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首页> 美国卫生研究院文献>Proceedings of the National Academy of Sciences of the United States of America >PNAS Plus: Self-assembled ruthenium (II) metallacycles and metallacages with imidazole-based ligands and their in vitro anticancer activity
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PNAS Plus: Self-assembled ruthenium (II) metallacycles and metallacages with imidazole-based ligands and their in vitro anticancer activity

机译：PNAS Plus：具有咪唑基配体的自组装钌（II）金属环和金属环及其体外抗癌活性

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摘要

Six tetranuclear rectangular metallacycles were synthesized via the [2+2] coordination-driven self-assembly of imidazole-based ditopic donor 1,4-bis(imidazole-1-yl)benzene and 1,3-bis(imidazol-1-yl)benzene, with dinuclear half-sandwich p-cymene ruthenium(II) acceptors [Ru2(µ-η4-oxalato)(η6-p-cymene)2](SO3CF3)2, [Ru2(µ-η4-2,5-dioxido-1,4-benzoquinonato)(η6-p-cymene)2](SO3CF3)2 and [Ru2(µ-η4-5,8-dioxido-1,4-naphtoquinonato)(η6-p-cymene)2](SO3CF3)2, respectively. Likewise, three hexanuclear trigonal prismatic metallacages were prepared via the [2+3] self-assembly of tritopic donor of 1,3,5-tri(1H-imidazol-1-yl)benzene with these ruthenium(II) acceptors respectively. Self-selection of the single symmetrical and stable metallacycle and cage was observed although there is the possibility of forming different conformational isomeric products due to different binding modes of these imidazole-based donors. The self-assembled macrocycles and cage containing the 5,8-dioxido-1,4-naphtoquinonato (donq) spacer exhibited good anticancer activity on all tested cancer cell lines (HCT-116, MDA-MB-231, MCF-7, HeLa, A549, and HepG-2), and showed decreased cytotoxicities in HBE and THLE-2 normal cells. The effect of Ru and imidazole moiety of these assemblies on the anticancer activity was discussed. The study of binding ability of these donq-based Ru assemblies with ctDNA indicated that the complex 9 with 180° linear 1 ligand has the highest bonding constant Kb to ctDNA.
机译：通过基于咪唑的对位供体1,4-双（咪唑-1-基）苯和1,3-双（咪唑-1-基）的[2 + 2]配位驱动自组装合成了六个四核矩形金属环）苯，具有双核半夹心对式Cymene钌（II）受体[Ru2（µ-η 4 -oxalato）（η 6 -p-cymene）2] （SO3CF3）2，[Ru2（µ-η 4 -2,5-dioxido-1,4-benzoquinonato）（η 6 -p-cymene）2]（ SO3CF3）2和[Ru2（µ-η 4 -5,8-dioxido-1,4-naphtoquinonatoto）（η 6 -p-cymene）2]（SO3CF3 ）2。同样地，分别通过1,3,5-三（1H-咪唑-1-基）苯的三位供体的[2 + 3]自组装与这些钌（II）受体制备了三个六核三角棱柱金属绷带。尽管由于这些咪唑基供体的结合方式不同而可能形成不同的构象异构产物，但仍观察到了单个对称且稳定的金属环和笼的自我选择。含有5,8-dioxido-1,4-naphtoquinonato（donq）间隔子的自组装大环化合物和笼子对所有测试的癌细胞系（HCT-116，MDA-MB-231，MCF-7，HeLa ，A549和HepG-2），并在HBE和THLE-2正常细胞中显示出降低的细胞毒性。讨论了这些组件中Ru和咪唑部分对抗癌活性的影响。对这些基于donq的Ru组件与ctDNA的结合能力的研究表明，具有180°线性1配体的复合物9与ctDNA的结合常数Kb最高。

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