Thermoresponsive Dendronized Polypeptides Showing Switchable Recognition to Catechols
Thermoresponsive Dendronized Polypeptides Showing Switchable Recognition to Catechols
复制标题
热响应性树枝状多肽显示出对儿茶酚的可切换识别
DOI：
10.1021/acs.macromol.5b02259
复制
发表时间：
2016-01-26
期刊：
影响因子：
5.5
通讯作者：
Zhang, Afang
中科院分区：
文献类型：
--
作者：
Yan, Jiatao;Liu, Kun;Zhang, Afang
通过氧氨基取代聚赖氨酸与乙二醇缩甲醛树枝高效连接，合成了一类新型的热响应性树枝状多肽。研究了它们的二级结构和热响应行为。由于树枝状结构和稳定的肟键，这些基于OEG的树枝状多肽在中性水溶液中表现出快速且完全可逆的相变，其相变温度可以控制在生理温度附近。考察了OEG树枝状化对多肽二级结构的影响，以考察其显著的树枝状屏蔽效应、空间位阻和热驱动相变。为了进一步扩展这些刺激响应性树枝状多肽的功能和潜在应用，引入了苯基硼酸部分来制备相应的树枝状共聚物，用于特异性识别含邻苯二酚的化合物，如茜素红S或多巴胺。与单体苯基硼酸相比，这些共聚肽与儿茶酚的结合力显著增强。此外，这种增强的结合可以通过热驱动的相变或通过添加竞争性儿茶酚来切换，这使得这类树枝状多肽成为选择性和可逆识别儿茶酚的独特支架。
A new class of thermoresponsive dendronized polypeptides was prepared through highly efficient oxime ligation between oxyamino-substituted polylysines and aldehyde-cored oligo-ethylene glycol (OEG) dendrons. Their secondary structures and thermoresponsive behavior were investigated. Because of the dendritic structures and stable oxime linkage, these OEG-based dendronized polypeptides exhibited fast and fully reversible phase transitions in neutrally aqueous solutions, and their phase transition temperatures can be controlled around physiological temperatures. The effect of OEG dendronization on secondary structures of polypeptides were examined to check their prominent dendritic shielding effect, steric hindrance, and thermally driven phase transitions. To further extend the functions and potential applications of these stimuli-responsive dendronized polypeptides, phenylboronic acid moieties were introduced to achieve the corresponding dendronized copolymers, which were utilized to specifically recognize catechol-containing compounds such as alizarin red S or dopamine. These copolypeptides showed a significant enhancement to bind to catechols when comparing to monomeric phenylboronic acid. Furthermore, this enhanced binding can be switched surprisingly by thermally driven phase transitions or through addition of competitive catechols, which makes this class of dendronized polypeptides as unique scaffolds for selective and reversible recognition of catechols.