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

机译：洞察铑催化剂朝向乙醇还原羰基化的配体效果的见解

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摘要

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 [Rh-2(mu-I)(mu-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 H-2, which promoted ethanol/acetaldehyde formation.
机译：研究了二膦配体改性Rh基催化剂催化的乙醇还原羰基化。 所有催化剂都显示出朝向周转频率和选择性的配体效应。 分离出四个rh-二膦络合物，得到单晶。 这些配合物的特征在于X射线单晶衍射，NMR，FTIR和XPS。 在这项工作中首次报告[rh-2（mu-i）（mu-i）（mu-c）（mu-co）（co）（2）（2）（2）（2）（+）的X射线晶体结构。 基于晶体结构的分析，我们解开了铑催化剂对甲醇的还原羰基化的配体对乙醇的起源。 具有适当数量的两种磷原子之间的二膦配体可以改善催化活性。 rh-二膦络合物中的空配位位点周围的空间充血导致铑与H-2的优先反应，促进乙醇/乙醛形成。

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  • 来源
    《RSC Advances》 |2017年第79期|共8页
  • 作者

    Chen Yingzan; Liu Dianhua; Yu Yi;

  • 作者单位

    East China Univ Sci &

    Technol State Key Lab Chem Engn Shanghai 200237 Peoples R China;

    East China Univ Sci &

    Technol State Key Lab Chem Engn Shanghai 200237 Peoples R China;

    East China Univ Sci &

    Technol State Key Lab Chem Engn Shanghai 200237 Peoples R China;

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  • 正文语种 eng
  • 中图分类 化学;
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