Reactivity descriptors for Cu bis-phenanthroline catalysts for the hydrogen peroxide reduction reaction
Following previous studies where the metal-centered redox potentials of MN4 complexes are proposed as a reactivity descriptor for different electrochemical reactions, in the present work we expand this idea to a series of substituted Cu(I)-phenanthrolines adsorbed on glassy carbon electrodes as cata...
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| Published in: | Electrochimica acta Vol. 357; p. 136881 |
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| Main Authors: | , , , , , , |
| Format: | Journal Article |
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| Abstract | Following previous studies where the metal-centered redox potentials of MN4 complexes are proposed as a reactivity descriptor for different electrochemical reactions, in the present work we expand this idea to a series of substituted Cu(I)-phenanthrolines adsorbed on glassy carbon electrodes as catalysts for the hydrogen peroxide reduction reaction (HPRR) in aqueous media. As the foot of the wave for HPRR on Cu-based modified electrodes is closely related to the Cu(II)/Cu(I) formal potential, we have found a linear correlation between the catalytic activity expressed as (log i)E and the E°'Cu(II)/Cu(I) redox potential of the complexes with a slope (dE°/dlogi)E close to +0.120 V dec−1, showing that the catalytic activity increases with the shift of E°'Cu(II)/Cu(I) to more positive potentials as a result of the electron-withdrawing nature of the substituents on the ligands. Moreover, the theoretical differences in the calculated chemical potentials (Δμ) of the reactive species follow a similar trend with the E°'Cu(II)/Cu(I) where a positive shift of this parameter is related with a higher Δμ and in consequence, with high catalytic activity. Furthermore, this strategy can be used for the smart design of biosensors as it was shown by the electroanalytical results.
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| AbstractList | Following previous studies where the metal-centered redox potentials of MN4 complexes are proposed as a reactivity descriptor for different electrochemical reactions, in the present work we expand this idea to a series of substituted Cu(I)-phenanthrolines adsorbed on glassy carbon electrodes as catalysts for the hydrogen peroxide reduction reaction (HPRR) in aqueous media. As the foot of the wave for HPRR on Cu-based modified electrodes is closely related to the Cu(II)/Cu(I) formal potential, we have found a linear correlation between the catalytic activity expressed as (log i)E and the E°'Cu(II)/Cu(I) redox potential of the complexes with a slope (dE°/dlogi)E close to +0.120 V dec−1, showing that the catalytic activity increases with the shift of E°'Cu(II)/Cu(I) to more positive potentials as a result of the electron-withdrawing nature of the substituents on the ligands. Moreover, the theoretical differences in the calculated chemical potentials (Δμ) of the reactive species follow a similar trend with the E°'Cu(II)/Cu(I) where a positive shift of this parameter is related with a higher Δμ and in consequence, with high catalytic activity. Furthermore, this strategy can be used for the smart design of biosensors as it was shown by the electroanalytical results.
[Display omitted] Following previous studies where the metal-centered redox potentials of MN4 complexes are proposed as a reactivity descriptor for different electrochemical reactions, in the present work we expand this idea to a series of substituted Cu(I)-phenanthrolines adsorbed on glassy carbon electrodes as catalysts for the hydrogen peroxide reduction reaction (HPRR) in aqueous media. As the foot of the wave for HPRR on Cu-based modified electrodes is closely related to the Cu(II)/Cu(I) formal potential, we have found a linear correlation between the catalytic activity expressed as (log i)E and the E°'Cu(II)/Cu(I) redox potential of the complexes with a slope (dE°/dlogi)E close to +0.120 V dec−1, showing that the catalytic activity increases with the shift of E°'Cu(II)/Cu(I) to more positive potentials as a result of the electron-withdrawing nature of the substituents on the ligands. Moreover, the theoretical differences in the calculated chemical potentials (Δμ) of the reactive species follow a similar trend with the E°'Cu(II)/Cu(I) where a positive shift of this parameter is related with a higher Δμ and in consequence, with high catalytic activity. Furthermore, this strategy can be used for the smart design of biosensors as it was shown by the electroanalytical results. |
| ArticleNumber | 136881 |
| Author | Bollo, Soledad Báez, Daniela F. Venegas, Ricardo Zagal, José H. Toro-Labbé, Alejandro Recio, F. Javier Muñoz-Becerra, Karina |
| Author_xml | – sequence: 1 givenname: Karina surname: Muñoz-Becerra fullname: Muñoz-Becerra, Karina organization: Laboratorio de Materiales y Energía, Facultad de Química y de Farmacia, Pontificia Universidad Católica de Chile, Santiago, Chile – sequence: 2 givenname: Daniela F. orcidid: 0000-0002-9663-8521 surname: Báez fullname: Báez, Daniela F. organization: Centro de Investigación de Procesos Redox (CiPRex), Facultad de Ciencias Químicas y Farmacéuticas, Universidad de Chile, Santiago, Chile – sequence: 3 givenname: José H. surname: Zagal fullname: Zagal, José H. organization: Facultad de Química y Biología, Departamento de Química de los Materiales, Universidad de Santiago de Chile, Santiago, Chile – sequence: 4 givenname: Soledad surname: Bollo fullname: Bollo, Soledad organization: Centro de Investigación de Procesos Redox (CiPRex), Facultad de Ciencias Químicas y Farmacéuticas, Universidad de Chile, Santiago, Chile – sequence: 5 givenname: Alejandro surname: Toro-Labbé fullname: Toro-Labbé, Alejandro organization: Laboratorio de Materiales y Energía, Facultad de Química y de Farmacia, Pontificia Universidad Católica de Chile, Santiago, Chile – sequence: 6 givenname: Ricardo orcidid: 0000-0001-7440-484X surname: Venegas fullname: Venegas, Ricardo email: rivenegas@uc.cl organization: Laboratorio de Materiales y Energía, Facultad de Química y de Farmacia, Pontificia Universidad Católica de Chile, Santiago, Chile – sequence: 7 givenname: F. Javier surname: Recio fullname: Recio, F. Javier email: javier.recio@uc.cl organization: Laboratorio de Materiales y Energía, Facultad de Química y de Farmacia, Pontificia Universidad Católica de Chile, Santiago, Chile |
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| Keywords | Copper catalysts Hydrogen peroxide reduction reaction Reactivity descriptors Hydrogen peroxide sensor |
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| Title | Reactivity descriptors for Cu bis-phenanthroline catalysts for the hydrogen peroxide reduction reaction |
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