Hydrogel Synthesis and Stabilization via Tetrazine Click-Induced Secondary Interactions.
Hydrogel Synthesis and Stabilization via Tetrazine Click-Induced Secondary Interactions.
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DOI：
10.1002/marc.202000287
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发表时间：
2020-07
影响因子：
4.6
通讯作者：
Alge DL
中科院分区：
文献类型：
--
作者：
Holt SE;Rakoski A;Jivan F;Pérez LM;Alge DL
据报道，四嗪点击诱导的二次相互作用的发现是聚合物生物材料合成的一种有前途的新工具。这种现象首先被证明是通过纯非共价相互作用进行聚（乙二醇）（PEG）水凝胶组装的工具，并被证明可以产生坚固的凝胶，其储能模量比其他非共价交联方法高 1-2 个数量级。此外，四嗪点击诱导的次级相互作用也增强了共价交联水凝胶的性能。与四嗪-降冰片烯和硫醇-降冰片烯点击化学交联的 PEG 水凝胶的头对头比较显示，四嗪点击交联凝胶的储能模量增加了约 6 倍，并且具有前所未有的抗水解降解性，而凝胶分数没有显着差异。分子动力学模拟将这些差异归因于四嗪-降冰片烯环加成产物之间存在次级相互作用，而硫醇-降冰片烯交联凝胶中不存在这种相互作用。在此，利用逆电子需求狄尔斯阿尔德（IEDDA）四嗪-降冰片烯点击反应产物之间的二次相互作用的发现来生产纯非共价交联的水凝胶。在共价交联的聚乙二醇（PEG）水凝胶中，与自由基介导的硫醇-降冰片烯化学交联的凝胶相比，这些次级相互作用的存在导致储能模量增加和耐水解降解。
The discovery of tetrazine click-induced secondary interactions is reported as a promising new tool for polymeric biomaterial synthesis. This phenomenon is first demonstrated as a tool for poly(ethylene glycol) (PEG) hydrogel assembly via purely non-covalent interactions and is shown to yield robust gels with storage moduli 1–2 orders of magnitude higher than other non-covalent crosslinking methods. In addition, tetrazine click-induced secondary interactons also enhance the properties of covalently crosslinked hydrogels. A head-to-head comparison of PEG hydrogels crosslinked with tetrazine-norbornene and thiol-norbornene click chemistry revealed an approximately 6-fold increase in storage modulus and unprecedented resistance to hydrolytic degradation in tetrazine click-crosslinked gels without substantial differences in gel fraction. Molecular dynamic simulations attribute these differences to the presence of secondary interactions between the tetrazine-norbornene cycloaddition products, which are absent in the thiol-norbornene crosslinked gels. Herein, the discovery of secondary interactions between the products of the inverse-electron demand Diels Alder (IEDDA) tetrazine-norbornene click reaction are leveraged to produce purely non-covalently crosslinked hydrogels. In covalently crosslinked poly(ethylene glycol) (PEG) hydrogels, the presence of these secondary interactions results in increased storage modulus and resistance to hydrolytic degradation compared to gels crosslinked with radical-mediated thiol-norbornene chemistry.
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影响因子：
14
作者：
Liu S;Moore AC;Zerdoum AB;Zhang H;Scinto SL;Zhang H;Gong L;Burris DL;Rajasekaran AK;Fox JM;Jia X
通讯作者：
Jia X
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作者：
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通讯作者：
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影响因子：
3.9
作者：
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通讯作者：
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15
作者：
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