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The effect of carbon dioxide on hydroformylation of 1-hexene by an immobilized rhodium catalyst.

机译：二氧化碳对固定化铑催化剂对1-己烯加氢甲酰化的影响。

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In situ high-pressure Diffuse Reflectance Infrared Fourier Transform Spectroscopy was performed to investigate the hydroformylation of 1-hexene in supercritical carbon dioxide. A rhodium complex was immobilized on phosphinated silica and used as a catalyst. The changes in the infrared spectrum over time showed the reaction profile, which was used to evaluate the effect of pressure on the reaction mechanism. Increasing the reaction pressure by adding carbon dioxide increased 1-hexene conversion and hydroformylation activity. Specific changes observed in the infrared spectrum when the supported complex interacted with carbon monoxide, hydrogen and/or mixture of carbon monoxide and hydrogen in the presence and absence of carbon dioxide at elevated pressures revealed the nature of the reacting species over time and pressure, and clearly demonstrated the role of carbon dioxide when it was used as the solvent. The catalyst activity and structure were compared for reaction in supercritical carbon dioxide with that in nitrogen in order to more completely delineate the role of the supercritical solvent on the reaction mechanism. It was found that the resting state of the catalyst was HRh(CO)2Lx, L=PPh 2CH2CH2 bound to silica, independent of the reaction pressure and the presence of carbon dioxide or nitrogen.
机译：进行了原位高压漫反射红外傅里叶变换光谱研究了1-己烯在超临界二氧化碳中的加氢甲酰化反应。铑配合物固定在次膦化的二氧化硅上并用作催化剂。红外光谱随时间的变化显示了反应曲线，该曲线用于评估压力对反应机理的影响。通过添加二氧化碳增加反应压力增加了1-己烯转化率和加氢甲酰化活性。当负载的配合物在存在和不存在二氧化碳的高压下与一氧化碳，氢气和/或一氧化碳和氢气的混合物相互作用时，在红外光谱中观察到的特定变化揭示了反应物种随时间和压力的变化，以及清楚地证明了二氧化碳用作溶剂时的作用。比较了催化剂在超临界二氧化碳中的反应活性和结构以及在氮气中的反应活性，以便更全面地描述超临界溶剂在反应机理中的作用。发现催化剂的静止状态为HRh（CO）2 L x，L ＝ PPh 2 CH 2 CH 2与二氧化硅键合，与反应压力和二氧化碳或氮气的存在无关。

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