Singly and multiply doped graphene oxide quantum dots have been synthesized by a simple electrochemical method using water as solvent. The obtained materials have been characterized by photoemission spectroscopy and scanning tunneling microscopy, in order to get a detailed picture of their chemical and structural properties. The electrochemical activity toward the oxygen reduction reaction of the doped graphene oxide quantum dots has been investigated by cyclic voltammetry and rotating disk electrode measurements, showing a clear decrease of the overpotential as a function of the dopant according to the sequence: N ∼ B > B,N. Moreover, assisted by density functional calculations of the Gibbs free energy associated with every electron transfer, we demonstrate that the selectivity of the reaction is controlled by the oxidation states of the dopants: as-prepared graphene oxide quantum dots follow a two-electron reduction path that leads to the formation of hydrogen peroxide, whereas after the reduction with NaBH4, the same materials favor a four-electron reduction of oxygen to water. (Chemical Equation Presented).

Favaro, M., Ferrighi, L., Fazio, G., Colazzo, L., Di Valentin, C., Durante, C., et al. (2015). Single and Multiple Doping in Graphene Quantum Dots: Unraveling the Origin of Selectivity in the Oxygen Reduction Reaction. ACS CATALYSIS, 5(1), 129-144 [10.1021/cs501211h].

Single and Multiple Doping in Graphene Quantum Dots: Unraveling the Origin of Selectivity in the Oxygen Reduction Reaction

FERRIGHI, LARA
Secondo
;
FAZIO, GIANLUCA;DI VALENTIN, CRISTIANA
;
2015

Abstract

Singly and multiply doped graphene oxide quantum dots have been synthesized by a simple electrochemical method using water as solvent. The obtained materials have been characterized by photoemission spectroscopy and scanning tunneling microscopy, in order to get a detailed picture of their chemical and structural properties. The electrochemical activity toward the oxygen reduction reaction of the doped graphene oxide quantum dots has been investigated by cyclic voltammetry and rotating disk electrode measurements, showing a clear decrease of the overpotential as a function of the dopant according to the sequence: N ∼ B > B,N. Moreover, assisted by density functional calculations of the Gibbs free energy associated with every electron transfer, we demonstrate that the selectivity of the reaction is controlled by the oxidation states of the dopants: as-prepared graphene oxide quantum dots follow a two-electron reduction path that leads to the formation of hydrogen peroxide, whereas after the reduction with NaBH4, the same materials favor a four-electron reduction of oxygen to water. (Chemical Equation Presented).
Articolo in rivista - Articolo scientifico
Scientifica
density functional theory; doped-quantum dots; electrochemical preparation; graphene; graphene oxide quantum dots; multidoping; oxygen reduction reaction; Catalysis
English
Favaro, M., Ferrighi, L., Fazio, G., Colazzo, L., Di Valentin, C., Durante, C., et al. (2015). Single and Multiple Doping in Graphene Quantum Dots: Unraveling the Origin of Selectivity in the Oxygen Reduction Reaction. ACS CATALYSIS, 5(1), 129-144 [10.1021/cs501211h].
Favaro, M; Ferrighi, L; Fazio, G; Colazzo, L; DI VALENTIN, C; Durante, C; Sedona, F; Gennaro, A; Agnoli, S; Granozzi, G
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Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/10281/91444
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