Substituent and Solvent Effects on Square-Planar-Tetrahedral Equilibria of Bis[4-(arylimino)pentan-2-onato]nickel(II) and Bis[1-aryl-3-(phenylimino)butan-1-onato]nickel(II) Complexes

Mori Y; Shirase H; Fukuda Y

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Substituent and Solvent Effects on Square-Planar-Tetrahedral Equilibria of Bis[4-(arylimino)pentan-2-onato]nickel(II) and Bis[1-aryl-3-(phenylimino)butan-1-onato]nickel(II) Complexes

机译：取代基和溶剂对双[4-（芳基基）戊丹-2-onato]镍（II）和双[1-芳基-3-（苯基亚氨基）丁丹-1-onato]镍（II）的方形-四面体平衡的影响）配合物

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Nickel(II) bis(Schiff base) complexes, NiL2 (1a-1f) and NiL2' (2a-2e) (where L = 4-(arylimino)pentan-2-onate and L' = 1-aryl-3-(phenylimino)butan-1-onate), exist in an equilibrium of square-planar (Sp) and tetrahedral (Td) forms in non-coordinating solvents. The Td form is more stabilized in polar solvents such as CH2Cl2 than in non-polar solvents Such as toluene. Thermodynamic data were determined from temperature-dependent H-1 NMR contact shift. It is suggested for 1a-1f that the oxygen atoms in Td Form interact with solvent Such as chloroform via hydrogen building. With increase in electron-donating ability of the substituents on aryl groups, the Td form becomes more favored. The free energy change roughly correlates with Hammet's sigma(p) value. The UV-vis-NIR spectra indicated that the ligand field strength increases with the electron-donating ability of the substituents in both the Sp and Td forms. Results of DFT calculation suggest that the observed substituent effect may result from small perturbation of the metal-ligand bonding character.

机译：镍（II）双（席夫碱）配合物NiL2（1a-1f）和NiL2'（2a-2e）（其中L = 4-（芳基）戊基-2-壬酸酯，L'= 1-芳基-3-（在非配位溶剂中以正方形平面（Sp）和四面体（Td）形式的平衡形式存在。 Td形式在极性溶剂（例如CH2Cl2）中比在非极性溶剂（例如甲苯）中更稳定。根据温度相关的H-1 NMR接触位移确定热力学数据。对于1a-1f，建议Td形式的氧原子通过氢的形成与溶剂（例如氯仿）相互作用。随着芳基上取代基的供电子能力的增强，Td形式变得更加有利。自由能变化与Hammet的sigma（p）值大致相关。 UV-vis-NIR光谱表明，随着Sp和Td形式的取代基的供电子能力，配体场强都会增加。 DFT计算的结果表明，观察到的取代基效应可能是由于金属-配体键合特性的微小扰动引起的。

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《Bulletin of the Chemical Society of Japan》 |2008年第9期|共8页
作者
Mori Y; Shirase H; Fukuda Y;
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正文语种 eng
中图分类化学;
关键词
PROTON MAGNETIC-RESONANCE; NICKEL(II) COMPLEXES; LIGAND SUBSTITUTION; NUCLEAR-RESONANCE; KINETICS; INTERCONVERSION; THERMODYNAMICS; CALIBRATION; MECHANISM; COPPER(2);

机译：质子磁共振;镍络合物;配体取代;核磁共振;动力学;互变;热力学;定标;机理;铜（2）;

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1. Substituent and Solvent Effects on Square-Planar-Tetrahedral Equilibria of Bis[4-(arylimino)pentan-2-onato]nickel(II) and Bis[1-aryl-3-(phenylimino)butan-1-onato]nickel(II) Complexes [J] . Mori Y, Shirase H, Fukuda Y Bulletin of the Chemical Society of Japan . 2008,第9期

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2. Bis[4-(methylthio)phenylmethyleneaminophenyl] disulfide, 2-[4-(methylthio)phenyl]-2,3-dihydro-1,3-benzothiazole, and its nickel(II) and cobalt(II) complexes: Synthesis, adsorption on gold surface and electrochemical characterization [J] . E. K. Beloglazkina, A. G. Majouga, I. V. Yudin, Journal of sulfur chemistry . 2007,第2期

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Substituent and Solvent Effects on Square-Planar-Tetrahedral Equilibria of Bis[4-(arylimino)pentan-2-onato]nickel(II) and Bis[1-aryl-3-(phenylimino)butan-1-onato]nickel(II) Complexes

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