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同质电子转移在控制有机电合成中介选择性的时空空间分离

Jack W Hodgson¹, Ana A Folgueiras-Amador¹, Derek Pletcher¹

¹School of Chemistry, University of Southampton, Highfield, Southampton SO17 1BJ, UK. rcb1@soton.ac.uk.

Faraday discussions

|July 31, 2023

概括

这项研究探讨了反直觉的电合成,其中介质比基质更难减少. 这种方法创建了一个分离的反应层,使新的电还原通路成为可能.

科学领域:

电化学电化学电化学
有机合成有机合成
化学工程是化学工程的重要组成部分.

背景情况:

在电合成中,电子转移 (ET) 媒介通常具有比选择性反应的基质更低的还原潜力.
传统的方法确保介质在与基板相互作用之前被减少到电极表面.

研究的目的:

为了研究一个反直觉介导的电还原过程,其中介质的还原潜力比基质的更为负.
探索条件和机制,导致在这些逆向潜在条件下成功的电合成.

主要方法:

使用计算模拟来建模质量运输,反应剂度和速率常数的复杂相互作用.
对未的批量 (1D) 和流量 (2D) 电解条件进行了模拟.
模拟结果与阿里酸的电还原循环的实验数据进行了比较.

主要成果:

复杂的因素相互作用可以导致同质反应层脱离电极表面.
这种脱离是由于介质基离子和基质的对立流量造成的,防止基质在电极上的减少.
模拟对介导和无介导反应的实验选择性结果进行了定性复制.

结论:

介导电合成是可行的,即使介导体的还原潜力比基质的更负.
反应层脱离是一个关键的现象,使得选择性电还原在这些条件下.
这种方法为在电合成中使用高降解性同质电子转移剂开辟了新的可能性.

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