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首页> 外文期刊>Chemistry: A European journal >Cyclometalated iridium(III)-polyamine complexes with intense and long-lived multicolor phosphorescence: Synthesis, crystal structure, photophysical behavior, cellular uptake, and transfection properties
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Cyclometalated iridium(III)-polyamine complexes with intense and long-lived multicolor phosphorescence: Synthesis, crystal structure, photophysical behavior, cellular uptake, and transfection properties

机译：具有强力和长寿命多色磷光的环金属化铱（III）-多胺配合物：合成，晶体结构，光物理行为，细胞吸收和转染特性

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摘要

A new class of phosphorescent cyclometalated iridium(III)-polyamine complexes [{Ir(NC) _2} _n(bPEI)](PF _6) _n (bPEI=branched poly(ethyleneimine), average M _w=25 kDa, n=15.6-27.4; HNC=2-phenylpyridine Hppy (1 a), 2-((1,1'-biphenyl)-4-yl)pyridine Hpppy (2 a), 2-phenylquinoline Hpq (3 a), 2-phenylbenzothiazole Hbt (4 a), 2-(1-naphthyl)benzothiazole Hbsn (5 a)) and [Ir(NC) _2(en)](PF _6) (en=ethylenediamine; HNC=Hppy (1 b), Hpppy (2 b), Hpq (3 b), Hbt (4 b), Hbsn (5 b)) have been synthesized and characterized. The X-ray crystal structure of complex 5 b was also determined. All of these complexes showed a reversible iridium(IV/III) oxidation couple at +1.01 to +1.26 V and a quasi-reversible ligand-based reduction couple at -1.54 to -2.08 V (versus SCE). Upon photoexcitation, the complexes displayed intense and long-lived green to orange-red emission in fluid solutions at room temperature and in low-temperature glass. Lipophilicity measurements indicated that bPEI played a dominant role in the polar nature of complexes 1 a-5 a, thus rendering them very soluble in aqueous solutions. Inductively coupled plasma-mass spectrometry (ICP-MS) and confocal laser scanning microscopy (CLSM) data indicated that an energy-requiring process, such as endocytosis, was involved in the cellular uptake of all of the complexes. In addition, the cytotoxicity of the complexes toward human cervix epithelioid carcinoma (HeLa) and human embryonic kidney 293T (HEK293T) cell-lines has been evaluated by the 3-(4,5-dimethyl-2-thiazolyl)-2, 5-diphenyltetrazolium bromide (MTT) assay. The DNA-binding properties of complex 5 a have been investigated by gel-retardation assays and the polyplexes that were formed from this complex with plasmid DNA (pDNA) were studied by zeta-potential measurements and particle-size estimation. Furthermore, complex 5 a was grafted with poly(ethylene glycol) (PEG, average M _w=2 kDa) to different extents, thereby yielding the phosphorescent copolymers PEG _(12.3)-g-5 a, PEG _(25.4)-g-5 a, and PEG _(62.1)-g-5 a. Interestingly, these copolymers showed enhanced transfection activity, as revealed by in vitro transfection experiments with tissue-culture-based luciferase assays.
机译：一类新型的磷光环金属化铱（III）-多胺配合物[{Ir（NC）_2} _n（bPEI）]（PF _6）_n（bPEI =支链聚（乙烯亚胺），平均M _w = 25 kDa，n = 15.6 -27.4; HNC = 2-苯基吡啶Hppy（1 a），2-（（（1,1'-联苯）-4-基）吡啶Hpppy（2 a），2-苯基喹啉Hpq（3 a），2-苯基苯并噻唑Hbt （4a），2-（1-萘基）苯并噻唑Hbsn（5a））和[Ir（NC）_2（en）]（PF _6）（en =乙二胺; HNC = Hppy（1b），Hpppy（2 b），Hpq（3 b），Hbt（4 b），Hbsn（5 b））已合成并表征。还测定了配合物5b的X射线晶体结构。所有这些络合物在+1.01至+1.26 V时均显示出可逆的铱（IV / III）氧化偶，在-1.54至-2.08 V时（与SCE相比）显示出基于准可逆配体的还原偶合。在光激发下，该复合物在室温和低温玻璃中的流体溶液中显示出强烈且长寿命的绿色至橙红色发射。亲脂性测量表明，bPEI在复合物1a-5a的极性性质中起主要作用，因此使其在水溶液中的溶解度很高。电感耦合等离子体质谱法（ICP-MS）和共聚焦激光扫描显微镜（CLSM）数据表明，所有复合物的细胞摄取都涉及能量消耗过程，例如胞吞作用。此外，该复合物对人宫颈上皮样癌（HeLa）和人胚胎肾293T（HEK293T）细胞系的细胞毒性已通过3-（4,5-二甲基-2-噻唑基）-2，5-溴化二苯四唑（MTT）分析。复合物5a的DNA结合特性已通过凝胶延迟分析进行了研究，并通过ζ电势测量和粒度估算研究了由该复合物与质粒DNA（pDNA）形成的多聚体。此外，将复合物5a以不同程度接枝有聚乙二醇（PEG，平均M _w = 2 kDa），从而得到磷光共聚物PEG _（12.3）-g-5a，PEG _（25.4）-g -5a和PEG _（62.1）-g-5a。有趣的是，这些共聚物显示出增强的转染活性，如通过基于组织培养的萤光素酶测定的体外转染实验所揭示的那样。

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