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首页> 外文期刊>Catalysis science & technology >New insights into the biphasic 'CO-free' Pauson-Khand cyclisation reaction through combined in situ spectroscopy and multiple linear regression modelling
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New insights into the biphasic 'CO-free' Pauson-Khand cyclisation reaction through combined in situ spectroscopy and multiple linear regression modelling

机译：新见解两相的“CO-free”Pauson-Khand cyclisation反应通过结合原位光谱和多线性的回归模型

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摘要

"CO-free" carbonylations are catalytic reactions, which strive to replace toxic synthesis gas with less harmful surrogate molecules like formaldehyde. This study sheds light on the mechanism of the biphasic, Rh-catalysed Pauson-Khand type cyclisation reaction by applying in situ Raman spectroscopy together with NMR, dynamic light scattering measurements, and quantum chemical calculations. The reaction is particularly challenging to analyse as the Rh-catalyst features different ligands in the aqueous and organic phase. To tackle this challenge, a novel approach was designed, coupling in situ Raman spectroscopy with an advanced data analysis model in the form of multiple linear regression. This fruitful combination of highly specific vibrational spectroscopy with state-of-the-art data analysis allowed not only identification of a new reaction mechanism, but also identification of parameters to accelerate the "CO-free" Pauson-Khand cyclisation, i.e. using mononuclear Rh-phosphine complexes with labile ligands, small organic micelles formed by an increased surfactant concentration, low formaldehyde concentration, and elevated temperature. This novel knowledge-driven optimisation protocol is superior to simple qualitative optimization routines and can be transferred to other reactions and spectroscopy techniques.
机译：“CO-free”羰基化反应催化反应,努力取代有毒合成天然气更少的有害的代孕分子甲醛。两相的机制,Rh-catalysedPauson-Khand cyclisation反应类型应用原位拉曼光谱在一起核磁共振,动态光散射测量,量子化学计算。特别具有挑战性的分析的Rh-catalyst特性不同的配体水和有机相。挑战,设计了新颖的方法,耦合与一个原位拉曼光谱先进的数据分析模型的形式多元线性回归。结合的非常具体的振动光谱学与先进的数据分析不仅允许识别的新反应机制,而且参数的识别加快“CO-free Pauson-Khand”使用单核Rh-phosphine cyclisation,即与不稳定配体复合物,小有机增加表面活性剂形成的胶束浓度、甲醛浓度低,和高温。知识优化协议是优于简单定性优化例程,可以转移到其他反应和光谱技术。

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