Spectroscopic observation of oxygen dissociation on nitrogen-doped graphene

Abstract Carbon nanomaterials’ reactivity towards oxygen is very poor, limiting their potential applications. However, nitrogen doping is an established way to introduce active sites that facilitate interaction with gases. This boosts the materials’ reactivity for bio-/gas sensing and enhances their...

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Autores principales:	Mattia Scardamaglia, Toma Susi, Claudia Struzzi, Rony Snyders, Giovanni Di Santo, Luca Petaccia, Carla Bittencourt
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2017
Materias:	Medicine R Science Q
Acceso en línea:	https://doaj.org/article/6a09a7585ae94a2e805e64bdb2f58cd4
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spelling	oai:doaj.org-article:6a09a7585ae94a2e805e64bdb2f58cd42021-12-02T11:41:12ZSpectroscopic observation of oxygen dissociation on nitrogen-doped graphene10.1038/s41598-017-08651-12045-2322https://doaj.org/article/6a09a7585ae94a2e805e64bdb2f58cd42017-08-01T00:00:00Zhttps://doi.org/10.1038/s41598-017-08651-1https://doaj.org/toc/2045-2322Abstract Carbon nanomaterials’ reactivity towards oxygen is very poor, limiting their potential applications. However, nitrogen doping is an established way to introduce active sites that facilitate interaction with gases. This boosts the materials’ reactivity for bio-/gas sensing and enhances their catalytic performance for the oxygen reduction reaction. Despite this interest, the role of differently bonded nitrogen dopants in the interaction with oxygen is obscured by experimental challenges and has so far resisted clear conclusions. We study the interaction of molecular oxygen with graphene doped via nitrogen plasma by in situ high-resolution synchrotron techniques, supported by density functional theory core level simulations. The interaction leads to oxygen dissociation and the formation of carbon-oxygen single bonds on graphene, along with a band gap opening and a rounding of the Dirac cone. The change of the N 1 s core level signal indicates that graphitic nitrogen is involved in the observed mechanism: the adsorbed oxygen molecule is dissociated and the two O atoms chemisorb with epoxy bonds to the nearest carbon neighbours of the graphitic nitrogen. Our findings help resolve existing controversies and offer compelling new evidence of the ORR pathway.Mattia ScardamagliaToma SusiClaudia StruzziRony SnydersGiovanni Di SantoLuca PetacciaCarla BittencourtNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 7, Iss 1, Pp 1-11 (2017)
institution	DOAJ
collection	DOAJ
language	EN
topic	Medicine R Science Q
spellingShingle	Medicine R Science Q Mattia Scardamaglia Toma Susi Claudia Struzzi Rony Snyders Giovanni Di Santo Luca Petaccia Carla Bittencourt Spectroscopic observation of oxygen dissociation on nitrogen-doped graphene
description	Abstract Carbon nanomaterials’ reactivity towards oxygen is very poor, limiting their potential applications. However, nitrogen doping is an established way to introduce active sites that facilitate interaction with gases. This boosts the materials’ reactivity for bio-/gas sensing and enhances their catalytic performance for the oxygen reduction reaction. Despite this interest, the role of differently bonded nitrogen dopants in the interaction with oxygen is obscured by experimental challenges and has so far resisted clear conclusions. We study the interaction of molecular oxygen with graphene doped via nitrogen plasma by in situ high-resolution synchrotron techniques, supported by density functional theory core level simulations. The interaction leads to oxygen dissociation and the formation of carbon-oxygen single bonds on graphene, along with a band gap opening and a rounding of the Dirac cone. The change of the N 1 s core level signal indicates that graphitic nitrogen is involved in the observed mechanism: the adsorbed oxygen molecule is dissociated and the two O atoms chemisorb with epoxy bonds to the nearest carbon neighbours of the graphitic nitrogen. Our findings help resolve existing controversies and offer compelling new evidence of the ORR pathway.
format	article
author	Mattia Scardamaglia Toma Susi Claudia Struzzi Rony Snyders Giovanni Di Santo Luca Petaccia Carla Bittencourt
author_facet	Mattia Scardamaglia Toma Susi Claudia Struzzi Rony Snyders Giovanni Di Santo Luca Petaccia Carla Bittencourt
author_sort	Mattia Scardamaglia
title	Spectroscopic observation of oxygen dissociation on nitrogen-doped graphene
title_short	Spectroscopic observation of oxygen dissociation on nitrogen-doped graphene
title_full	Spectroscopic observation of oxygen dissociation on nitrogen-doped graphene
title_fullStr	Spectroscopic observation of oxygen dissociation on nitrogen-doped graphene
title_full_unstemmed	Spectroscopic observation of oxygen dissociation on nitrogen-doped graphene
title_sort	spectroscopic observation of oxygen dissociation on nitrogen-doped graphene
publisher	Nature Portfolio
publishDate	2017
url	https://doaj.org/article/6a09a7585ae94a2e805e64bdb2f58cd4
work_keys_str_mv	AT mattiascardamaglia spectroscopicobservationofoxygendissociationonnitrogendopedgraphene AT tomasusi spectroscopicobservationofoxygendissociationonnitrogendopedgraphene AT claudiastruzzi spectroscopicobservationofoxygendissociationonnitrogendopedgraphene AT ronysnyders spectroscopicobservationofoxygendissociationonnitrogendopedgraphene AT giovannidisanto spectroscopicobservationofoxygendissociationonnitrogendopedgraphene AT lucapetaccia spectroscopicobservationofoxygendissociationonnitrogendopedgraphene AT carlabittencourt spectroscopicobservationofoxygendissociationonnitrogendopedgraphene
_version_	1718395465481846784

Spectroscopic observation of oxygen dissociation on nitrogen-doped graphene

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