Jiang Xin-Dong, Matsukawa Shiro, Yamamoto Yohsuke
Department of Chemistry, Graduate School of Science, Hiroshima University, 1-3-1 Kagamiyama, Higashi-Hiroshima, 739-8526, Japan.
Dalton Trans. 2008 Jul 28(28):3678-87. doi: 10.1039/b802947d. Epub 2008 Jun 13.
A series of anti-apicophilic pentacoordinate phosphoranes (with one chelating substituent in an O-equatorial, C-apical bonding mode at pentacoordinated phosphorus atom) bearing a para-substituted aryl group (-C(6)H(4)(p-X); X = H, CF(3), F, OMe) or a mesityl (2,4,6-trimethylphenyl) group were isolated using a novel bulky bidentate ligand with two C(2)F(5) groups. These phosphoranes were stable to isomerization at room temperature, and quantitatively converted into the corresponding more stable isomers (O-apical) at elevated temperatures in solution. On the basis of a kinetic study, the free energy of activation (DeltaG(double dagger)) of the stereomutation of the O-equatorial mesitylphosphorane to its O-apical isomer was higher than that of the CF(3) derivative by 2.6 kcal mol(-1), giving rise to a further example of the steric effect of the C(2)F(5) group to freeze the isomerization of the pentacoordinate phosphorus compounds. Kinetic measurements of the isomerization of the O-equatorial ortho-unsubstituted derivatives (-C(6)H(4)(p-X)) to the corresponding O-apical isomers suggested that the O-equatorial isomers were stabilized by the pi --> sigma*(P-O) interaction in the ground state.
使用一种带有两个五氟乙基基团的新型大位阻双齿配体,分离得到了一系列反亲顶五配位磷烷(在五配位磷原子上,一个螯合取代基以氧-赤道面、碳-顶点键合模式存在),其带有对取代芳基(-C(6)H(4)(p-X);X = H、CF(3)、F、OMe)或均三甲苯基(2,4,6-三甲基苯基)基团。这些磷烷在室温下对异构化稳定,并且在溶液中升高温度时定量转化为相应更稳定的异构体(氧-顶点)。基于动力学研究,氧-赤道面均三甲苯基磷烷向其氧-顶点异构体立体异构化的活化自由能(ΔG‡)比三氟甲基衍生物的高2.6 kcal mol(-1),这进一步例证了五氟乙基基团的空间效应可抑制五配位磷化合物的异构化。对氧-赤道面邻位未取代衍生物(-C(6)H(4)(p-X))向相应氧-顶点异构体异构化的动力学测量表明,氧-赤道面异构体在基态通过π→σ*(P-O)相互作用得以稳定。