Versatile coordination behaviour of the chloro-tetrazine-picolylamine ligand: mixed-valence binuclear Cu()/Cu() complexes
The 3-Cl-6-amino-(2′-picolyl)-1,2,4,5-tetrazine ligand HL 1 has been synthesized and structurally characterized. Its versatile coordination behavior has been evidenced through reactions with Cu(Hfac) 2 and Cu(triflate) 2 precursors, which provided mixed-valence bimetallic Cu 1.5 Cu 1.5 complexes [Cu...
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| Published in | Dalton transactions : an international journal of inorganic chemistry Vol. 48; no. 31; pp. 11966 - 11977 |
|---|---|
| Main Authors | , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
England
Royal Society of Chemistry
06.08.2019
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| Subjects | |
| Online Access | Get full text |
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| Abstract | The 3-Cl-6-amino-(2′-picolyl)-1,2,4,5-tetrazine ligand
HL
1
has been synthesized and structurally characterized. Its versatile coordination behavior has been evidenced through reactions with Cu(Hfac)
2
and Cu(triflate)
2
precursors, which provided mixed-valence bimetallic Cu
1.5
Cu
1.5
complexes [Cu
2
(μ-Cl)(
L
1
)
2
]
2
and [Cu
2
(μ-triflate)(
L
1
)
2
]
5
. Changing the Cu(
ii
) precursor and the solvent leads to the formation of mononuclear octahedral Cu(
ii
) complexes [CuCl
2
(
HL
1
)
2
]·2CH
3
CN
3
and [Cu(Hfac)
2
(
HL
1
)]
4
, in which only the amino-pyridine unit is involved in the coordination of the metal center. In contrast, in complexes
2
and
5
, the ligands are deprotonated and bridge the metal centers as pyridine-amido-tetrazine fragments, while a bridging chloride or triflate ligand completes the coordination sphere of the metal ions. The Cu-Cu distances of 2.4313(4) Å in
2
and 2.5198(10) Å in
5
lie among the shorter values within mixed-valence bimetallic Cu complexes. Mixed-valence character is strongly supported by DFT calculations, showing the equal repartition of the unpaired electron between the two metal centers.
Neutral mixed-valence binuclear Cu(
i
)/Cu(
ii
) complexes, containing the deprotonated chloro-picolylamine-tetrazine ligand, have been prepared and characterized by single crystal X-ray diffraction and DFT calculations. |
|---|---|
| AbstractList | The 3-Cl-6-amino-(2′-picolyl)-1,2,4,5-tetrazine ligand
HL
1
has been synthesized and structurally characterized. Its versatile coordination behavior has been evidenced through reactions with Cu(Hfac)
2
and Cu(triflate)
2
precursors, which provided mixed-valence bimetallic Cu
1.5
Cu
1.5
complexes [Cu
2
(μ-Cl)(
L
1
)
2
]
2
and [Cu
2
(μ-triflate)(
L
1
)
2
]
5
. Changing the Cu(
ii
) precursor and the solvent leads to the formation of mononuclear octahedral Cu(
ii
) complexes [CuCl
2
(
HL
1
)
2
]·2CH
3
CN
3
and [Cu(Hfac)
2
(
HL
1
)]
4
, in which only the amino-pyridine unit is involved in the coordination of the metal center. In contrast, in complexes
2
and
5
, the ligands are deprotonated and bridge the metal centers as pyridine-amido-tetrazine fragments, while a bridging chloride or triflate ligand completes the coordination sphere of the metal ions. The Cu-Cu distances of 2.4313(4) Å in
2
and 2.5198(10) Å in
5
lie among the shorter values within mixed-valence bimetallic Cu complexes. Mixed-valence character is strongly supported by DFT calculations, showing the equal repartition of the unpaired electron between the two metal centers.
Neutral mixed-valence binuclear Cu(
i
)/Cu(
ii
) complexes, containing the deprotonated chloro-picolylamine-tetrazine ligand, have been prepared and characterized by single crystal X-ray diffraction and DFT calculations. The 3-Cl-6-amino-(2′-picolyl)-1,2,4,5-tetrazine ligand HL1 has been synthesized and structurally characterized. Its versatile coordination behavior has been evidenced through reactions with Cu(Hfac)2 and Cu(triflate)2 precursors, which provided mixed-valence bimetallic Cu1.5Cu1.5 complexes [Cu2(μ-Cl)(L1)2] 2 and [Cu2(μ-triflate)(L1)2] 5. Changing the Cu(II) precursor and the solvent leads to the formation of mononuclear octahedral Cu(II) complexes [CuCl2(HL1)2]·2CH3CN 3 and [Cu(Hfac)2(HL1)] 4, in which only the amino-pyridine unit is involved in the coordination of the metal center. In contrast, in complexes 2 and 5, the ligands are deprotonated and bridge the metal centers as pyridine-amido-tetrazine fragments, while a bridging chloride or triflate ligand completes the coordination sphere of the metal ions. The Cu–Cu distances of 2.4313(4) Å in 2 and 2.5198(10) Å in 5 lie among the shorter values within mixed-valence bimetallic Cu complexes. Mixed-valence character is strongly supported by DFT calculations, showing the equal repartition of the unpaired electron between the two metal centers. The 3-Cl-6-amino-(2′-picolyl)-1,2,4,5-tetrazine ligand HL1 has been synthesized and structurally characterized. Its versatile coordination behavior has been evidenced through reactions with Cu(Hfac) 2 and Cu(triflate) 2 precursors, which provided mixed-valence bimetallic Cu 1.5 Cu 1.5 complexes [Cu 2 (μ-Cl)( L1 ) 2 ] 2 and [Cu 2 (μ-triflate)( L1 ) 2 ] 5 . Changing the Cu( ii ) precursor and the solvent leads to the formation of mononuclear octahedral Cu( ii ) complexes [CuCl 2 ( HL1 ) 2 ]·2CH 3 CN 3 and [Cu(Hfac) 2 ( HL1 )] 4 , in which only the amino-pyridine unit is involved in the coordination of the metal center. In contrast, in complexes 2 and 5 , the ligands are deprotonated and bridge the metal centers as pyridine-amido-tetrazine fragments, while a bridging chloride or triflate ligand completes the coordination sphere of the metal ions. The Cu–Cu distances of 2.4313(4) Å in 2 and 2.5198(10) Å in 5 lie among the shorter values within mixed-valence bimetallic Cu complexes. Mixed-valence character is strongly supported by DFT calculations, showing the equal repartition of the unpaired electron between the two metal centers. |
| Author | El-Ghayoury, Abdelkrim Avarvari, Narcis Attia, Amr A. A Kokozay, Vladimir N Petrusenko, Svitlana R Lupan, Alexandru Stetsiuk, Oleh Sorace, Lorenzo |
| AuthorAffiliation | CNRS Department of Inorganic Chemistry Taras Shevchenko National University of Kyiv Dipartimento di Chimica "Ugo Schiff" and UdR INSTM Faculty of Chemistry and Chemical Engineering Università di Firenze MOLTECH-Anjou Babes-Bolyai University UMR 6200 UNIV Angers |
| AuthorAffiliation_xml | – name: Dipartimento di Chimica "Ugo Schiff" and UdR INSTM – name: Babes-Bolyai University – name: Università di Firenze – name: UNIV Angers – name: Department of Inorganic Chemistry – name: CNRS – name: MOLTECH-Anjou – name: UMR 6200 – name: Taras Shevchenko National University of Kyiv – name: Faculty of Chemistry and Chemical Engineering |
| Author_xml | – sequence: 1 givenname: Oleh surname: Stetsiuk fullname: Stetsiuk, Oleh – sequence: 2 givenname: Svitlana R surname: Petrusenko fullname: Petrusenko, Svitlana R – sequence: 3 givenname: Lorenzo surname: Sorace fullname: Sorace, Lorenzo – sequence: 4 givenname: Alexandru surname: Lupan fullname: Lupan, Alexandru – sequence: 5 givenname: Amr A. A surname: Attia fullname: Attia, Amr A. A – sequence: 6 givenname: Vladimir N surname: Kokozay fullname: Kokozay, Vladimir N – sequence: 7 givenname: Abdelkrim surname: El-Ghayoury fullname: El-Ghayoury, Abdelkrim – sequence: 8 givenname: Narcis surname: Avarvari fullname: Avarvari, Narcis |
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| Copyright | Copyright Royal Society of Chemistry 2019 Distributed under a Creative Commons Attribution 4.0 International License |
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| Notes | Electronic supplementary information (ESI) available: Full experimental section including description of the synthesis and characterization of all new materials and all the techniques employed in the research reported herein. CCDC 1850384-1850388 For ESI and crystallographic data in CIF or other electronic format see DOI 10.1039/c9dt02379h ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
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| Snippet | The 3-Cl-6-amino-(2′-picolyl)-1,2,4,5-tetrazine ligand
HL
1
has been synthesized and structurally characterized. Its versatile coordination behavior has been... The 3-Cl-6-amino-(2'-picolyl)-1,2,4,5-tetrazine ligand HL1 has been synthesized and structurally characterized. Its versatile coordination behavior has been... The 3-Cl-6-amino-(2′-picolyl)-1,2,4,5-tetrazine ligand HL1 has been synthesized and structurally characterized. Its versatile coordination behavior has been... The 3-Cl-6-amino-(2′-picolyl)-1,2,4,5-tetrazine ligand HL1 has been synthesized and structurally characterized. Its versatile coordination behavior has been... |
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| SubjectTerms | Bimetals Chemical Sciences Coordination Coordination chemistry Copper Crystallography Ligands Precursors |
| Title | Versatile coordination behaviour of the chloro-tetrazine-picolylamine ligand: mixed-valence binuclear Cu()/Cu() complexes |
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