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首页> 外文期刊>Chemistry: A European journal >Palladium(II) Complexes of New Bulky Bidentate Phosphanes: Active and Highly Regioselective Catalysts for the Hydroxy carbonylation of Styrene
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Palladium(II) Complexes of New Bulky Bidentate Phosphanes: Active and Highly Regioselective Catalysts for the Hydroxy carbonylation of Styrene

机译：新型大体积双齿膦的钯（II）配合物：苯乙烯羟基羰基化的活性和高区域选择性催化剂

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摘要

The synthesis of four newbulky bidentate phosphines that pos-sess both tert-butyl and trifluorome-thylphenyl substituents is described.Symmetric ligands were readily ob-tained by alkylation of phosphidobor-anes of the type Li[P(BH_3)(tBu)(Ar)]with dihaloalkanes. Non-symmetric li-gands were prepared from a new stableprecursor, tBu_2P(BH_3)(CH_2)_3Br, thatshould prove useful for other ligandsyntheses. Palladium(II) complexes ofthe four new ligands were prepared and were characterised by spectroscop-ic methods, microanalysis and X-raycrystallography. The new [PdC1_2(L)]complexes were evaluated as catalystsfor the hydroxycarbonylation of sty-rene and found to give unprecedentedregioselectivity and yields for a diphos-phine-based catalyst. A study on pro-moter effects reveals that the presenceof acid and chloride is necessary toachieve such selectivities. It has beenproposed in the literature that suchconditions result in a new pathway inwhich styrene is converted into 2-phe-nethyl chloride, with the latter beingthe real substrate in the reaction. How-ever, a deuterium labelling study seemsto rule out this mechanism, at leastunder the conditions used herein.
机译：描述了同时具有叔丁基和三氟甲基苯基苯基取代基的四种新的二齿膦膦的合成。通过Li [P（BH_3）（tBu）（Ar）型磷硼烷的烷基化可轻松获得对称的配体）]与二卤代烷烃。由新的稳定前体tBu_2P（BH_3）（CH_2）_3Br制备非对称配体，这对其他配体合成很有用。制备了四个新配体的钯（II）配合物，并通过分光光度法，显微分析和X射线晶体学对其进行了表征。评价了新的[PdC1_2（L）]配合物作为苯乙烯-苯乙烯羰基化的催化剂，发现该化合物对二膦膦类催化剂具有前所未有的区域选择性和产率。对促进剂作用的研究表明，要实现这样的选择性，必须要有酸和氯化物的存在。在文献中已经提出，这种条件导致新的途径，其中苯乙烯被转化为2-苯乙基氯，后者是反应中的真正底物。但是，氘标记研究似乎至少在本文使用的条件下可以排除这种机制。

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