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首页> 外文期刊>Polyhedron: The International Journal for Inorganic and Organometallic Chemistry >H-type aggregation of functional metal ion sensing phthalocyanines: Synthesis, characterization and electrochemistry
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H-type aggregation of functional metal ion sensing phthalocyanines: Synthesis, characterization and electrochemistry

机译：功能金属离子感测酞菁的H型聚集体：合成，表征和电化学

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摘要

We report, in this study, the preparation and physical characterization of the peripherally functionalized ionophore ligand, 4,5-bis(6-hydroxyhexan- 3ylthio)-1,2-dicyanobenzene (1) and its branched thioalcohol-substituted phthalocyanines, 2,3,7,8,12,13,17,18-octakis{6-hydroxyhexan-3-ylthio)-metal (II) or (III) phthalocyanines {M{Pc[SCH(C_3H_7)(C _2H_5OH)]_8} {M = Pb(II) (2), Zn(II) (3), Cu(II) (4), Co(II) (5) and Mn(III), X = Cl~- (6)} which can selectively bind soft-metal ions such as silver (I) and palladium (II). It was observed by means of UV-Vis absorption spectrophotometry that the aggregates formed lead to a low solubility of the phthalocyanines in protic solvents, such as low molecular alcohols. However, the addition of AgNO_3 and Na_2PdCl _4 into a THF-MeOH solution of {M{Pc[SCH(C_3H _7)(C_2H_5OH)]_8X} {M = Pb(II) (2), Zn(II) (3), Cu(II) (4), Co(II) (5) and Mn(III), X = Cl~- (6)} induced optical changes, which indicated the formation of twisted H-type dimers (blue shift, face-to-face fashion) of {M{Pc[SCH(C_3H_7)(C _2H_5OH)]_8} complexes, bound by four PdCl _2 and AgNO_3 units in THF solution. Elemental analysis data, matrix-assisted laser desorption ionization time-of-flight mass spectrometry (MALDI-TOF/MS), FT-IR, ~1H, ~(13)C NMR, and UV-Vis spectral data were used as complementary techniques. Voltammetry and in situ spectroelectrochemistry of the complexes were performed on Pt in DMSO/TBAP. The first reduction and oxidation processes of 5 were found to be split due to the presence of facile equilibria between the species coordinated differently at axial positions. The Mn(III)Pc(-2)X~- complex (6) displayed well-defined colour changes during its reduction processes. The redox behaviour of the Mn(III)Pc(-2)X~- complex was observed to be affected significantly by the existence of oxygen in solution due to the formation of μ-oxo MnPc species, Mn(III)Pc-O-PcMn(III). This effect was clarified well by in situ spectroelectrochemical measurements.
机译：我们在这项研究中报告了外围功能化的离子载体配体4,5-双（6-羟基己-3-基硫基）-1,2-二氰基苯（1）及其支链硫醇取代的酞菁的制备和物理表征，2， 3,7,8,12,13,17,18-辛基{6-羟基己-3-基硫基）-金属（II）或（III）酞菁{M {Pc [SCH（C_3H_7）（C _2H_5OH）] _ 8} {M = Pb（II）（2），Zn（II）（3），Cu（II）（4），Co（II）（5）和Mn（III），X = Cl〜-（6）}，其中可以选择性地结合软金属离子，例如银（I）和钯（II）。通过UV-Vis吸收分光光度法观察到，形成的聚集体导致酞菁在质子溶剂如低分子醇中的低溶解度。但是，将AgNO_3和Na_2PdCl _4添加到{M {Pc [SCH（C_3H _7）（C_2H_5OH）] _ 8X} {M = Pb（II）（2），Zn（II）（3）的THF-MeOH溶液中，Cu（II）（4），Co（II）（5）和Mn（III），X = Cl〜-（6）}引起的光学变化，表明形成了扭曲的H型二聚体（蓝移，面{M {Pc [SCH（C_3H_7）（C _2H_5OH）] _ 8}络合物的表面修饰），由THF溶液中的四个PdCl _2和AgNO_3单元结合。元素分析数据，基质辅助激光解吸电离飞行时间质谱（MALDI-TOF / MS），FT-IR，〜1H，〜（13）C NMR和UV-Vis光谱数据用作补充技术。络合物的伏安法和原位光谱电化学在DMSO / TBAP中的Pt上进行。发现5的第一个还原和氧化过程由于存在于轴向位置以不同方式协调的物种之间存在的容易的平衡而分裂。 Mn（III）Pc（-2）X-络合物（6）在还原过程中显示出明确的颜色变化。观察到Mn（III）Pc（-2）X〜-络合物的氧化还原行为受μ-氧代MnPc物种Mn（III）Pc-O-形成的溶液中氧的存在的显着影响。 PcMn（III）。通过原位光谱电化学测量很好地阐明了这种作用。

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