Cadmium(II) complexes of the glycerophosphodiester-degrading enzyme GpdQ and a biomimetic N,O ligand
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Mirams, Ruth E; Smith, Sarah J; Hadler, Kieran S; Ollis, David; Schenk, Gerhard; Gahan, Lawrence
Description
The glycerophosphodiester-degrading enzyme GpdQ from Enterobacter aerogenes is a promising bioremediator owing to its ability to degrade some organophosphate pesticides and diester products originating from the hydrolysis of nerve agents such as VX. Here, the cadmium derivative of GpdQ was prepared by reconstituting the apoenzyme. Catalytic measurements with (Cd2+)2-GpdQ and the phosphodiester substrate bis(4-nitrophenyl)phosphate yield kcat = 15 s-1. The pKa of 9.4, determined from the pH...[Show more]
dc.contributor.author | Mirams, Ruth E | |
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dc.contributor.author | Smith, Sarah J | |
dc.contributor.author | Hadler, Kieran S | |
dc.contributor.author | Ollis, David | |
dc.contributor.author | Schenk, Gerhard | |
dc.contributor.author | Gahan, Lawrence | |
dc.date.accessioned | 2015-12-10T22:21:48Z | |
dc.identifier.issn | 0949-8257 | |
dc.identifier.uri | http://hdl.handle.net/1885/52366 | |
dc.description.abstract | The glycerophosphodiester-degrading enzyme GpdQ from Enterobacter aerogenes is a promising bioremediator owing to its ability to degrade some organophosphate pesticides and diester products originating from the hydrolysis of nerve agents such as VX. Here, the cadmium derivative of GpdQ was prepared by reconstituting the apoenzyme. Catalytic measurements with (Cd2+)2-GpdQ and the phosphodiester substrate bis(4-nitrophenyl)phosphate yield kcat = 15 s-1. The pKa of 9.4, determined from the pH dependence of the catalytic activity, implicates a hydroxide ligand as the catalytic nucleophile. Also prepared was the cadmium-containing biomimetic [Cd2((HP)2B)(OAc)2(OH2)](PF6) (where (HP)2B is [2,6-bis([(2-pyridylmethyl)(2-hydroxyethyl)amino]methyl)-4- methylphenol]), which mimics the asymmetry of the metal ion coordination in the active site of GpdQ. The phosphoesterase-like activity of [Cd2((HP)2B)(OAc)2(OH2)](PF6) was studied using the substrate bis(2,4-dinitrophenyl)phosphate, yielding a kinetically relevant pKa of 8.9, with kcat = 0.004 s-1. In summary, the model is both an adequate structural and a reasonable functional mimic of GpdQ. | |
dc.publisher | Springer | |
dc.source | Journal of Biological Inorganic Chemistry | |
dc.subject | Keywords: [2,6 bis[[(2 pyridylmethyl)(2 hydroxyethyl)amino]methyl] 4 methylphenol]; apoenzyme; biomimetic material; bis(4 nitrophenyl) phosphate; cadmium; cadmium derivative; GpdQ enzyme; hydroxide; ligand; phosphodiesterase; unclassified drug; article; biomimetics Binuclear metallohydrolases; Biomimetics; Bioremediation; Cadmium complexes; Glycerophosphodiester-degrading enzyme | |
dc.title | Cadmium(II) complexes of the glycerophosphodiester-degrading enzyme GpdQ and a biomimetic N,O ligand | |
dc.type | Journal article | |
local.description.notes | Imported from ARIES | |
local.identifier.citationvolume | 13 | |
dc.date.issued | 2008 | |
local.identifier.absfor | 030403 - Characterisation of Biological Macromolecules | |
local.identifier.ariespublication | u4005981xPUB245 | |
local.type.status | Published Version | |
local.contributor.affiliation | Mirams, Ruth E, University of Queensland | |
local.contributor.affiliation | Smith, Sarah J, University of Queensland | |
local.contributor.affiliation | Hadler, Kieran S, University of Queensland | |
local.contributor.affiliation | Ollis, David, College of Physical and Mathematical Sciences, ANU | |
local.contributor.affiliation | Schenk, Gerhard, University of Queensland | |
local.contributor.affiliation | Gahan, Lawrence, University of Queensland | |
local.description.embargo | 2037-12-31 | |
local.bibliographicCitation.issue | 7 | |
local.bibliographicCitation.startpage | 1065 | |
local.bibliographicCitation.lastpage | 1072 | |
local.identifier.doi | 10.1007/s00775-008-0392-5 | |
dc.date.updated | 2015-12-09T08:57:43Z | |
local.identifier.scopusID | 2-s2.0-51849163244 | |
local.identifier.thomsonID | 000259248900003 | |
Collections | ANU Research Publications |
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