硫氧化物功能化N-异环碳素复合物的二重选择性合成:一个实验和计算研究
Victoria Mechrouk1, Baptiste Leforestier2, Weighang Chen1
1Institut de Physique et Chimie des Matériaux de Strasbourg, Université de Strasbourg-CNRS UMR 7504, 23 rue du Loess, BP 43, 67034, Strasbourg Cedex 2, France.
Chemistry (Weinheim an der Bergstrasse, Germany)
|June 11, 2024
概括
合成了新的硫氧化物功能化N-异环碳素 (NHC-SO) 配体及其复合物. 这些复合物有效催化二次醇的β-化,显示出高反应性和选择性.
科学领域:
- 有机金属化学 有机金属化学
- 催化剂是一种催化剂.
- 有机合成 有机合成
背景情况:
- 新型配体的开发对于推进催化应用至关重要.
- 复合物是有机转换中的多功能催化剂.
- 硫氧化物功能化的配体具有独特的协调特性.
研究的目的:
- 合成新型的硫氧化物功能化N-异环碳素 (NHC-SO) 连接体前体.
- 准备和表征含有这些NHC-SO连接体的阴阳性 (II) 复合体.
- 为了研究这些复合物的催化活性在酒精的β-化.
主要方法:
- 乙烯前体的轻度氧化为硫化物功能化的NHC接体盐.
- 通过Ag2O转移合成阴离子[Ru(II) ((η6-p-cymene) ((NHC-SO) Cl]+复合物.
- 使用NMR光谱学和X射线衍光度学进行结构性表征.
- 计算研究 (DFT) 了解二聚体形成和反转障碍.
- 对二次醇的β-化进行催化评价.
主要成果:
- 成功合成具有高选择性的硫化物功能化的NHC配体前体.
- 制备优异产量的鲁 (II) 复合物,证实了双酸盐 (κ2,C,S) 协调.
- 由于热力学控制,对单个二聚体 (作为一个反聚体对) 的观察.
- 在二次醇的β-化中表现出催化活性.
- 复合物4dPF6与各种酒精基质表现出高反应性和选择性.
结论:
- 新型硫氧化物功能化的NHC配体及其复合物已成功合成和特征化.
- 这些复合物表现出一种首选的双双体协调模式,并形成一个单一的二聚体.
- 这些复合物是二次醇β-化的有效催化剂,显示出有希望的反应性和选择性.
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