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Homodinuclear copper(II) and zinc(II) complexes of a carboxylate-rich ligand as synthetic mimics of phosphoester hydrolase in aqueous solutions
Journal of Inorganic Biochemistry ( IF 3.8 ) Pub Date : 2021-08-27 , DOI: 10.1016/j.jinorgbio.2021.111589
William Foley 1 , Hadi Arman 1 , Ghezai T Musie 1
Affiliation  

The synthesis, characterization and catalytic activities of two homodinuclear Cu(II) and Zn(II) complexes of a carboxylate-rich ligand, N,N′-Bis[2-carboxybenzomethyl]-N,N′ -Bis[carboxymethyl]-1,3-diaminopropan-2-ol (H5ccdp) ligand towards the hydrolysis of (p-nitrophenyl phosphate) (PNPP) and bis(p-nitrophenyl) phosphate (BNPP) substrates in aqueous systems are described. Kinetic investigations were carried out using UV–Vis spectrophotometric techniques at 25 °C and 37 °C and different pH (7–10) conditions. The kinetic studies revealed that the turnover rate (kcat) values among the PNPP hydrolysis systems, the highest and the lowest kcat values were displayed by [Cu2(ccdp)(μ-OAc)]2− at 2.34 × 10−6 s−1 (pH 8 and 37 °C) and 2.13 × 10−8 s−1 (pH 8 and 25 °C), respectively. However, similar comparisons among the BNPP hydrolysis revealed that highest and the lowest kcat values were displayed by [Zn2(ccdp)(μ-OAc)]2− at 4.64 × 10−8 s−1 (pH 9 and 37 °C) and 2.38 × 10−9 (pH 9 and 25 °C). Significantly enough, the catalyst−substrate adduct species containing a metal bound PNPP and BNPP have been detected by ESI-MS techniques. Additionally, a PNPP-bound copper complex has been isolated and crystalized using single crystal X-ray diffraction technique. Based on the structural and activity information obtained in this study, reaction mechanisms for the hydrolysis of PNPP have been proposed.



中文翻译:

富含羧酸盐的配体的同双核铜 (II) 和锌 (II) 配合物作为水溶液中磷酸酯水解酶的合成模拟物

富含羧酸盐的配体N,N' -Bis[2-carboxybenzomethyl]- N,N' -Bis[carboxymethyl]-1的两种同双核 Cu(II) 和 Zn(II) 配合物的合成、表征和催化活性描述了 ,3-diaminopropan-2-ol (H 5 ccdp) 配体在水性体系中对 ( p -nitrophenyl phosphate) (PNPP) 和( p - nitrophenyl) phosphate (BNPP) 底物的水解。在 25 °C 和 37 °C 和不同 pH (7-10) 条件下,使用 UV-Vis 分光光度计技术进行动力学研究。动力学研究表明,在 PNPP 水解系统中,周转率 ( k cat ) 值最高和最低k cat值由 [Cu 2 (ccdp)( μ -OAc)] 2-在 2.34 × 10 -6  s -1 (pH 8 和 37 °C) 和 2.13 × 10 -8  s -1 (pH 8 和25 °C),分别。然而,BNPP 水解之间的类似比较表明,在 4.64 × 10 -8  s -1(pH 9 和 37 °C )下,[Zn 2 (ccdp)( μ -OAc)] 2-显示出最高和最低的k cat值) 和 2.38 × 10 -9(pH 9 和 25 °C)。值得注意的是,ESI-MS 技术已检测到含有金属结合的 PNPP 和 BNPP 的催化剂-底物加合物物质。此外,已使用单晶 X 射线衍射技术分离并结晶了 PNPP 结合的铜络合物。根据本研究中获得的结构和活性信息,提出了 PNPP 水解的反应机理。

更新日期:2021-09-13
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