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Dual-Emissive Tris-Heteroleptic Ruthenium Complexes: Tuning the DNA-Triggered Ratiometric Emission Response by Ancillary Ligands
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2021-09-21 , DOI: 10.1021/acs.inorgchem.1c02077 Si-Hai Wu 1 , Rong Yang 1 , Bin Sun 2 , Jian-Hong Tang 3 , Zhong-Liang Gong 3 , Junjie Ma 1 , Lianhui Wang 1 , Jieqing Liu 1 , Dian-Xue Ma 3 , Jiang-Yang Shao 3 , Yu-Wu Zhong 3, 4
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2021-09-21 , DOI: 10.1021/acs.inorgchem.1c02077 Si-Hai Wu 1 , Rong Yang 1 , Bin Sun 2 , Jian-Hong Tang 3 , Zhong-Liang Gong 3 , Junjie Ma 1 , Lianhui Wang 1 , Jieqing Liu 1 , Dian-Xue Ma 3 , Jiang-Yang Shao 3 , Yu-Wu Zhong 3, 4
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Three tris-heteroleptic mononuclear Ru(II) complexes with dual fluorescence and phosphorescence—[Ru(dpma)(bpy)(phen)]2+ (12+), [Ru(dpma)(bpy)(dppz)]2+ (22+), and [Ru(dpma)(phen)(dppz)]2+ (32+)—have been designed and used as ratiometric light-response probes for DNA, where dpma is di(pyrid-2-yl)(methyl)-amine, bpy is 2,2′-bipyridine, phen is 1,10-phenanthroline, and dppz is dipyridophenazine, respectively. Single crystals of complex 2(PF6)2 have been obtained and studied by X-ray analysis. The interactions of these complexes with different DNAs are investigated by means of spectroscopic methods, viscosity measurements, and molecular modeling. In the presence of calf thymus DNA, complexes 2(PF6)2 and 3(PF6)2 show the emergence of a new lower-energy phosphorescence emission band; meanwhile, the higher-energy fluorescence emission band is essentially unchanged, functioning as an intrinsic internal reference. These two complexes exhibit stronger preference for calf thymus DNA over single-strand DNA (d(A)16 and d(C)16). In contrast, no binding interaction between 1(PF6)2 and calf thymus DNA is observed. The intrinsic binding constants (Kb) of 2(PF6)2 and 3(PF6)2 with calf thymus DNA are determined to be (1.4 ± 0.4) × 105 and (9.5 ± 0.15) × 104 M–1, respectively. In addition, these spectroscopic results are compared with those of the prototype complex [Ru(bpy)2(dppz)]2+ (42+), and density functional theory and time-dependent density functional theory calculations are employed to elucidate these experimental findings.
中文翻译：
双发射 Tris-杂配钌配合物：通过辅助配体调节 DNA 触发的比率发射响应
三种具有双重荧光和磷光的三杂配单核 Ru(II) 配合物——[Ru(dpma)(bpy)(phen)] 2+ ( 1 2+ ), [Ru(dpma)(bpy)(dppz)] 2+ ( 2 2+ ) 和 [Ru(dpma)(phen)(dppz)] 2+ ( 3 2+ )—已被设计并用作 DNA 的比率光响应探针，其中 dpma 是 di(pyrid-2- yl)(甲基)-胺，bpy是2,2'-联吡啶，phen是1,10-菲咯啉，dppz是双吡啶并吩嗪。配合物2 (PF 6 ) 2 的单晶已通过 X 射线分析获得和研究。通过光谱方法、粘度测量和分子建模研究了这些复合物与不同 DNA 的相互作用。在小牛胸腺 DNA 的存在下，复合物2 (PF 6 ) 2和3 (PF 6 ) 2显示出新的低能量磷光发射带的出现；同时，高能荧光发射带基本不变，起到内参的作用。这两种复合物对小牛胸腺 DNA 的偏好比单链 DNA 更强（d(A) 16和 d(C) 16）。相比之下，之间没有结合相互作用1 (PF 6 ) 2和小牛胸腺DNA被观察到。2 (PF 6 ) 2和3 (PF 6 ) 2与小牛胸腺 DNA的固有结合常数 ( K b )确定为 (1.4 ± 0.4) × 10 5和 (9.5 ± 0.15) × 10 4 M –1， 分别。此外，这些光谱结果与原型复合物 [Ru(bpy) 2 (dppz)] 2+ ( 4 2+)，并采用密度泛函理论和瞬态密度泛函理论计算来阐明这些实验结果。
更新日期：2021-10-04
中文翻译：
双发射 Tris-杂配钌配合物：通过辅助配体调节 DNA 触发的比率发射响应
三种具有双重荧光和磷光的三杂配单核 Ru(II) 配合物——[Ru(dpma)(bpy)(phen)] 2+ ( 1 2+ ), [Ru(dpma)(bpy)(dppz)] 2+ ( 2 2+ ) 和 [Ru(dpma)(phen)(dppz)] 2+ ( 3 2+ )—已被设计并用作 DNA 的比率光响应探针，其中 dpma 是 di(pyrid-2- yl)(甲基)-胺，bpy是2,2'-联吡啶，phen是1,10-菲咯啉，dppz是双吡啶并吩嗪。配合物2 (PF 6 ) 2 的单晶已通过 X 射线分析获得和研究。通过光谱方法、粘度测量和分子建模研究了这些复合物与不同 DNA 的相互作用。在小牛胸腺 DNA 的存在下，复合物2 (PF 6 ) 2和3 (PF 6 ) 2显示出新的低能量磷光发射带的出现；同时，高能荧光发射带基本不变，起到内参的作用。这两种复合物对小牛胸腺 DNA 的偏好比单链 DNA 更强（d(A) 16和 d(C) 16）。相比之下，之间没有结合相互作用1 (PF 6 ) 2和小牛胸腺DNA被观察到。2 (PF 6 ) 2和3 (PF 6 ) 2与小牛胸腺 DNA的固有结合常数 ( K b )确定为 (1.4 ± 0.4) × 10 5和 (9.5 ± 0.15) × 10 4 M –1， 分别。此外，这些光谱结果与原型复合物 [Ru(bpy) 2 (dppz)] 2+ ( 4 2+)，并采用密度泛函理论和瞬态密度泛函理论计算来阐明这些实验结果。
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