期刊
ACS CATALYSIS
卷 5, 期 1, 页码 129-144出版社
AMER CHEMICAL SOC
DOI: 10.1021/cs501211h
关键词
graphene; graphene oxide quantum dots; doped-quantum dots; multidoping; electrochemical preparation; oxygen reduction reaction; density functional theory
资金
- Fondazione Cariparo
- PRIN Project DESCARTES [2010BNZ3F2]
- Fuel Cell and Hydrogen Initiative-Joint Undertaking (FCH-JU) within the CathCat project [303492]
- Italian MIUR [RBFR128BEC]
- University of Padova [CPDA128318/12]
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 similar to 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.
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