一些具有磷光功能的多联吡啶Pt（Ⅱ）和Cu（Ⅰ）配合物：合成、结构及光物理性质
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摘要
平面正方形配位不饱和Pt(Ⅱ)配合物由于丰富的光物理及光化学性质而引起了人们的广泛关注。这种构型使得配合物分子的金属中心沿dz~2方向易产生金属—金属相互作用而使得其光物理性质发生改变。由于这些配合物对易挥发的有机气体具有非常敏感的光谱响应,因而在微环境中经常被应用作为分子探针材料。本文合成出一系列含不同活性官能团的6-苯基-2,2'-联吡啶为主配体及不同辅助配体的Pt(Ⅱ)配合物,并详细调查了这些配合物在常温及低温(77K)下固态、溶液的光物理性质;同时还研究了含有新的多联吡啶配体的磷光Cu(Ⅰ)配合物的结构、光物理,得到了一些有意义的结果:
1.以(-C≡C-Ph-R)为辅助配体的含磷酸酯取代的二联吡啶环Pt(Ⅱ)配合物的合成及光物理性质:本节合成了一系列以芳炔基作辅助配体的含磷酸酯取代的二联吡啶环Pt(Ⅱ)配合物,并从吸收和发射光谱对它们的性质作了研究。发现含有N,N-二甲基的Pt(Ⅱ)配合物,对酸起作用,当有酸存在时,光谱性质发生明显的变化,这样通过光谱变化可以起到对质子的识别作用。
2.含羧酸根取代的二联吡啶环Pt(Ⅱ)配合物的合成及光物理性能研究:本章主要介绍了四种羧酸取代联吡啶环Pt(Ⅱ)配合物的合成及其光物理性质的研究,通过荧光可以看出当不存在三苯磷取代时,配合物之间存在金属与金属到配体与配体之间的~3MMLCT跃迁,而引入了三苯磷之后产生了空间位阻,不能产生分子间相互作用。
3.几种新型含三环己基磷基二亚胺Cu(Ⅰ)配合物的合成、结构及光物理性质研究:在本章中我们合成了四种含三环己基磷基二亚胺Cu(Ⅰ)配合物,得到了Cu-2,Cu-3,Cu-4的晶体结构。并对它们吸收光谱和发射光谱进行了研究,发现不同取代的二亚胺的Cu(Ⅰ)配合物的光物理性质不同,主要归因于配体的σ给电子的能力不同,随着σ给电子的能力增强,光谱发生红移。
Planar platinum(Ⅱ) complexes have attracted most attention for their abundant photophysical and photochemical properties.Indeed,this type of complexes display intensive phosphorescent emission in ~3MLCT or ~3MMLCT excited state in solid state at room temperature,and their photoluminescence excited state are often environment-sensitive which can be a useful operating principle for the design of luminescent sensory device.In this thesis,we reported a serial of platinum(Ⅱ) complexes of 6-phenyl-2,2'-bipyridine with functional group,and studied their photophysical properties in solid or solution state.In addition,we have synthesized a serial of copper(Ⅰ) complexes with substituted 2,2'-bipyridine,and researched their structure,electronic spectra properties.Many interesting results were obtained:
1.Synthesis and spesctroscopic study of cyclometalated Platinum(Ⅱ) bipyridyl complexescontain phosphonate group with(-C=C-Ph-R) ligand.A series of The platinum(Ⅱ) bipyridyl acetylide complexes were synthesised,from the study for their electronic spectra,we found that when the platinum(Ⅱ) bipyridyl acetylide complexes contained the simple amine group in the acetylide ligand utilized as a chemo-sensor for detection of micromolar concentration of protons by monitoring the changes in luminescence.
2.Synthesis and spesctroscopic study of cyclometalated Platinum(Ⅱ) bipyridyl complexes with carboxylic group.Four new cyclometalated Platinum(Ⅱ) bipyridyl complexes with carboxylic group were synthsised,we found that, Pt-13 and Pt-15 have metal-metal interaction,and Pt-14 and Pt-16 didn't have souch interaction because of the steric hindrance of triphenylphosphine as a large substituted group.
3.Synthesis,structure and electronic spectra of novel three coordinated copper(Ⅰ) complexes with tricyclohexylphosphine and substituted diimine mixed ligands. Four novel copper(Ⅰ) complexes with tricyclohexylphosphine and substituted diimine mixed ligands were obtained,and researched from their structures and electronic spectra.Cu-1,Cu-2,Cu-4 and Cu-3 have a red shifted with the increase of donating electron ability.
1.以(-C≡C-Ph-R)为辅助配体的含磷酸酯取代的二联吡啶环Pt(Ⅱ)配合物的合成及光物理性质:本节合成了一系列以芳炔基作辅助配体的含磷酸酯取代的二联吡啶环Pt(Ⅱ)配合物,并从吸收和发射光谱对它们的性质作了研究。发现含有N,N-二甲基的Pt(Ⅱ)配合物,对酸起作用,当有酸存在时,光谱性质发生明显的变化,这样通过光谱变化可以起到对质子的识别作用。
2.含羧酸根取代的二联吡啶环Pt(Ⅱ)配合物的合成及光物理性能研究:本章主要介绍了四种羧酸取代联吡啶环Pt(Ⅱ)配合物的合成及其光物理性质的研究,通过荧光可以看出当不存在三苯磷取代时,配合物之间存在金属与金属到配体与配体之间的~3MMLCT跃迁,而引入了三苯磷之后产生了空间位阻,不能产生分子间相互作用。
3.几种新型含三环己基磷基二亚胺Cu(Ⅰ)配合物的合成、结构及光物理性质研究:在本章中我们合成了四种含三环己基磷基二亚胺Cu(Ⅰ)配合物,得到了Cu-2,Cu-3,Cu-4的晶体结构。并对它们吸收光谱和发射光谱进行了研究,发现不同取代的二亚胺的Cu(Ⅰ)配合物的光物理性质不同,主要归因于配体的σ给电子的能力不同,随着σ给电子的能力增强,光谱发生红移。
Planar platinum(Ⅱ) complexes have attracted most attention for their abundant photophysical and photochemical properties.Indeed,this type of complexes display intensive phosphorescent emission in ~3MLCT or ~3MMLCT excited state in solid state at room temperature,and their photoluminescence excited state are often environment-sensitive which can be a useful operating principle for the design of luminescent sensory device.In this thesis,we reported a serial of platinum(Ⅱ) complexes of 6-phenyl-2,2'-bipyridine with functional group,and studied their photophysical properties in solid or solution state.In addition,we have synthesized a serial of copper(Ⅰ) complexes with substituted 2,2'-bipyridine,and researched their structure,electronic spectra properties.Many interesting results were obtained:
1.Synthesis and spesctroscopic study of cyclometalated Platinum(Ⅱ) bipyridyl complexescontain phosphonate group with(-C=C-Ph-R) ligand.A series of The platinum(Ⅱ) bipyridyl acetylide complexes were synthesised,from the study for their electronic spectra,we found that when the platinum(Ⅱ) bipyridyl acetylide complexes contained the simple amine group in the acetylide ligand utilized as a chemo-sensor for detection of micromolar concentration of protons by monitoring the changes in luminescence.
2.Synthesis and spesctroscopic study of cyclometalated Platinum(Ⅱ) bipyridyl complexes with carboxylic group.Four new cyclometalated Platinum(Ⅱ) bipyridyl complexes with carboxylic group were synthsised,we found that, Pt-13 and Pt-15 have metal-metal interaction,and Pt-14 and Pt-16 didn't have souch interaction because of the steric hindrance of triphenylphosphine as a large substituted group.
3.Synthesis,structure and electronic spectra of novel three coordinated copper(Ⅰ) complexes with tricyclohexylphosphine and substituted diimine mixed ligands. Four novel copper(Ⅰ) complexes with tricyclohexylphosphine and substituted diimine mixed ligands were obtained,and researched from their structures and electronic spectra.Cu-1,Cu-2,Cu-4 and Cu-3 have a red shifted with the increase of donating electron ability.
引文
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