Volume 2016, Issue 10 p. 1604-1618

Full Paper

Synthesis, Theoretical Study and Catalytic Application of Oxidometal (Mo or V) Complexes: Unexpected Coordination Due to Ligand Rearrangement through Metal-Mediated C–C Bond Formation^†

Sagarika Pasayat

Department of Chemistry, National Institute of Technology, Rourkela 769008 Odisha, India, http://https://sites.google.com/site/drrupamdinda/

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Michael Böhme,

Michael Böhme

Institute of Inorganic and Analytical Chemistry, Chair of Inorganic Chemistry II, Friedrich Schiller University Jena, Humboldtstr. 8, 07743 Jena, Germany, http://www.plass.uni-jena.de/

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Sarita Dhaka,

Sarita Dhaka

Department of Chemistry, Indian Institute of Technology Roorkee, Roorkee 247667, India

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Subhashree P. Dash,

Subhashree P. Dash

Department of Chemistry, National Institute of Technology, Rourkela 769008 Odisha, India, http://https://sites.google.com/site/drrupamdinda/

Department of Chemistry, Indira Gandhi Institute of Technology, Sarang, Parjang, Dhenkanal 759146, India

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Sudarshana Majumder,

Sudarshana Majumder

Department of Chemistry, National Institute of Technology, Rourkela 769008 Odisha, India, http://https://sites.google.com/site/drrupamdinda/

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Mannar R. Maurya,

Mannar R. Maurya

Department of Chemistry, Indian Institute of Technology Roorkee, Roorkee 247667, India

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Winfried Plass,

Corresponding Author

Winfried Plass

[email protected]

Institute of Inorganic and Analytical Chemistry, Chair of Inorganic Chemistry II, Friedrich Schiller University Jena, Humboldtstr. 8, 07743 Jena, Germany, http://www.plass.uni-jena.de/

Winfried Plass, Institute of Inorganic and Analytical Chemistry, Chair of Inorganic Chemistry II, Friedrich Schiller University Jena, Humboldtstr. 8, 07743 Jena, Germany

Rupam Dinda, Department of Chemistry, National Institute of Technology, Rourkela 769008 Odisha, India

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Werner Kaminsky,

Werner Kaminsky

Department of Chemistry, University of Washington, Box 351700, Seattle, WA 98195, USA

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Rupam Dinda,

Corresponding Author

Rupam Dinda

[email protected]

Department of Chemistry, National Institute of Technology, Rourkela 769008 Odisha, India, http://https://sites.google.com/site/drrupamdinda/

Winfried Plass, Institute of Inorganic and Analytical Chemistry, Chair of Inorganic Chemistry II, Friedrich Schiller University Jena, Humboldtstr. 8, 07743 Jena, Germany

Rupam Dinda, Department of Chemistry, National Institute of Technology, Rourkela 769008 Odisha, India

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Sagarika Pasayat,

Sagarika Pasayat

Department of Chemistry, National Institute of Technology, Rourkela 769008 Odisha, India, http://https://sites.google.com/site/drrupamdinda/

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Michael Böhme,

Michael Böhme

Institute of Inorganic and Analytical Chemistry, Chair of Inorganic Chemistry II, Friedrich Schiller University Jena, Humboldtstr. 8, 07743 Jena, Germany, http://www.plass.uni-jena.de/

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Sarita Dhaka,

Sarita Dhaka

Department of Chemistry, Indian Institute of Technology Roorkee, Roorkee 247667, India

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Subhashree P. Dash,

Subhashree P. Dash

Department of Chemistry, National Institute of Technology, Rourkela 769008 Odisha, India, http://https://sites.google.com/site/drrupamdinda/

Department of Chemistry, Indira Gandhi Institute of Technology, Sarang, Parjang, Dhenkanal 759146, India

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Sudarshana Majumder,

Sudarshana Majumder

Department of Chemistry, National Institute of Technology, Rourkela 769008 Odisha, India, http://https://sites.google.com/site/drrupamdinda/

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Mannar R. Maurya,

Mannar R. Maurya

Department of Chemistry, Indian Institute of Technology Roorkee, Roorkee 247667, India

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Winfried Plass,

Corresponding Author

Winfried Plass

[email protected]

Institute of Inorganic and Analytical Chemistry, Chair of Inorganic Chemistry II, Friedrich Schiller University Jena, Humboldtstr. 8, 07743 Jena, Germany, http://www.plass.uni-jena.de/

Winfried Plass, Institute of Inorganic and Analytical Chemistry, Chair of Inorganic Chemistry II, Friedrich Schiller University Jena, Humboldtstr. 8, 07743 Jena, Germany

Rupam Dinda, Department of Chemistry, National Institute of Technology, Rourkela 769008 Odisha, India

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Werner Kaminsky,

Werner Kaminsky

Department of Chemistry, University of Washington, Box 351700, Seattle, WA 98195, USA

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Rupam Dinda,

Corresponding Author

Rupam Dinda

[email protected]

Department of Chemistry, National Institute of Technology, Rourkela 769008 Odisha, India, http://https://sites.google.com/site/drrupamdinda/

Winfried Plass, Institute of Inorganic and Analytical Chemistry, Chair of Inorganic Chemistry II, Friedrich Schiller University Jena, Humboldtstr. 8, 07743 Jena, Germany

Rupam Dinda, Department of Chemistry, National Institute of Technology, Rourkela 769008 Odisha, India

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First published: 07 March 2016

https://doi.org/10.1002/ejic.201501465

Citations: 30

^†

Dedicated to Professor Ekkehardt Fluck on the occasion of his 85th birthday

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Graphical Abstract

Two unique dioxidomolybdenum(VI) complexes [MoO₂L′^1–2] (1 and 2) containing ligands generated by metal-mediated interligand C–C bond formation are reported and are investigated by DFT calculations. Unique observations not found in the corresponding vanadium(V) complexes [VO₂L^1–2] (3 and 4) and the catalytic potentials of 1–4 are disclosed.

Abstract

Two novel dioxidomolybdenum(VI) complexes [MoO₂L′¹] (1) and [MoO₂L′²] (2) containing the MoO₂²⁺ motif with unexpected coordination motifs due to ligand rearrangement through Mo-mediated interligand C–C bond formation are reported. The ligands (H₂L′^1–2) are tetradentate C–C-coupled O₂N₂-donor systems formed in situ during synthesis of the complexes by reaction of [Mo^VIO₂(acac)₂] with Schiff base ligands of 2-aminophenol with 2-pyridinecarbaldehyde (HL¹) and 2-quinolinecarbaldehyde (HL²). To confirm that the ligand rearrangement is assisted by molybdenum, the corresponding vanadium complexes [VO₂L¹] (3) and [VO₂L²] (4) containing original Schiff base ligand (HL^1,2) are also reported here. All complexes 1–4 are characterized by several physicochemical techniques and the structural features of 1 and 2 have been solved by X-ray crystallography. The proposed mechanism of molybdenum-mediated interligand C–C bond formation is supported by DFT calculations including the comparisons with the synthesized vanadium analogues. The catalytic potentials of 1–4 for the epoxidation of styrene and cyclohexene have also been explored.

Supporting Information

References

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Volume2016, Issue10

April 2016

Pages 1604-1618

Synthesis, Theoretical Study and Catalytic Application of Oxidometal (Mo or V) Complexes: Unexpected Coordination Due to Ligand Rearrangement through Metal-Mediated C–C Bond Formation^†

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Synthesis, Theoretical Study and Catalytic Application of Oxidometal (Mo or V) Complexes: Unexpected Coordination Due to Ligand Rearrangement through Metal-Mediated C–C Bond Formation†

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Synthesis, Theoretical Study and Catalytic Application of Oxidometal (Mo or V) Complexes: Unexpected Coordination Due to Ligand Rearrangement through Metal-Mediated C–C Bond Formation^†