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    Título
    (1,2-Azole)bis(bipyridyl)ruthenium(II) Complexes: Electrochemistry, Luminescent Properties, And Electro- And Photocatalysts for CO2 Reduction
    Autor
    Cuéllar, Elena
    Pastor, Laura
    García Herbosa, GabrielAutoridad UBU Orcid
    Nganga, John
    Angeles-Boza, Alfredo M.
    Diez Varga, Alberto
    Torroba Pérez, TomásAutoridad UBU Orcid
    Martín-Alvarez, Jose M.
    Miguel, Daniel
    Villafañe, Fernando
    Publicado en
    Inorganic Chemistry. 2021, V. 60, n. 2, p. 692–704
    Editorial
    American Chemical Society
    Fecha de publicación
    2020-12
    ISSN
    0020-1669
    DOI
    10.1021/acs.inorgchem.0c02716
    Resumen
    New cis-(1,2-azole)-aquo bis(2,2′-bipyridyl)ruthenium(II) (1,2-azole (az*H) = pzH (pyrazole), dmpzH (3,5-dimethylpyrazole), and indzH (indazole)) complexes are synthesized via chlorido abstraction from cis-[Ru(bipy)2Cl(az*H)]OTf. The latter are obtained from cis-[Ru(bipy)2Cl2] after the subsequent coordination of the 1,2-azole. All the compounds are characterized by 1H, 13C, 15N NMR spectroscopy as well as IR spectroscopy. Two chlorido complexes (pzH and indzH) and two aquo complexes (indzH and dmpzH) are also characterized by X-ray diffraction. Photophysical and electrochemical studies were carried out on all the complexes. The photophysical data support the phosphorescence of the complexes. The electrochemical behavior of all the complexes in an Ar atmosphere indicate that the oxidation processes assigned to Ru(II) → Ru(III) occurs at higher potentials in the aquo complexes. The reduction processes under Ar lead to several waves, indicating that the complexes undergo successive electron-transfer reductions that are centered in the bipy ligands. The first electron reduction is reversible. The electrochemical behavior in CO2 media is consistent with CO2 electrocatalyzed reduction, where the values of the catalytic activity [icat(CO2)/ip(Ar)] ranged from 2.9 to 10.8. Controlled potential electrolysis of the chlorido and aquo complexes affords CO and formic acid, with the latter as the major product after 2 h. Photocatalytic experiments in MeCN with [Ru(bipy)3]Cl2 as the photosensitizer and TEOA as the electron donor, which were irradiated with >300 nm light for 24 h, led to CO and HCOOH as the main reduction products, achieving a combined turnover number (TONCO+HCOO–) as high as 107 for 2c after 24 h of irradiation.
    Palabras clave
    Catalytic reactions
    Electrochemical reduction
    Ligands
    Oxidation
    Redox reactions
    Materia
    Química inorgánica
    Chemistry, Inorganic
    URI
    http://hdl.handle.net/10259/6817
    Versión del editor
    https://dx.doi.org/10.1021/acs.inorgchem.0c02716
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    Nombre:
    Cuellar-ic_2020.pdf
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    1.402Mb
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