Multivalent Metallosupramolecular Assemblies as Effective DNA Binding Agents

被引:35
作者
Drozdz, Wojciech [1 ,2 ]
Walczak, Anna [1 ,2 ]
Bessin, Yannick [3 ]
Gervais, Virginie [4 ]
Cao, Xiao-Yu [5 ]
Lehn, Jean-Marie [5 ]
Ulrich, Sebastien [3 ]
Stefankiewicz, Artur R. [1 ,2 ]
机构
[1] Adam Mickiewicz Univ, Fac Chem, Umultowska 89b, PL-61614 Poznan, Poland
[2] Adam Mickiewicz Univ, Ctr Adv Technol, Umultowska 89c, PL-61614 Poznan, Poland
[3] Univ Montpellier, CNRS, IBMM, UMR 5247,ENSCM, Montpellier, France
[4] Univ Toulouse, UPS, CNRS, IPBS, 205 Route Narbonne, F-31077 Toulouse, France
[5] Univ Strasbourg, CNRS, ISIS, Lab Chim Supramol,UMR 7006, 8 Allee Gaspard Monge, F-67000 Strasbourg, France
关键词
coordination chemistry; DNA recognition; multivalency; self-assembly; zinc; ARCHITECTURES; LIGAND; RECOGNITION; COMPLEXES; LESSONS; HIV;
D O I
10.1002/chem.201801552
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
We report the implementation of coordination chemistry onto the generation of new types of metallosupramolecular complexes with laterally appended cationic moieties for DNA binding in buffered aqueous media. Utilization of an N,N,O-type coordination pocket along with an octahedral zinc(II) metal ion allowed us to obtain mono- and tetranuclear complexes in both solution and solid state, as confirmed by NMR spectroscopy and single-crystal X-ray diffraction, respectively. By using isothermal titration calorimetry and gel electrophoresis, multiply charged cationic assemblies were observed to effectively bind to DNA through multivalent electrostatic interactions. Furthermore, we observed a correlation between the multivalency of the compounds employed and the effectiveness of DNA binding.
引用
收藏
页码:10802 / 10811
页数:10
相关论文
共 55 条
[1]   Let's twist again - Double-stranded, triple-stranded, and circular helicates [J].
Albrecht, M .
CHEMICAL REVIEWS, 2001, 101 (11) :3457-3497
[2]  
[Anonymous], ANGEW CHEM
[3]  
[Anonymous], 2012, ANGEW CHEM
[4]  
[Anonymous], 2012, ANGEW CHEM, DOI DOI 10.1002/ANGE.201201114
[5]   Self-Assembled Multivalency: Dynamic Ligand Arrays for High-Affinity Binding [J].
Barnard, Anna ;
Smith, David K. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2012, 51 (27) :6572-6581
[6]  
Bartolami E, 2015, ANGEW CHEM, V127, P10321
[7]   Bioactive clusters promoting cell penetration and nucleic acid complexation for drug and gene delivery applications: from designed to self-assembled and responsive systems [J].
Bartolami, Eline ;
Bouillon, Camille ;
Dumy, Pascal ;
Ulrich, Sebastien .
CHEMICAL COMMUNICATIONS, 2016, 52 (23) :4257-4273
[8]   Multivalent DNA recognition by self-assembled clusters: deciphering structural effects by fragments screening and evaluation as siRNA vectors [J].
Bartolami, Eline ;
Bessin, Yannick ;
Bettache, Nadir ;
Gary-Bobo, Magali ;
Garcia, Marcel ;
Dumy, Pascal ;
Ulrich, Sebastien .
ORGANIC & BIOMOLECULAR CHEMISTRY, 2015, 13 (36) :9427-9438
[9]   Dynamic Expression of DNA Complexation with Self-assembled Biomolecular Clusters [J].
Bartolami, Eline ;
Bessin, Yannick ;
Gervais, Virginie ;
Dumy, Pascal ;
Ulrich, Sebastien .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2015, 54 (35) :10183-10187
[10]   Rotaxanes as new architectures for photoinduced electron transfer and molecular motions [J].
Blanco, MJ ;
Jiménez, MC ;
Chambron, JC ;
Heitz, V ;
Linke, M ;
Sauvage, JP .
CHEMICAL SOCIETY REVIEWS, 1999, 28 (05) :293-305