通过电荷中性素和素结合折叠体受体在水中的离子识别
Arseni Borissov1, Igor Marques2, Jason Y C Lim1
1Chemistry Research Laboratory, Department of Chemistry , University of Oxford , Mansfield Road , Oxford OX1 3TA , U.K.
Journal of the American Chemical Society
|February 8, 2019
概括
电荷中性的非循环宿主首次能够在水中进行选择性离子识别. 这种新的策略通过σ-孔相互作用实现了前所未有的结合亲和力,例如化物.
科学领域:
- 超分子化学
- 离子识别
- 主机与客户之间的化学反应
背景情况:
- 由于水的高介电常数和竞争性水合性,在水中识别阴离子具有挑战性.
- 现有的受体通常依赖于阴离子框架或缺乏水性介质的选择性.
- σ-孔结合为离子结合提供了一个有希望的,但未被充分探索的非共价相互作用.
研究的目的:
- 开发一种新型的电荷中性宿主系统,用于水中的选择性离子识别.
- 为了研究 σ-孔素和素结合在水性离子结合中的有效性.
- 建立新的分子工具,以克服纯水中的离子识别挑战.
主要方法:
- 设计和合成含有素和素结合剂的水溶性,基于折叠剂的非循环宿主.
- 用于各种离子的定量结合研究的异热定位热量计 (ITC).
- 分子动力学 (MD) 模拟以阐明水中的结合机制和复杂结构.
主要成果:
- 受体表现出很强的和选择性的结合大,弱水合的离子 (例如,I−,ReO4−).
- 通过合作的多牙 σ-孔捐赠体稳定了2:1宿主-客群的形成.
- 在水中达到前所未有的酸亲和度 (β2高达1.68 × 1011 M-2),超过已知的σ孔受体.
结论:
- 在水中使用电荷中性的σ-孔相互作用进行阳离子识别的新策略得到了成功证明.
- 与现有系统相比,开发的受体提供了更高的性能,创造了新的基准.
- 素和素结合被证实是促进在水环境中的离子识别的强大工具.
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