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首页> 外文期刊>Chemistry: A European journal >14-Electron T-Shaped [PdRXL] Complexes: Evidence or Illusion? Mechanistic Consequences for the Stille Reaction and Related Processes
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14-Electron T-Shaped [PdRXL] Complexes: Evidence or Illusion? Mechanistic Consequences for the Stille Reaction and Related Processes

机译:14电子T形[PdRXL]配合物:证据还是幻觉?斯蒂勒反应及相关过程的机械后果

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摘要

A recent claimed spectroscopic observation (by ~1H NMR) of 14-electron T-shaped 3-coordnated palladium complexes turns out to be a mis-interpretation. A thorough study of the species formed by [PdRX(AsPh_3)_2] (R = Ph, C_6Cl_2F_3; X = Cl, I) in different solvents (S = CDCl_3, THF, DMF) suggests that: 1) there is no NMR-detectable amount of [PdRX(AsPH_3)], and 2) in the presence of free arsine (AsPh_3/[PdRX(AsPh_3)_2] 2:1) the concentration of [PdRX(AsPH_3)(S)] is negligible. This clearly settles matters in the controversy of dissociative or associative pathways for the transmetalation step involved in the Stille coupling in favor of the latter: under catalytic conditions the dominant pathways is the associative reaction of the stannane with the square-planar complex [PdRXAsPh_3)_2].
机译:最近声称的14电子T形3配位的钯配合物的光谱观察(通过〜1 H NMR)证明是一种错误的解释。对[PdRX(AsPh_3)_2](R = Ph,C_6Cl_2F_3; X = Cl,I)在不同溶剂(S = CDCl_3,THF,DMF)中形成的物种的彻底研究表明:1)没有NMR-在存在游离砷(AsPh_3 / [PdRX(AsPh_3)_2] 2:1)的情况下,[PdRX(AsPH_3)]和2)的可检测量可忽略不计[PdRX(AsPH_3)(S)]的浓度。这显然解决了在斯蒂勒偶联中涉及的重金属化步骤的解离或缔合途径争议中的问题,有利于后者:在催化条件下,主要途径是锡烷与方形-平面络合物[PdRXAsPh_3] _2的缔合反应。 ]。

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