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首页> 外文期刊>Coordination chemistry reviews >Electronic structures, photophysical properties, and electrochemistry of ruthenium(Ⅱ)(bpy)_2 pyridylimidazole complexes
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Electronic structures, photophysical properties, and electrochemistry of ruthenium(Ⅱ)(bpy)_2 pyridylimidazole complexes

机译：钌（Ⅱ）（bpy）_2吡啶基咪唑配合物的电子结构，光物理性质和电化学

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摘要

The properties of Ru~Ⅱ complexes involving the imidazole moiety are discussed. Complexes [Ru(bpy)_2(L)]~(2+) [bpy = 2,2'-bipyridine, L = 2-(2'-pyridyl)imidazole (2-pimH) and 4-(2'-pyridyl)imidazole (4-pimH)] have been synthesized and fully characterized. Reduction potentials are 0.76 V vs. Fc~+/Fc~0 for both complexes in acetonitrile solution, and the deprotonated complexes undergo irreversible electrochemical oxidation at 0.38 V vs. Fc~+/Fc~0. Density functional theory (DFT) calculations suggest that oxidation of the protonated complexes is primarily metal-based and that of the deprotonated complexes is ligand-centered. The pK_a of the 4-pimH complex was found to be 9.7 ± 0.2; the pK_a of the 2-pimH complex is 7.9 ± 0.2. Luminescence lifetimes (L = 4-pimH, 277 ns; 2-pimH, 224ns; 4pim~- , 40ns; 2pim~- , 34ns in 5% methanol/water solution) combined with quantum yield data and acid-base behavior suggest that the non-coordinated imidazole nitrogen tunes deactivation pathways.
机译：讨论了含咪唑部分的Ru〜Ⅱ配合物的性质。配合物[Ru（bpy）_2（L）]〜（2+）[bpy = 2,2'-联吡啶，L = 2-（2'-吡啶基）咪唑（2-pimH）和4-（2'-吡啶基）咪唑（4-pimH）]已合成并充分表征。乙腈溶液中两种络合物的还原电位均为0.76 V vs. Fc〜+ / Fc〜0，去质子化的络合物在0.38 V vs. Fc〜+ / Fc〜0时发生不可逆的电化学氧化。密度泛函理论（DFT）计算表明，质子化配合物的氧化主要基于金属，而去质子化配合物的氧化则以配体为中心。发现4-pimH复合物的pK_a为9.7±0.2。 2-pimH复合物的pK_a为7.9±0.2。在5％甲醇/水溶液中的发光寿命（L = 4-pimH，277 ns; 2-pimH，224ns; 4pim〜-，40ns; 2pim〜-，34ns）结合量子产率数据和酸碱行为表明非配位的咪唑氮可调节失活途径。

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  • 来源
    《Coordination chemistry reviews》 |2010年第16期|P.1803-1811|共9页
  • 作者

    Kyle M. Lancaster; James B. Gerken; Alec C. Durrell; Joshua H. Palmer; Harry B. Gray;

  • 作者单位

    Beckman Institute, California Institute of Technology, 1200 E California Blvd, Pasadena, CA 91125, USA;

    Department of Chemistry, University of Wisconsin-Madison, Madison, WI 53706, USA;

    rnBeckman Institute, California Institute of Technology, 1200 E California Blvd, Pasadena, CA 91125, USA;

    rnBeckman Institute, California Institute of Technology, 1200 E California Blvd, Pasadena, CA 91125, USA;

    rnBeckman Institute, California Institute of Technology, 1200 E California Blvd, Pasadena, CA 91125, USA;

  • 收录信息 美国《科学引文索引》(SCI);美国《生物学医学文摘》(MEDLINE);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    ruthenium; pyridylimidazoles; photophysics; cyclic voltammetry;

    机译：钌;吡啶咪唑;光物理循环伏安法;

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