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三态双链的水媒可逆控制 (IV) 螺旋

Naoki Ousaka^1,2, Manabu Itakura¹, Akira Nagasaka²

¹Department of Molecular and Macromolecular Chemistry, Graduate School of Engineering, Nagoya University, Chikusa-ku, Nagoya 464-8603, Japan.

Journal of the American Chemical Society

|March 10, 2021

概括

这项研究证明了三种不同的 (IV) 螺旋体之间的新型水控制可逆转变. 这些动态的结构变化,由水化/脱水驱动,提供可控的合和无合金属复合物的合成.

科学领域:

超分子化学
协调化学
材料科学

背景情况:

在生物系统中,响应刺激的可逆结构转变至关重要.
控制复杂分子结构的组装和拆卸仍然是一个重大挑战.

研究的目的:

报告一个独特的水介导可逆转变在三个离散的双链双核中.
调查化/脱水和氧化键动态在结构互转中的作用.
为了证明可控的Achiral中和的rac-helicates的产生.

主要方法:

合成二氧化 (-) 桥 (IV) 中.
在各种溶剂条件下进行受控的水化/脱水实验 (CD3CN,水性CD3CN).
研究酸催化和密度[2.2.1]对反应速率和途径的影响.
通过光谱方法进行结构性表征 (隐含).

主要成果:

通过化/脱水和Ti-OPh键动态证明了 bis (μ-hydroxo) 桥接的半酸盐和 mono (μ-oxo) 桥接的 rac-helicate 之间的可逆转化.
在较低的温度下加速转化.
在无水条件下,受 Na+ 离子去除的影响,报告了介质到介质酸盐的转化.
通过调整含水量以可控的方式成功生成了三种不同的螺旋.

结论:

水含量是控制 (IV) 螺旋体可逆结构变化的关键外部刺激.
这些转换的核心是由水介导的Ti-OPh键的动态裂变和重新形成.
这项工作提供了一个可控合成复杂的性和无性超分子结构的多功能平台.

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