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确定三氟甲磺酸根阴离子在阳离子三有机锡（IV）路易斯酸活化氢中的作用。

Establishing the Role of Triflate Anions in H Activation by a Cationic Triorganotin(IV) Lewis Acid.

作者信息

Sapsford Joshua S, Csókás Dániel, Scott Daniel J, Turnell-Ritson Roland C, Piascik Adam D, Pápai Imre, Ashley Andrew E

机构信息

Molecular Sciences Research Hub, Imperial College, White City Campus, 80 Wood Lane, London W12 0BZ, U.K.

Institute of Organic Chemistry, Research Center for Natural Sciences, Magyar tudósok körútja 2, Budapest H-1117, Hungary.

出版信息

ACS Catal. 2020 Jul 17;10(14):7573-7583. doi: 10.1021/acscatal.0c02023. Epub 2020 Jun 8.

DOI:10.1021/acscatal.0c02023
PMID:32905389
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC7469243/
Abstract

Cationic Lewis acids (LAs) are gaining interest as targets for frustrated Lewis pair (FLP)-mediated catalysis. Unlike neutral boranes, which are the most prevalent LAs for FLP hydrogenations, the Lewis acidity of cations can be tuned through modulation of the counteranion; however, detailed studies on such anion effects are currently lacking in the literature. Herein, we present experimental and computational studies which probe the mechanism of H activation using PrSnOTf (-OTf) in conjunction with a coordinating (quinuclidine; qui) and noncoordinating (2,4,6-collidine; col) base and compare its reactivity with {PrSn·base}{Al[OC(CF)]} (base = qui/col) systems which lack a coordinating anion to investigate the active species responsible for H activation and hence resolve any mechanistic roles for OTf in the PrSnOTf-mediated pathway.

摘要

阳离子路易斯酸（LAs）作为受阻路易斯对（FLP）介导催化的目标正受到关注。与用于FLP氢化的最常见LAs——中性硼烷不同，阳离子的路易斯酸度可通过抗衡阴离子的调节来调整；然而，目前文献中缺乏对此类阴离子效应的详细研究。在此，我们展示了实验和计算研究，这些研究使用PrSnOTf（-OTf）与配位碱（奎宁环；qui）和非配位碱（2,4,6-可力丁；col）一起探究H活化的机制，并将其反应性与缺乏配位阴离子的{PrSn·碱}{Al[OC(CF)]}（碱 = qui/col）体系进行比较，以研究负责H活化的活性物种，从而解析OTf在PrSnOTf介导途径中的任何机制作用。

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