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探索不寻常的封闭化学:激发状态的质子转移反应在支持的液体膜中,使用深度欧特克溶剂

Sangeeta¹, Arnab Sil¹, Vikash Singh¹

¹Department of Chemistry, School of Natural Sciences Shiv Nadar Institution of Eminence, Delhi-NCR, Uttar Pradesh 201314, India.

The journal of physical chemistry. B

|September 28, 2024

概括

激发状态质子转移发生在基于溶剂的支持液体膜中,与散装溶剂不同. 这表明膜毛孔内的有序溶剂结构能够实现新的化学过程.

科学领域:

超分子化学超分子化学
材料科学材料科学材料科学
物理化学物理化学

背景情况:

含有离子液体 (IL) 或深溶剂 (DES) 的支液体膜 (SLM) 对分离和二氧化碳捕获具有前景.
了解这些有限的SLM环境中的分子行为,包括化学反应,对于它们的应用至关重要.

研究的目的:

在基于DES的SLM中调查光酸 (HPTS) 的激发状态质子转移 (ESPT) 的发生和特征.
与散装DES相比,阐明封闭的DES环境对ESPT动态和溶剂放松的影响.

主要方法:

使用稳定状态和时间分辨率的光谱学研究 HPTS 在各种基于 DES 的 SLM (∼280 nm 孔径大小) 中.
分析时间解析区域规范化发射光谱 (TRANES) 以确定ESPT时间表.
研究了溶剂放松动态和红边激发变化.

主要成果:

观察到,ESPT,在大量DES中不利,在基于DES的SLM中发生大量.
ESPT时间尺度从2.6到7.5毫秒不等,对DES成分敏感.
在封闭的DES中,溶剂放松速度明显低于散装,这表明由于界面影响而改变了溶剂结构.

结论:

受膜毛孔内的远程界面效应影响的有序的DES结构促进ESPT.
限制在SLM中显著影响DES特性,减缓溶剂放松,促进化学反应.
基于DES的SLM提供了一个可行的平台,用于在封闭的环境中探索新的化学过程.

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