultrasound (HIFU). Rheological quantification of these gels suggests stronger crosslinking by HIFU compared to heating.

中文翻译：

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机械-热刺激在水中使梳状聚甲基丙烯酸酯共聚物发生溶胶-凝胶转变

超分子胶凝剂的声凝胶法作为其在材料和生物医学领域中的潜在应用的范式转移而突出。然而，这些材料需要有机溶剂和低频超声，限制了它们的实用性。在这里，合成了一种梳状聚甲基丙烯酸酯共聚物，其中的2,6-双（1-甲基苯并咪唑基）-4-氧吡啶三齿配体随机分布在聚（乙二醇）侧链上。加入高氯酸锌盐后，该共聚物在暴露于机械刺激（即超声）或热刺激后迅速形成水凝胶。为了阐明机理，光谱分析表明金属离子与配体以及羰基和乙二醇单元配位。有趣的是，¹1 H-NMR表明，三齿配体部分和Zn ²⁺之间的配比在水中比在乙腈中出乎意料地弱。通过动态光散射进行的研究表明，该共聚物在过量的盐中形成了纳米分散体，该盐通过加热或高强度聚焦超声（HIFU）聚结形成水凝胶。这些凝胶的流变学定量表明，与加热相比，HIFU的交联作用更强。