Characterization of copper complexes with derivatives of the ligand (2-aminoethyl)bis(2-pyridylmethyl)amine (uns-penp) and their reactivity towards oxygen
A series of copper(I) complexes with ligands derived from the tripodal ligand (2-aminoethyl)bis(2-pyridylmethyl)amine (uns-penp) have been structurally characterized and their redox chemistry analyzed by cyclic voltammetry. While the redox potentials of most of the complexes were similar their react...
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Published in | Journal of inorganic biochemistry Vol. 223; p. 111544 |
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Language | English |
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Abstract | A series of copper(I) complexes with ligands derived from the tripodal ligand (2-aminoethyl)bis(2-pyridylmethyl)amine (uns-penp) have been structurally characterized and their redox chemistry analyzed by cyclic voltammetry. While the redox potentials of most of the complexes were similar their reactivity towards dioxygen was quite different. While the complex with a ferrocene derived ligand of uns-penp reacted in solution at low temperatures in a two-step reaction from the preliminary formed mononuclear end-on superoxido complex to a quite stable dinuclear peroxido complex it did not react with dioxygen in the solid state. Other complexes also did not react with dioxygen in the solid state while some showed a reversible formation to a green compound, indicating formation of an end-on superoxido complex that unfortunately so far could not be characterized. In contrast, copper complexes with the Me2uns-penp and Et-iProp-uns-penp formed dinuclear peroxido complexes in a solid-state reaction. While the reaction of dioxygen with the [Cu(Me2uns-penp]BPh4 was quite slow an instant reaction took place for [Cu(Et-iProp-uns-penp]BPh. Very unusual, it turned out that crystals of the copper(I) complex that could be structurally characterized still were crystalline when reacted with dioxygen. Therefore, it was possible to solve the structure of the corresponding dinuclear peroxido complex directly from the same batch of crystals. The crystalline structures of the copper(I) and copper(II) complex revealed that the reason for this is the fact, that the copper(I) complex is kind of preorganized for the uptake of dioxygen and does not really change in its overall structure when being oxidized.
During a systematic study of the reactivity of a series of copper(I) complexes with tripodal ligands towards dioxygen a crystalline transformation of a copper(I) complex to the corresponding end-on peroxido complex was observed. [Display omitted]
•Detailed study on the reactivity of copper(I) complexes towards dioxygen.•Low temperature UV–vis studies to detect labile “dioxygen adduct” copper complexes.•Optimization of ligand system to obtain more stable peroxido copper complexes.•Solid state reactions of copper(I) complexes with dioxygen.•Molecular structure of an end-on copper peroxido complex. |
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AbstractList | A series of copper(I) complexes with ligands derived from the tripodal ligand (2-aminoethyl)bis(2-pyridylmethyl)amine (uns-penp) have been structurally characterized and their redox chemistry analyzed by cyclic voltammetry. While the redox potentials of most of the complexes were similar their reactivity towards dioxygen was quite different. While the complex with a ferrocene derived ligand of uns-penp reacted in solution at low temperatures in a two-step reaction from the preliminary formed mononuclear end-on superoxido complex to a quite stable dinuclear peroxido complex it did not react with dioxygen in the solid state. Other complexes also did not react with dioxygen in the solid state while some showed a reversible formation to a green compound, indicating formation of an end-on superoxido complex that unfortunately so far could not be characterized. In contrast, copper complexes with the Me2uns-penp and Et-iProp-uns-penp formed dinuclear peroxido complexes in a solid-state reaction. While the reaction of dioxygen with the [Cu(Me2uns-penp]BPh4 was quite slow an instant reaction took place for [Cu(Et-iProp-uns-penp]BPh. Very unusual, it turned out that crystals of the copper(I) complex that could be structurally characterized still were crystalline when reacted with dioxygen. Therefore, it was possible to solve the structure of the corresponding dinuclear peroxido complex directly from the same batch of crystals. The crystalline structures of the copper(I) and copper(II) complex revealed that the reason for this is the fact, that the copper(I) complex is kind of preorganized for the uptake of dioxygen and does not really change in its overall structure when being oxidized.
During a systematic study of the reactivity of a series of copper(I) complexes with tripodal ligands towards dioxygen a crystalline transformation of a copper(I) complex to the corresponding end-on peroxido complex was observed. [Display omitted]
•Detailed study on the reactivity of copper(I) complexes towards dioxygen.•Low temperature UV–vis studies to detect labile “dioxygen adduct” copper complexes.•Optimization of ligand system to obtain more stable peroxido copper complexes.•Solid state reactions of copper(I) complexes with dioxygen.•Molecular structure of an end-on copper peroxido complex. A series of copper(I) complexes with ligands derived from the tripodal ligand (2-aminoethyl)bis(2-pyridylmethyl)amine (uns-penp) have been structurally characterized and their redox chemistry analyzed by cyclic voltammetry. While the redox potentials of most of the complexes were similar their reactivity towards dioxygen was quite different. While the complex with a ferrocene derived ligand of uns-penp reacted in solution at low temperatures in a two-step reaction from the preliminary formed mononuclear end-on superoxido complex to a quite stable dinuclear peroxido complex it did not react with dioxygen in the solid state. Other complexes also did not react with dioxygen in the solid state while some showed a reversible formation to a green compound, indicating formation of an end-on superoxido complex that unfortunately so far could not be characterized. In contrast, copper complexes with the Me uns-penp and Et-iProp-uns-penp formed dinuclear peroxido complexes in a solid-state reaction. While the reaction of dioxygen with the [Cu(Me uns-penp]BPh was quite slow an instant reaction took place for [Cu(Et-iProp-uns-penp]BPh. Very unusual, it turned out that crystals of the copper(I) complex that could be structurally characterized still were crystalline when reacted with dioxygen. Therefore, it was possible to solve the structure of the corresponding dinuclear peroxido complex directly from the same batch of crystals. The crystalline structures of the copper(I) and copper(II) complex revealed that the reason for this is the fact, that the copper(I) complex is kind of preorganized for the uptake of dioxygen and does not really change in its overall structure when being oxidized. |
ArticleNumber | 111544 |
Author | Brückmann, Tim Heuler, Dominik Weiß, Morten Müller-Buschbaum, Klaus Becker, Jonathan Würtele, Christian Seuffert, Marcel Thomas Schindler, Siegfried |
Author_xml | – sequence: 1 givenname: Tim surname: Brückmann fullname: Brückmann, Tim organization: Institut für Anorganische und Analytische Chemie, Justus-Liebig-Universität, Heinrich-Buff-Ring 17, 35392 Gießen, Germany – sequence: 2 givenname: Jonathan surname: Becker fullname: Becker, Jonathan organization: Institut für Anorganische und Analytische Chemie, Justus-Liebig-Universität, Heinrich-Buff-Ring 17, 35392 Gießen, Germany – sequence: 3 givenname: Christian surname: Würtele fullname: Würtele, Christian organization: Institut für Anorganische und Analytische Chemie, Justus-Liebig-Universität, Heinrich-Buff-Ring 17, 35392 Gießen, Germany – sequence: 4 givenname: Marcel Thomas surname: Seuffert fullname: Seuffert, Marcel Thomas organization: Institut für Anorganische und Analytische Chemie, Justus-Liebig-Universität, Heinrich-Buff-Ring 17, 35392 Gießen, Germany – sequence: 5 givenname: Dominik surname: Heuler fullname: Heuler, Dominik organization: Institut für Anorganische und Analytische Chemie, Justus-Liebig-Universität, Heinrich-Buff-Ring 17, 35392 Gießen, Germany – sequence: 6 givenname: Klaus surname: Müller-Buschbaum fullname: Müller-Buschbaum, Klaus organization: Institut für Anorganische und Analytische Chemie, Justus-Liebig-Universität, Heinrich-Buff-Ring 17, 35392 Gießen, Germany – sequence: 7 givenname: Morten surname: Weiß fullname: Weiß, Morten organization: Fakultät für Biologie, Chemie und Geowissenschaften, Universität Bayreuth, Universitätsstrasse 30, 95447 Bayreuth, Germany – sequence: 8 givenname: Siegfried surname: Schindler fullname: Schindler, Siegfried email: siegfried.schindler@anorg.chemie.uni-giessen.de organization: Institut für Anorganische und Analytische Chemie, Justus-Liebig-Universität, Heinrich-Buff-Ring 17, 35392 Gießen, Germany |
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Keywords | Superoxido complex Peroxido complex Tripodal ligands Copper complex Dioxygen activation Stopped-flow |
Language | English |
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Snippet | A series of copper(I) complexes with ligands derived from the tripodal ligand (2-aminoethyl)bis(2-pyridylmethyl)amine (uns-penp) have been structurally... |
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SubjectTerms | Coordination Complexes - chemical synthesis Coordination Complexes - chemistry Copper - chemistry Copper complex Dioxygen activation Ligands Molecular Structure Oxidation-Reduction Oxygen - chemistry Peroxido complex Pyridines - chemical synthesis Pyridines - chemistry Stopped-flow Superoxido complex Tripodal ligands |
Title | Characterization of copper complexes with derivatives of the ligand (2-aminoethyl)bis(2-pyridylmethyl)amine (uns-penp) and their reactivity towards oxygen |
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