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Nitric Oxide Oxygenation Reactions of Cobalt-Peroxo and Cobalt-Nitrosyl Complexes

Cite this: Inorg. Chem. 2023, 62, 19, 7385–7392
Publication Date (Web):May 1, 2023
https://doi.org/10.1021/acs.inorgchem.3c00639
Copyright © 2023 American Chemical Society

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    Abstract

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    Here, we report a comparative study of nitric oxide oxidation (NOO) reactions of CoIII-peroxo (CoIII–O22–) and Co-nitrosyl ({CoNO}8) complexes bearing the same N4-donor ligand (HMTETA) framework. In this regard, we prepared and characterized two new [(HMTETA)CoIII(O22–)]+ (2, S = 2) and [(HMTETA)Co(NO)]2+ (3, S = 1) complexes from [(HMTETA)CoII(CH3CN)2]2+ (1). Both complexes (2 and 3) are characterized by different spectroscopic measurements, including their DFT-optimized structures. Complex 2 produces CoII-nitrato [(HMTETA)CoII(NO3)]+ (CoII–NO3, 4) complex in the presence of NO. In contrast, when 3 reacted with a superoxide (O2•–) anion, it generated CoII-nitrito [(HMTETA)CoII(NO2)]+ (CoII–NO2, 5) with O2 evolution. Experiments performed using 18/16O-labeled superoxide (18O2•–/16O2•–) showed that O2 originated from the O2•– anion. Both the NOO reactions are believed to proceed via a presumed peroxynitrite (PN) intermediate. Although we did not get direct spectral evidence for the proposed PN species, the mechanistic investigation using 2,4-di-tert-butylphenol indirectly suggests the formation of a PN intermediate. Furthermore, tracking the source of the N-atom in the above NOO reactions using 15N-labeled nitrogen (15NO) revealed N-atoms in 4 (CoII15NO3) and 5 (CoII15NO2) derived from the 15NO moiety.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.inorgchem.3c00639.

    • Experimental details, crystallographic data, single-crystal X-ray diffraction structures and their parameters, 1H NMR of all compounds, ESI-mass spectra, additional FI-IR data, UV–vis absorption spectra, kinetics of reactivity, computed Eigen-value plot, and B3LYP/D2 optimized Cartesian coordinates (PDF)

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    CCDC 22149262214928 contain the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/data_request/cif, or by emailing [email protected], or by contacting The Cambridge Crystallographic Data Centre, 12 Union Road, Cambridge CB2 1EZ, UK; fax: +44 1223 336033.

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    Cited By

    This article is cited by 1 publications.

    1. Cheng-Jhe Liao, Yu-Ting Tseng, Yu-An Cheng, Loise Ann Dayao, Linda Iffland-Mühlhaus, Leland B. Gee, Ryan D. Ribson, Ting-Shan Chan, Ulf-Peter Apfel, Tsai-Te Lu. Ligand Control of Dinitrosyl Iron Complexes for Selective Superoxide-Mediated Nitric Oxide Monooxygenation and Superoxide–Dioxygen Interconversion. Journal of the American Chemical Society 2023, 145 (37) , 20389-20402. https://doi.org/10.1021/jacs.3c05577