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首页> 外文期刊>Chemistry: A European journal >Degradable Hybrid Materials Based on Cationic Acylhydrazone Dynamic Covalent Polymers Promote DNA Complexation through Multivalent Interactions
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Degradable Hybrid Materials Based on Cationic Acylhydrazone Dynamic Covalent Polymers Promote DNA Complexation through Multivalent Interactions

机译：基于阳离子酰基hydr动态共价聚合物的可降解杂化材料通过多价相互作用促进DNA络合

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摘要

The design of smart nonviral vectors for gene delivery is of prime importance for the successful implementation of gene therapies. In particular, degradable analogues of macromolecules represent promising targets as they would combine the multivalent presentation of multiple binding units that is necessary for achieving effective complexation of therapeutic oligonucleotides with the controlled degradation of the vector that would in turn trigger drug release. Toward this end, we have designed and synthesized hybrid polyacylhydrazone-based dynamic materials that combine bis-functionalized cationic monomers with ethylene oxide containing monomers. Polymer formation was characterized by ~1H and DOSY NMR spectroscopy and was found to take place at high concentration, whereas macrocycles were predominantly formed at low concentration. HPLC monitoring of solutions of these materials in aqueous buffers at pH values ranging from 5.0 to 7.0 revealed their acidcatalyzed degradation. An ethidium bromide displacement assay and gel electrophoresis clearly demonstrated that, despite being dynamic, these materials are capable of effectively complexing dsDNA in aqueous buffer and biological serum at N/P ratios comparable to polyethyleneimine polymers. The self-assembly of dynamic covalent polymers through the incorporation of a reversible covalent bond within their main chain is therefore a promising strategy for generating degradable materials that are capable of establishing multivalent interactions and effectively complexing dsDNA in biological media.
机译：用于基因传递的智能非病毒载体的设计对于成功实施基因疗法至关重要。特别地，大分子的可降解类似物代表有希望的靶标，因为它们将结合多个结合单元的多价呈递，这对于实现治疗性寡核苷酸的有效络合是必需的，而载体的受控降解又会触发药物释放。为此，我们设计并合成了基于杂酰基hydr的杂化动态材料，该材料结合了双官能化阳离子单体和含环氧乙烷的单体。用〜1H和DOSY NMR光谱对聚合物的形成进行了表征，发现高浓度时会形成聚合物，而低浓度时会形成大环。在pH值为5.0到7.0的水性缓冲液中对这些物质的溶液进行HPLC监测，发现它们被酸催化降解。溴化乙锭置换试验和凝胶电泳清楚地表明，尽管它们是动态的，但这些材料能够以与聚乙烯亚胺聚合物相当的N / P比有效地复合dsDNA在水性缓冲液和生物血清中。因此，通过在其主链中引入可逆共价键来实现动态共价聚合物的自组装是产生可降解材料的有前途的策略，该材料能够在生物介质中建立多价相互作用并有效地复合dsDNA。

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