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基于Binaphthalene的Tetraimidazolium宏循环的温度驱动的合规切换,以增强水中二核酸的序列选择性识别

Tianci He¹, Mengxin Huo¹, Pingxia Wang¹

¹College of Chemistry and Materials Science, Northwest University, Xi'an, 710069, P.R. China.

Angewandte Chemie (International ed. in English)

|September 11, 2025

概括

研究人员开发了随温度改变形状的人造宿主,以了解生物识别. 这些宿主选择性地结合特定的DNA序列,如d(TpA),在更高的温度下增强亲和力.

科学领域:

超分子化学超分子化学
化学生物学化学生物学
分子识别分子识别

背景情况:

人工宿主对于模仿自然识别系统和理解温度依赖的全雌激素至关重要.
开发具有可调节性质的宿主,如温度驱动的 conformational 切换,有助于研究适应机制.

研究的目的:

设计和合成新的水溶性,以二甲基为基础的四聚胺宏循环作为人工宿主.
通过使用这些宿主,研究在水性介质中对二核酸的序列选择性识别.
探索合成的宏观循环的依赖温度的结合行为和构造性切换.

主要方法:

合成了三对基于双纳甲的四化宏循环 (SS/RR-1•4Cl-到SS/RR-3•4Cl-).
利用温度变化在宏循环宿主中诱导构造性切换 (cis 到 trans).
使用结合测试来确定不同温度 (288 K和323 K) 的各种二核酸的关联常数 (K_a).

主要成果:

大循环SS-1•4Cl-表现出温度驱动的形状转换,随着温度的增加,从cis转变为trans形状.
对d (TpA) 的结合亲和力随温度显著增加,在323K时达到K_a ~10⁶ M^-1,证明了温度合作结合.
在d(TpA) 与d(ApT) 之间实现了高序列选择性,选择性因子 (K_rel) 在323K时达到~118.8.

结论:

合成的宏循环作为水中的二核酸识别的有效人工宿主.
温度驱动的 conformational switching 是一个可行的策略来调节结合亲和力,并实现序列选择性.
这项研究提供了有关生物系统的温度依赖性全和适应性识别机制的见解.

关键词:

基于比纳夫他林的宏循环.符合性的切换丁核酸是核酸中的一种.主机客户系统.序列选择性识别序列选择性识别

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