Modelling Binuclear Metallobiosites: Insights from Pyrazole‐Supported Biomimetic and Bioinspired Complexes

作者: Kristian E. Dalle , Franc Meyer

DOI: 10.1002/EJIC.201500185

关键词: Small moleculePyrazole ligandsCombinatorial chemistryPyrazoleStereochemistryChemistry

摘要: Numerous enzymes use two closely spaced metal ions to activate and transform small molecules. This allows these biocatalysts perform diverse physiological functions, achieving impressive chemistry under remarkably mild conditions. Model studies of metalloenzymes contribute furthering our understanding the unusual mechanistic aspects interplay cooperative effects used by Nature, help provide clues as how such reactivity might be harnessed for applications outside natural systems. microreview describes synthetic models binuclear metalloenzymes, focusing on complexes which are bridged pyrazole ligand scaffolds. Structural functional iron, nickel, copper zinc active sites discussed, in addition several cobalt possessing biologically relevant features. Metal separation secondary-coordination-sphere interactions recurring themes aid highlighting common importance native enzymes.

参考文章(127)
Edward I. Solomon, David E. Heppner, Esther M. Johnston, Jake W. Ginsbach, Jordi Cirera, Munzarin Qayyum, Matthew T. Kieber-Emmons, Christian H. Kjaergaard, Ryan G. Hadt, Li Tian, Copper Active Sites in Biology Chemical Reviews. ,vol. 114, pp. 3659- 3853 ,(2014) , 10.1021/CR400327T
Simone Wöckel, Joanna Galezowska, Sebastian Dechert, Franc Meyer, Binding of β-lactam antibiotics to a bioinspired dizinc complex reminiscent of the active site of metallo-β-lactamases. Inorganic Chemistry. ,vol. 51, pp. 2486- 2493 ,(2012) , 10.1021/IC202425M
Iryna A. Koval, Patrick Gamez, Catherine Belle, Katalin Selmeczi, Jan Reedijk, Synthetic models of the active site of catechol oxidase: mechanistic studies Chemical Society Reviews. ,vol. 35, pp. 814- 840 ,(2006) , 10.1039/B516250P
Lucie Ducháčková, Detlef Schröder, Jana Roithová, Effect of the carboxylate shift on the reactivity of zinc complexes in the gas phase. Inorganic Chemistry. ,vol. 50, pp. 3153- 3158 ,(2011) , 10.1021/IC2002767
Kristian E. Dalle, Tim Gruene, Sebastian Dechert, Serhiy Demeshko, Franc Meyer, Weakly Coupled Biologically Relevant CuII2(μ-η1:η1-O2) cis-Peroxo Adduct that Binds Side-On to Additional Metal Ions Journal of the American Chemical Society. ,vol. 136, pp. 7428- 7434 ,(2014) , 10.1021/JA5025047
Joseph W. Ziller, A. S. Borovik, Gary K.-Y. Ng, Structural diversity in metal complexes with a dinucleating ligand containing carboxyamidopyridyl groups. Inorganic Chemistry. ,vol. 50, pp. 7922- 7924 ,(2011) , 10.1021/IC200881T
Lina K. Blusch, Oliver Mitevski, Vlad Martin-Diaconescu, Kevin Pröpper, Serena DeBeer, Sebastian Dechert, Franc Meyer, Selective synthesis and redox sequence of a heterobimetallic nickel/copper complex of the noninnocent Siamese-twin porphyrin. Inorganic Chemistry. ,vol. 53, pp. 7876- 7885 ,(2014) , 10.1021/IC500460N
Anna L. Gavrilova, Brice Bosnich, Principles of Mononucleating and Binucleating Ligand Design Chemical Reviews. ,vol. 104, pp. 349- 384 ,(2004) , 10.1021/CR020604G
S. J. Lippard, W. B. Tolman, R. Lynn Rardin, Monodentate carboxylate complexes and the carboxylate shift : implications for polymetalloprotein structure and function New Journal of Chemistry. ,vol. 15, pp. 417- 430 ,(1991)