Phosphatase-like Activity of Tetranuclear Iron(III) and Zinc(II) Complexes

Publikationstyp:
Zeitschriftenaufsatz
Metadaten:
Autoren
  • Nityananda Dutta
  • Shobhraj Haldar
  • Gonela Vijaykumar
  • Suvendu Paul
  • Asoke Prasun Chattopadhyay
  • Luca Carrella
  • Manindranath Bera
Autoren-URL
https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=fis-test-1&SrcAuth=WosAPI&KeyUT=WOS:000443923700039&DestLinkType=FullRecord&DestApp=WOS_CPL
DOI
10.1021/acs.inorgchem.8b01441
eISSN
1520-510X
Externe Identifier
  • Clarivate Analytics Document Solution ID: GS7ZB
  • PubMed Identifier: 30130107
ISSN
0020-1669
Ausgabe der Veröffentlichung
17
Zeitschrift
INORGANIC CHEMISTRY
Paginierung
10802 - 10820
Datum der Veröffentlichung
2018
Status
Published
Titel
Phosphatase-like Activity of Tetranuclear Iron(III) and Zinc(II) Complexes
Sub types
  • Article
Ausgabe der Zeitschrift
57

Datenquelle: Web of Science (Lite)

Andere Metadatenquellen:
Autoren
  • Nityananda Dutta
  • Shobhraj Haldar
  • Gonela Vijaykumar
  • Suvendu Paul
  • Asoke Prasun Chattopadhyay
  • Luca Carrella
  • Manindranath Bera
DOI
10.1021/acs.inorgchem.8b01441
eISSN
1520-510X
ISSN
0020-1669
Ausgabe der Veröffentlichung
17
Zeitschrift
Inorganic Chemistry
Sprache
en
Online publication date
2018
Paginierung
10802 - 10820
Datum der Veröffentlichung
2018
Status
Published
Herausgeber
American Chemical Society (ACS)
Herausgeber URL
http://dx.doi.org/10.1021/acs.inorgchem.8b01441
Datum der Datenerfassung
2023
Titel
Phosphatase-like Activity of Tetranuclear Iron(III) and Zinc(II) Complexes
Ausgabe der Zeitschrift
57

Datenquelle: Crossref

Abstract
Three new tetranuclear iron(III) and zinc(II) complexes, [Fe<sub>4</sub>(cpdp)<sub>2</sub>(phth)<sub>2</sub>(OH)<sub>2</sub>]·8H<sub>2</sub>O (1), [Fe<sub>4</sub>(cpdp)<sub>2</sub>(terephth)<sub>2</sub>(OH)<sub>2</sub>] (2), and [Zn<sub>4</sub>(Hcpdp)<sub>2</sub>(suc)]Br<sub>2</sub>·12H<sub>2</sub>O (3), have been synthesized as models for the active site of phosphoester hydrolases by utilizing a polydentate ligand, N, N'-bis[2-carboxybenzomethyl]- N, N'-bis[2-pyridylmethyl]-1,3-diaminopropan-2-ol (H<sub>3</sub>cpdp) in combination with exogeneous phthalate (phth), terephthalate (terephth), and succinate (suc). Single crystal X-ray analyses reveal that the metallic core of complex 1 consists of four distorted octahedral iron(III) ions with average intraligand Fe---Fe separation of 3.656(2) Å, while the structure 3 represents a tetranuclear metallic core containing four distorted trigonal bipyramidal zinc(II) ions with average intraligand Zn---Zn separation of 3.472(2) Å. The molecular structure of complex 2 has been optimized by the DFT method which shows that its core arrangement is similar to that of 1. Complex 1 has a very interesting centrosymmetric structure that includes two crystallographically equivalent [Fe<sub>2</sub>(cpdp)]<sup>3+</sup> dinuclear units, connected together by a pair of syn-syn bridging phthalates and a pair of bridging hydroxides to generate a "dimer of dimers" structural motif. In complex 3, a succinate group connects two crystallographically equivalent [Zn<sub>2</sub>(Hcpdp)]<sup>2+</sup> dinuclear units in a syn-syn bidentate manner forming a "dimer of dimers" structural design. All three complexes show phosphatase-like activity that has been examined in methanol-water (1:1; v/v) using bis( p-nitrophenyl) phosphate (BNPP) as model substrate by applying the UV-vis spectrophotometric technique. In each case, the kinetic data have been analyzed by the Michaelis-Menten approach. The order of catalytic efficiency for the conversion of substrate to product follows the trend 1 > 2 > 3 with turnover rates ( k<sub>cat</sub>) of (2.73 ± 0.13) × 10<sup>-5</sup> for 1, (1.06 ± 0.07) × 10<sup>-5</sup> for 2, and (2.33 ± 0.18) × 10<sup>-6</sup> s<sup>-1</sup> for 3. These k<sub>cat</sub> values are comparable to, albeit slightly lower than, the values reported for similar iron(III)- and zinc(II)-based model complexes in the literature. DFT calculations have been carried out to support the proposed mechanism for phosphatase-like activity.
Addresses
  • Department of Chemistry , University of Kalyani , Kalyani , West Bengal - 741235 , India.
Autoren
  • Nityananda Dutta
  • Shobhraj Haldar
  • Gonela Vijaykumar
  • Suvendu Paul
  • Asoke Prasun Chattopadhyay
  • Luca Carrella
  • Manindranath Bera
DOI
10.1021/acs.inorgchem.8b01441
eISSN
1520-510X
Externe Identifier
  • PubMed Identifier: 30130107
Funding acknowledgements
  • Council of Scientific and Industrial Research: 01(2732)/13/EMR-II
  • University Grants Commission:
  • University of Kalyani:
Open access
false
ISSN
0020-1669
Ausgabe der Veröffentlichung
17
Zeitschrift
Inorganic chemistry
Schlüsselwörter
  • Iron
  • Zinc
  • Phosphoric Monoester Hydrolases
  • Solutions
  • Crystallography, X-Ray
  • Drug Stability
  • Catalytic Domain
  • Hydrogen-Ion Concentration
  • Quantum Theory
  • Models, Molecular
  • Mass Spectrometry
  • Coordination Complexes
Sprache
eng
Medium
Print-Electronic
Online publication date
2018
Paginierung
10802 - 10820
Datum der Veröffentlichung
2018
Status
Published
Datum der Datenerfassung
2018
Titel
Phosphatase-like Activity of Tetranuclear Iron(III) and Zinc(II) Complexes.
Sub types
  • Journal Article
Ausgabe der Zeitschrift
57

Datenquelle: Europe PubMed Central

Abstract
Three new tetranuclear iron(III) and zinc(II) complexes, [Fe4(cpdp)2(phth)2(OH)2]·8H2O (1), [Fe4(cpdp)2(terephth)2(OH)2] (2), and [Zn4(Hcpdp)2(suc)]Br2·12H2O (3), have been synthesized as models for the active site of phosphoester hydrolases by utilizing a polydentate ligand, N, N'-bis[2-carboxybenzomethyl]- N, N'-bis[2-pyridylmethyl]-1,3-diaminopropan-2-ol (H3cpdp) in combination with exogeneous phthalate (phth), terephthalate (terephth), and succinate (suc). Single crystal X-ray analyses reveal that the metallic core of complex 1 consists of four distorted octahedral iron(III) ions with average intraligand Fe---Fe separation of 3.656(2) Å, while the structure 3 represents a tetranuclear metallic core containing four distorted trigonal bipyramidal zinc(II) ions with average intraligand Zn---Zn separation of 3.472(2) Å. The molecular structure of complex 2 has been optimized by the DFT method which shows that its core arrangement is similar to that of 1. Complex 1 has a very interesting centrosymmetric structure that includes two crystallographically equivalent [Fe2(cpdp)]3+ dinuclear units, connected together by a pair of syn-syn bridging phthalates and a pair of bridging hydroxides to generate a "dimer of dimers" structural motif. In complex 3, a succinate group connects two crystallographically equivalent [Zn2(Hcpdp)]2+ dinuclear units in a syn-syn bidentate manner forming a "dimer of dimers" structural design. All three complexes show phosphatase-like activity that has been examined in methanol-water (1:1; v/v) using bis( p-nitrophenyl) phosphate (BNPP) as model substrate by applying the UV-vis spectrophotometric technique. In each case, the kinetic data have been analyzed by the Michaelis-Menten approach. The order of catalytic efficiency for the conversion of substrate to product follows the trend 1 > 2 > 3 with turnover rates ( kcat) of (2.73 ± 0.13) × 10-5 for 1, (1.06 ± 0.07) × 10-5 for 2, and (2.33 ± 0.18) × 10-6 s-1 for 3. These kcat values are comparable to, albeit slightly lower than, the values reported for similar iron(III)- and zinc(II)-based model complexes in the literature. DFT calculations have been carried out to support the proposed mechanism for phosphatase-like activity.
Autoren
  • Nityananda Dutta
  • Shobhraj Haldar
  • Gonela Vijaykumar
  • Suvendu Paul
  • Asoke Prasun Chattopadhyay
  • Luca Carrella
  • Manindranath Bera
Autoren-URL
https://www.ncbi.nlm.nih.gov/pubmed/30130107
DOI
10.1021/acs.inorgchem.8b01441
eISSN
1520-510X
Ausgabe der Veröffentlichung
17
Zeitschrift
Inorg Chem
Schlüsselwörter
  • Catalytic Domain
  • Coordination Complexes
  • Crystallography, X-Ray
  • Drug Stability
  • Hydrogen-Ion Concentration
  • Iron
  • Mass Spectrometry
  • Models, Molecular
  • Phosphoric Monoester Hydrolases
  • Quantum Theory
  • Solutions
  • Zinc
Sprache
eng
Country
United States
Paginierung
10802 - 10820
Datum der Veröffentlichung
2018
Status
Published
Datum, an dem der Datensatz öffentlich gemacht wurde
2018
Titel
Phosphatase-like Activity of Tetranuclear Iron(III) and Zinc(II) Complexes.
Sub types
  • Journal Article
Ausgabe der Zeitschrift
57

Datenquelle: PubMed

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