Literature DB >> 34714402

Mono- and dinuclear zinc complexes bearing identical bis(thiosemicarbazone) ligand that exhibit alkaline phosphatase-like catalytic reactivity.

Hyeri Jeon1, Hugo Vazquez-Lima2,3, Haewon Jeong1, Kyung-Bin Cho4, Seungwoo Hong5.   

Abstract

Mono- and dinuclear zinc(II) complexes bearing bis(thiosemicarbazone) (bTSC) ligand were employed in the cleavage of phosphoester bonds. Comparative kinetic studies combined with theory suggested that the P-O bond cleavage is much accelerated by dinuclear zinc(II) complex in the presence of base. Based on the DFT-optimized structures of the proposed intermediates, it is plausible that (1) the removal of sulfur atoms of bTSC ligand from the zinc center provides two vacant sites for the binding of water (or hydroxide ion) and phosphoester and (2) the H-bonding between water (or hydroxide ion) and phosphoester, through several water molecules, may also assist the P-O bond cleavage and facilitate the nucleophilic attack. The kinetic and catalytic studies on the hydrolysis of phosphoester by dinuclear zinc complex showed a much-enhanced reactivity under basic reaction conditions, reaching over 95% conversion yield within 4 h. The currently presented compounds are arguably one of the faster synthetic Zn-based model performing phosphatase-like activity presented so far.
© 2021. The Author(s), under exclusive licence to Society for Biological Inorganic Chemistry (SBIC).

Entities:  

Keywords:  Computational chemistry; Density functional theory; Enzyme kinetics; Hydrolysis; Model compound

Mesh:

Substances:

Year:  2021        PMID: 34714402     DOI: 10.1007/s00775-021-01909-0

Source DB:  PubMed          Journal:  J Biol Inorg Chem        ISSN: 0949-8257            Impact factor:   3.358


  31 in total

Review 1.  Protein phosphorylation and signal transduction.

Authors:  J D Graves; E G Krebs
Journal:  Pharmacol Ther       Date:  1999 May-Jun       Impact factor: 12.310

2.  DNA-bound structures and mutants reveal abasic DNA binding by APE1 and DNA repair coordination [corrected].

Authors:  C D Mol; T Izumi; S Mitra; J A Tainer
Journal:  Nature       Date:  2000-01-27       Impact factor: 49.962

3.  Recent Advances in Zinc Enzymology.

Authors:  William N. Lipscomb; Norbert Sträter
Journal:  Chem Rev       Date:  1996-11-07       Impact factor: 60.622

4.  Kinetics and Mechanisms for the Cleavage and Isomerization of the Phosphodiester Bonds of RNA by Brønsted Acids and Bases.

Authors:  Mikko Oivanen; Satu Kuusela; Harri Lönnberg
Journal:  Chem Rev       Date:  1998-05-07       Impact factor: 60.622

Review 5.  Mode of action of bi- and trinuclear zinc hydrolases and their synthetic analogues.

Authors:  Jennie Weston
Journal:  Chem Rev       Date:  2005-06       Impact factor: 60.622

Review 6.  Enzymatic mechanisms of phosphate and sulfate transfer.

Authors:  W Wallace Cleland; Alvan C Hengge
Journal:  Chem Rev       Date:  2006-08       Impact factor: 60.622

7.  Unsymmetrical dizinc complexes as models for the active sites of phosphohydrolases.

Authors:  Martin Jarenmark; Edit Csapó; Jyoti Singh; Simone Wöckel; Etelka Farkas; Franc Meyer; Matti Haukka; Ebbe Nordlander
Journal:  Dalton Trans       Date:  2010-08-04       Impact factor: 4.390

Review 8.  Dimetallic hydrolases and their models.

Authors:  E Kimura
Journal:  Curr Opin Chem Biol       Date:  2000-04       Impact factor: 8.822

Review 9.  Proteomic analysis of phosphorylation, oxidation and nitrosylation in signal transduction.

Authors:  Corinne M Spickett; Andrew R Pitt; Nicholas Morrice; Walter Kolch
Journal:  Biochim Biophys Acta       Date:  2006-09-29

10.  DNA-catalyzed sequence-specific hydrolysis of DNA.

Authors:  Madhavaiah Chandra; Amit Sachdeva; Scott K Silverman
Journal:  Nat Chem Biol       Date:  2009-08-16       Impact factor: 15.040

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