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Role of the carbon defects in the catalytic oxygen reduction by graphite nanoparticles: a spectromagnetic, electrochemical and modellistic integrated approach

Abstract

The chemical groups present at the surface of graphite have been thought of for a long time as the main responsible for the catalytic activity in the oxygen reduction. Recently, it was proposed that also the surface defects give a significant contribution to promote this reaction, but the behaviour was only reported and with few comments on the mechanism and the intermediate species. The present paper aims to give a more detailed explanation of the catalytic activity, basing on the structure of the defects and on the size of the graphite particles. Structural, spectral and magnetic investigations (X ray, Raman and Electron Spin Resonance), electrochemical measurements contributed to describe the nature of the defects and their attitude to transfer electrons. Computational description gives a precise detail of the energy of the different defects and of their attitude to promote the reduction, also suggesting the structure of the intermediate adduct in the oxygen reduction. It resulted that molecular oxygen preferentially interacts with graphite defects, which involve the π-electron system and accumulate the spin density on the edges of grain, in particular, on the zig-zag edges present on the ball milled graphite. This promotes a more pronounced reactivity of this nanomaterial. The activation increases by decreasing the particle size.

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Publication details

The article was received on 13 Nov 2018, accepted on 11 Feb 2019 and first published on 12 Feb 2019


Article type: Paper
DOI: 10.1039/C8CP07023G
Citation: Phys. Chem. Chem. Phys., 2019, Accepted Manuscript

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    Role of the carbon defects in the catalytic oxygen reduction by graphite nanoparticles: a spectromagnetic, electrochemical and modellistic integrated approach

    C. Greco, U. Cosentino, D. Pitea, G. Moro, S. Santangelo, S. Patanè, M. D'Arienzo, M. Fiore, F. Morazzoni and R. Ruffo, Phys. Chem. Chem. Phys., 2019, Accepted Manuscript , DOI: 10.1039/C8CP07023G

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