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Insights into the ligand effects of rhodium catalysts toward reductive carbonylation of methanol to ethanol

机译：深入了解铑催化剂对甲醇还原羰基化为乙醇的配体作用

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Methanol reductive carbonylation to ethanol catalyzed by diphosphine ligand modified Rh-based catalysts has been studied. All the catalysts show ligand effects toward the turnover frequency and selectivity. Four Rh–diphosphine complexes were isolated and single crystals were obtained. These complexes were characterized by X-ray single-crystal diffraction, NMR, FTIR, and XPS. The X-ray crystal structure of [Rh2(μ-I)(μ-CO)(CO)2(dppm)2]+ was reported for the first time in this work. Based on the analysis of crystal structures, we unraveled the origin of the ligand effects of rhodium catalysts toward reductive carbonylation of methanol to ethanol. The diphosphine ligand with the appropriate number of methylene groups between two phosphorus atoms can improve the catalytic activity. The steric congestion around the empty coordination site in the Rh–diphosphine complexes led to a preferential reaction of rhodium with H2, which promoted ethanol/acetaldehyde formation.
机译：研究了二膦配体修饰的Rh基催化剂催化甲醇还原羰基化为乙醇。所有的催化剂都表现出配体对转换频率和选择性的影响。分离出四个Rh-二膦配合物，获得了单晶。这些配合物通过X射线单晶衍射，NMR，FTIR和XPS进行表征。 [Rh 2 （μ-I）（μ-CO）（CO） 2 （dppm） 2 ] + 。基于晶体结构的分析，我们阐明了铑催化剂对甲醇还原羰基化为乙醇的配位作用的起源。在两个磷原子之间具有适当数目的亚甲基的二膦配体可以提高催化活性。 Rh-二膦配合物中空配位位点附近的空间拥挤导致铑与H 2 的优先反应，从而促进了乙醇/乙醛的形成。

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