新型膦氧類化合物及其鉑配合物的合成與發(fā)光性能研究
發(fā)布時間：2019-02-25 18:07
【摘要】：本文設(shè)計合成了一系列新型的膦氧類大位阻化合物以及鉑配合物和異核雙金屬Pt-M配合物。應(yīng)用核磁、元素分析、X-射線單晶衍射對化合物進行了結(jié)構(gòu)確證,系統(tǒng)研究了化合物的發(fā)光性能。通過測定它們的紫外吸收光譜和循環(huán)伏安圖譜,計算出了化合物的HOMO、LUMO軌道。主要研究內(nèi)容如下:1、合成了六種新型的苯并咪唑、三氮唑和四氮唑膦氧類化合物(L1-L6),其中,苯并咪唑系列化合物L(fēng)1,L3,L4都具有較高的發(fā)光量子效率,固體發(fā)光效率均在50%以上�；衔風(fēng)1表現(xiàn)出了深藍色發(fā)光,溶液發(fā)光效率為45.6%,固體發(fā)光效率高達69.4%。苯并咪唑上引入推電子基導(dǎo)致化合物發(fā)光增強,吸電子基使化合物發(fā)射光譜藍移。2、以化合物L(fēng)1-L5為解聚配體、ppy為環(huán)金屬配體,合成了五種金屬Pt(Ⅱ)配合物(Pt-L1~Pt-L5)。Pt(Ⅱ)與L1-L4和ppy分別以N^O、C^N的形式配位,形成平面四邊形結(jié)構(gòu)。晶體結(jié)構(gòu)分析證明,分子間沒有明顯的堆積相互作用。Pt(Ⅱ)與L5和ppy形成雙核鉑配合物。這五個配合物均表現(xiàn)出長壽命的高效磷光發(fā)射,其中配合物Pt-L5的固體發(fā)光效率高達77%。配體上取代基的改變對配合物的發(fā)射峰位置以及軌道能級影響不大。3、以四氮唑膦氧化合物L(fēng)6為配體,結(jié)合ppy合成了6種新型異核雙金屬配合物Pt-L6-M(M=Na、Fe、Zn、Mg、Ca、Cd)。其中配合物Pt-L6-Na結(jié)構(gòu)獨特,中心Pt(Ⅱ)離子形成了六配位的變形八面體構(gòu)型。該系列配合物-P=O基團的O原子均未參與鉑的配位。這類配合物表現(xiàn)出了非常好的磷光性質(zhì),其固體發(fā)光效率分別為62.5%、54.2%、54.6%、58.9%、42.8%、41.6%,而溶液發(fā)光效率分別為55.4%、94.1%、93.7%、94.2%、89.0%、88.6%。77K下配合物的磷光發(fā)射證明,所有鉑配合物的磷光發(fā)射主要是來自配體三線態(tài)(3LC)的輻射躍遷。
[Abstract]:In this paper, we have designed and synthesized a series of novel phosphonoxins, platinum complexes and heteronuclear bimetallic Pt-M complexes. The structure of the compound was confirmed by NMR, elemental analysis and X-ray single crystal diffraction. The luminescent properties of the compound were studied systematically. The HOMO,LUMO orbitals of the compounds were calculated by measuring their UV absorption spectra and cyclic voltammetry. The main contents are as follows: 1. Six new benzimidazole, triazole and tetrazolium phosphine oxide compounds (L1-L6) were synthesized. Among them, benzimidazole series compounds L _ 1, L _ 3, L _ 4 all have high luminescence quantum efficiency. The solid luminescence efficiency is above 50%. The luminescence efficiency of the compound L1 is 45.6% in solution and 69.4% in solid state, and the luminescence efficiency in solution is 45.6% and that in solid state is 69.4%. The introduction of electron-pushing groups on benzimidazole resulted in the enhancement of the luminescence of the compounds. The emission spectra of the compounds were blue-shifted by the electron-absorbing group. The compound L1-L5 was used as the depolymerized ligand and the ppy as the cyclic metal ligand. Five metal Pt (鈪，
本文編號：2430402
[Abstract]:In this paper, we have designed and synthesized a series of novel phosphonoxins, platinum complexes and heteronuclear bimetallic Pt-M complexes. The structure of the compound was confirmed by NMR, elemental analysis and X-ray single crystal diffraction. The luminescent properties of the compound were studied systematically. The HOMO,LUMO orbitals of the compounds were calculated by measuring their UV absorption spectra and cyclic voltammetry. The main contents are as follows: 1. Six new benzimidazole, triazole and tetrazolium phosphine oxide compounds (L1-L6) were synthesized. Among them, benzimidazole series compounds L _ 1, L _ 3, L _ 4 all have high luminescence quantum efficiency. The solid luminescence efficiency is above 50%. The luminescence efficiency of the compound L1 is 45.6% in solution and 69.4% in solid state, and the luminescence efficiency in solution is 45.6% and that in solid state is 69.4%. The introduction of electron-pushing groups on benzimidazole resulted in the enhancement of the luminescence of the compounds. The emission spectra of the compounds were blue-shifted by the electron-absorbing group. The compound L1-L5 was used as the depolymerized ligand and the ppy as the cyclic metal ligand. Five metal Pt (鈪，
本文編號：2430402
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