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首页> 外文期刊>Journal of Organometallic Chemistry >Synthesis, characterization and coordination chemistry of a new phosphite-ether ligand: The effects of alkali metal salts and the ligand/Rh molar ratio on the catalytic activity and regioselectivity of a Rh(I) complex of this ligand in the hydroformylation of styrene
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Synthesis, characterization and coordination chemistry of a new phosphite-ether ligand: The effects of alkali metal salts and the ligand/Rh molar ratio on the catalytic activity and regioselectivity of a Rh(I) complex of this ligand in the hydroformylation of styrene

机译：新型亚磷酸酯-醚配体的合成，表征和配位化学：碱金属盐和配体/ Rh摩尔比对苯乙烯加氢甲酰化反应中该配体Rh（I）配合物的催化活性和区域选择性的影响

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We have recently reported that the addition of alkali metal salts to styrene hydroformylation reactions catalyzed by Rh(I) complexes of bis(phosphite) ligands can significantly improve the iso regioselectivity. To better understand the effects of the alkali metal salts on these styrene hydroformylation reactions, a monodentate phosphite-ether ligand, (2,2′-C_(12)H_8O_2)POCH_2CH_2OCH_3, 1 has been prepared, and its Rh(I) complex has been evaluated as a catalyst for the hydroformylation of styrene. Both the activity and regioselectivity of the catalyst are sensitive to the ligand:Rh molar ratio and to the presence of salts such as LiBPh_4·3dme, NaBPh_4 and HgCl_2. The most active catalyst has a 1:2.5 Rh:1 molar ratio and a 1:8 Rh:Li~+ molar ratio, but the most regioselective catalyst has a 1:8.2 Rh:1 ratio and a 1:4 Rh:Li~+ ratio. Model complexes for various steps in the catalytic cycle, cis-Mo(CO)_4(1)_2, 6, cis-PtCl_2(1)_2, 7, and PdCl_2(1)_2, 8, have been synthesized and characterized by multinuclear NMR spectroscopy and X-ray crystallography to provide insight into the factors that may affect the rates and regioselectivities of the hydroformylation catalysts. The cis-trans isomerization of 6 in the presence of catalytic amount HgCl_2 has been carried out to determine the cis-trans preference of 1 in the octahedral coordination geometry.
机译：最近，我们报道了由双（亚磷酸酯）配体的Rh（I）配合物催化向苯乙烯加氢甲酰化反应中添加碱金属盐可以显着提高iso / n区域选择性。为了更好地理解碱金属盐对这些苯乙烯加氢甲酰化反应的影响，已制备了单齿亚磷酸酯-醚配体（2,2'-C_（12）H_8O_2）POCH_2CH_2OCH_3，1，并且其Rh（I）配合物具有被评估为苯乙烯加氢甲酰化的催化剂。催化剂的活性和区域选择性都对配体：Rh摩尔比和盐的存在敏感，例如LiBPh_4·3dme，NaBPh_4和HgCl_2。活性最高的催化剂的摩尔比为1：2.5，Rh：Li〜+摩尔比为1：8，区域选择性最高的催化剂的比率为1：8.2 Rh：1，Rh：Li〜为1：4，Rh：Li〜 +比例。已合成并通过多核表征了催化循环中各个步骤的模型配合物cis-Mo（CO）_4（1）_2，6，cis-PtCl_2（1）_2，7，和PdCl_2（1）_2，8， NMR光谱学和X射线晶体学可以深入了解可能影响加氢甲酰化催化剂的速率和区域选择性的因素。已经进行了在催化量HgCl_2存在下6的顺反异构化，以确定八面体配位几何中1的顺反偏好。

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