Ci-Symmetry, [2 × 2] grid, square copper complex with the N4,N5-bis(4-fluorophenyl)-1H-imidazole-4,5-dicarboxamide ligand: structure, catecholase activity, magnetic properties and DFT calculations

A new square tetranuclear copper complex of formula Cu4(LH)4·4DMF with the dinucleating amide ligand N4,N5-bis(4-fluorophenyl)-1H-imidazole-4,5-dicarboxamide (LH3) is reported herein. This ligand and the complex have been characterized by elemental analysis, FTIR, NMR, mass and UV-visible spectrosco...

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Main Authors: Parween, Arfa, Naskar, Sumita, Mota, Antonio J., Espinosa Ferao, Arturo, Chattopadhyay, Shyamal Kumar, Rivière, Eric, Lewis, William, Naskar, Subhendu
Format: Article
Published: Royal Society of Chemistry 2017
Online Access:https://eprints.nottingham.ac.uk/46516/
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author Parween, Arfa
Naskar, Sumita
Mota, Antonio J.
Espinosa Ferao, Arturo
Chattopadhyay, Shyamal Kumar
Rivière, Eric
Lewis, William
Naskar, Subhendu
author_facet Parween, Arfa
Naskar, Sumita
Mota, Antonio J.
Espinosa Ferao, Arturo
Chattopadhyay, Shyamal Kumar
Rivière, Eric
Lewis, William
Naskar, Subhendu
author_sort Parween, Arfa
building Nottingham Research Data Repository
collection Online Access
description A new square tetranuclear copper complex of formula Cu4(LH)4·4DMF with the dinucleating amide ligand N4,N5-bis(4-fluorophenyl)-1H-imidazole-4,5-dicarboxamide (LH3) is reported herein. This ligand and the complex have been characterized by elemental analysis, FTIR, NMR, mass and UV-visible spectroscopy, as well as magnetic and electrochemical measurements. The single crystal X-ray diffraction study showed each Cu centre in a distorted square pyramidal environment, the square plane being formed by the extended coordination of two sets (N,N and N,O) of donor atoms from pairs of different ligands. The Cu4 unit has a Ci symmetry and crystallises in the P[1 with combining macron] space group in between DMF layers. The electronic spectrum of the complex exhibits a d–d transition at 676 nm. The complex also displays mild catecholase activity in DMF solution by using 3,5-di-tert-butylcatechol as substrate. Variable temperature magnetic measurements reveal an antiferromagnetic interaction between the copper centres with two different coupling constants of −143.4 and −169.0 cm−1. DFT calculations made on a single Cu4 unit from the crystal structure corroborated the antiferromagnetic coupling, the spin density of the lower-energy broken-symmetry state being consistent with an alternating +−+− singlet state operating at low temperature.
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spelling nottingham-465162020-05-04T19:13:12Z https://eprints.nottingham.ac.uk/46516/ Ci-Symmetry, [2 × 2] grid, square copper complex with the N4,N5-bis(4-fluorophenyl)-1H-imidazole-4,5-dicarboxamide ligand: structure, catecholase activity, magnetic properties and DFT calculations Parween, Arfa Naskar, Sumita Mota, Antonio J. Espinosa Ferao, Arturo Chattopadhyay, Shyamal Kumar Rivière, Eric Lewis, William Naskar, Subhendu A new square tetranuclear copper complex of formula Cu4(LH)4·4DMF with the dinucleating amide ligand N4,N5-bis(4-fluorophenyl)-1H-imidazole-4,5-dicarboxamide (LH3) is reported herein. This ligand and the complex have been characterized by elemental analysis, FTIR, NMR, mass and UV-visible spectroscopy, as well as magnetic and electrochemical measurements. The single crystal X-ray diffraction study showed each Cu centre in a distorted square pyramidal environment, the square plane being formed by the extended coordination of two sets (N,N and N,O) of donor atoms from pairs of different ligands. The Cu4 unit has a Ci symmetry and crystallises in the P[1 with combining macron] space group in between DMF layers. The electronic spectrum of the complex exhibits a d–d transition at 676 nm. The complex also displays mild catecholase activity in DMF solution by using 3,5-di-tert-butylcatechol as substrate. Variable temperature magnetic measurements reveal an antiferromagnetic interaction between the copper centres with two different coupling constants of −143.4 and −169.0 cm−1. DFT calculations made on a single Cu4 unit from the crystal structure corroborated the antiferromagnetic coupling, the spin density of the lower-energy broken-symmetry state being consistent with an alternating +−+− singlet state operating at low temperature. Royal Society of Chemistry 2017-10-21 Article PeerReviewed Parween, Arfa, Naskar, Sumita, Mota, Antonio J., Espinosa Ferao, Arturo, Chattopadhyay, Shyamal Kumar, Rivière, Eric, Lewis, William and Naskar, Subhendu (2017) Ci-Symmetry, [2 × 2] grid, square copper complex with the N4,N5-bis(4-fluorophenyl)-1H-imidazole-4,5-dicarboxamide ligand: structure, catecholase activity, magnetic properties and DFT calculations. New Journal of Chemistry, 41 (20). pp. 11750-11758. ISSN 1369-9261 http://pubs.rsc.org/en/Content/ArticleLanding/2017/NJ/C7NJ01667K#!divAbstract doi:10.1039/C7NJ01667K doi:10.1039/C7NJ01667K
spellingShingle Parween, Arfa
Naskar, Sumita
Mota, Antonio J.
Espinosa Ferao, Arturo
Chattopadhyay, Shyamal Kumar
Rivière, Eric
Lewis, William
Naskar, Subhendu
Ci-Symmetry, [2 × 2] grid, square copper complex with the N4,N5-bis(4-fluorophenyl)-1H-imidazole-4,5-dicarboxamide ligand: structure, catecholase activity, magnetic properties and DFT calculations
title Ci-Symmetry, [2 × 2] grid, square copper complex with the N4,N5-bis(4-fluorophenyl)-1H-imidazole-4,5-dicarboxamide ligand: structure, catecholase activity, magnetic properties and DFT calculations
title_full Ci-Symmetry, [2 × 2] grid, square copper complex with the N4,N5-bis(4-fluorophenyl)-1H-imidazole-4,5-dicarboxamide ligand: structure, catecholase activity, magnetic properties and DFT calculations
title_fullStr Ci-Symmetry, [2 × 2] grid, square copper complex with the N4,N5-bis(4-fluorophenyl)-1H-imidazole-4,5-dicarboxamide ligand: structure, catecholase activity, magnetic properties and DFT calculations
title_full_unstemmed Ci-Symmetry, [2 × 2] grid, square copper complex with the N4,N5-bis(4-fluorophenyl)-1H-imidazole-4,5-dicarboxamide ligand: structure, catecholase activity, magnetic properties and DFT calculations
title_short Ci-Symmetry, [2 × 2] grid, square copper complex with the N4,N5-bis(4-fluorophenyl)-1H-imidazole-4,5-dicarboxamide ligand: structure, catecholase activity, magnetic properties and DFT calculations
title_sort ci-symmetry, [2 × 2] grid, square copper complex with the n4,n5-bis(4-fluorophenyl)-1h-imidazole-4,5-dicarboxamide ligand: structure, catecholase activity, magnetic properties and dft calculations
url https://eprints.nottingham.ac.uk/46516/
https://eprints.nottingham.ac.uk/46516/
https://eprints.nottingham.ac.uk/46516/