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    Por favor, use este identificador para citar o enlazar este ítem: http://hdl.handle.net/10259/6823

    Título
    Luminescent Rhenium(I)tricarbonyl Complexes Containing Different Pyrazoles and Their Successive Deprotonation Products: CO2 Reduction Electrocatalysts
    Autor
    Merillas, Beatriz
    Cuéllar, Elena
    Diez Varga, Alberto
    Torroba Pérez, TomásAutoridad UBU Orcid
    García Herbosa, GabrielAutoridad UBU Orcid
    Fernández, Sergio
    Lloret-Fillol, Julio
    Martín-Alvarez, Jose M.
    Miguel, Daniel
    Villafañe, Fernando
    Publicado en
    Inorganic Chemistry. 2020, V. 59, n. 15, p. 11152–11165
    Editorial
    American Chemical Society
    Fecha de publicación
    2020-07
    ISSN
    0020-1669
    DOI
    10.1021/acs.inorgchem.0c01654
    Resumen
    Cationic fac-[Re(CO)3(pz*H)(pypzH)]OTf (pz*H = pyrazole, pzH; 3,5-dimethylpyrazole, dmpzH; indazole, indzH; 3-(2-pyridyl)pyrazole, pypzH) were obtained from fac-[ReBr(CO)3(pypzH)] by halide abstraction with AgOTf and subsequent addition of the corresponding pyrazole. Successive deprotonation with Na2CO3 and NaOH gave neutral fac-[Re(CO)3(pz*H)(pypz)] and anionic Na{fac-[Re(CO)3(pz*)(pypz)]} complexes, respectively. Cationic fac-[Re(CO)3(pz*H)(pypzH)]OTf, neutral complexes fac-[Re(CO)3(pz*H)(pypz)], and fac-[Re(CO)3(pypz)2Na] were subjected to photophysical and electrochemical studies. They exhibit phosphorescent decays from a prevalently 3MLCT excited state with quantum yields (Φ) in the range between 0.03 and 0.58 and long lifetimes (τ from 220 to 869 ns). The electrochemical behavior in Ar atmosphere of cationic and neutral complexes indicates that the oxidation processes assigned to ReI → ReII occurs at lower potentials for the neutral complex compared to cationic complex. The reduction processes occur at the ligands and do not depend on the charge of the complexes. The electrochemical behavior in CO2 saturated media is consistent with CO2 electrocatalyzed reduction, where the values of the catalytic activity [icat(CO2)/icat(Ar)] ranged from 2.7 to 11.5 (compared to 8.1 for fac-[Re(CO)3Cl(bipy)] studied as a reference). Controlled potential electrolysis for the pyrazole cationic (3a) and neutral (4a) complexes after 1 h affords CO in faraday yields of 61 and 89%, respectively. These values are higher for indazole complexes and may be related to the acidity of the coordinated pyrazole.
    Palabras clave
    Deprotonation
    Diimides
    Electrodes
    Ligands
    Reaction mechanisms
    Materia
    Química inorgánica
    Chemistry, Inorganic
    URI
    http://hdl.handle.net/10259/6823
    Versión del editor
    https://doi.org/10.1021/acs.inorgchem.0c01654
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    • Artículos SUPRABUR
    • Artículos AMIDORUCA
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    Nombre:
    Merillas-ic_2020.pdf
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    724.9Kb
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