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首页> 外文期刊>Chemistry: A European journal >Electronic Structural Changes between NickeI(n)-Semiquinonato and Nickel(m)-Catecholato States Driven by Chemical and Physical Perturbation
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Electronic Structural Changes between NickeI(n)-Semiquinonato and Nickel(m)-Catecholato States Driven by Chemical and Physical Perturbation

机译：化学和物理扰动驱动NickeI（n）-Semiquinonato和Nickel（m）-Catecholato状态之间的电子结构变化

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摘要

The selective synthesis of tet-racoordinate square-planar low-spin nickel(II)-semiquinonato (Ni~(II)-SQ) and nickel(III)-catecholato (Ni~(III)-Cat) complexes,1 and 2,respectively,was achieved by using bidentate ligands with modulated nitrogen-donor ability to the nickel ion.The electronic structures of 1 and 2 were revealed by XPS and EPR measurements.The absorption spectra of 1 and 2 in a noncoordinating solvent,dichloromethane (CH_2C1_2),are completely different from those in tet-rahydrofuran (THF),being a coordinating solvent.As expected from this result,the gradual addition of N,N-di-methylformamide (DMF),which is also a coordinating solvent like THF,into a solution of 1 or 2 in CH_2C1_2 leads to color changes from blue (for 1) and brown (for 2) to light green,which is the same color observed for solutions of 1 or 2 in THF.Furthermore,the same color changes are induced by varying the temperature.Such spectral changes are attributable to the transformation from square-planar low-spin Ni~(II)-SQ and Ni~(III)-Cat complexes to octahedral high-spin Ni~(II)-SQ ones,caused by the coordination of two solvent molecules to the nickel ion.
机译：tet-座标方平面低旋镍（II）-半喹诺酮（Ni〜（II）-SQ）和镍（III）-邻苯二酚（Ni〜（III）-Cat）配合物的选择性合成1、2通过使用对氮离子具有调节性的氮供体能力的二齿配体，分别获得了电子。通过XPS和EPR测量揭示了1和2的电子结构。在非配位溶剂二氯甲烷（CH_2C1_2）中1和2的吸收光谱。完全不同于四氢呋喃（THF）中的配位溶剂。从该结果可以预料，将N，N-二甲基甲酰胺（DMF）（也是THF等配位溶剂）逐步加入在CH_2C1_2中1或2的溶液导致颜色从蓝色（对于1）和棕色（对于2）变为浅绿色，这与在THF中1或2的溶液所观察到的颜色相同。温度变化引起的这种光谱变化归因于方平面低spi的转换Ni〜（II）-SQ和Ni〜（III）-Cat与八面体高自旋Ni〜（II）-SQ的配合物，是由于两个溶剂分子与镍离子的配位所致。

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