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Materials (Basel). 2019 Feb 23;12(4). pii: E666. doi: 10.3390/ma12040666.

Electroanalytical Performance of Nitrogen-Doped Graphene Films Processed in One Step by Pulsed Laser Deposition Directly Coupled with Thermal Annealing.

Author information

1
Laboratoire Hubert Curien, UMR 5516 CNRS, Université de Lyon, Université Jean Monnet, F-42000 Saint-Étienne, France. Florent.Bourquard@univ-st-etienne.fr.
2
Laboratoire Hubert Curien, UMR 5516 CNRS, Université de Lyon, Université Jean Monnet, F-42000 Saint-Étienne, France. yannick.bleu@univ-st-etienne.fr.
3
Laboratoire Hubert Curien, UMR 5516 CNRS, Université de Lyon, Université Jean Monnet, F-42000 Saint-Étienne, France. Anne.Sophie.Loir@univ-st-etienne.fr.
4
Synchrotron SOLEIL, Université Paris-Saclay, Saint Aubin, F-91192 Gif sur Yvette, France. borja.caja-munoz@synchrotron-soleil.fr.
5
Synchrotron SOLEIL, Université Paris-Saclay, Saint Aubin, F-91192 Gif sur Yvette, France. jose.avila@synchrotron-soleil.fr.
6
Instituto de Ciencia de Materiales de Madrid, Sor Juana Inés de la Cruz, 328049 Madrid, Spain. mc.asensio@csic.es.
7
Institut des Sciences Analytiques, UMR 5280 CNRS, Université de Lyon, Université Claude Bernard Lyon 1, F-69100 Villeurbanne, France. gaetan.raimondi@isa-lyon.fr.
8
Institut des Sciences Analytiques, UMR 5280 CNRS, Université de Lyon, Université Claude Bernard Lyon 1, F-69100 Villeurbanne, France. m.shokouhi89@gmail.com.
9
Institut des Sciences Analytiques, UMR 5280 CNRS, Université de Lyon, Université Claude Bernard Lyon 1, F-69100 Villeurbanne, France. ilhemras@hotmail.fr.
10
Institut des Sciences Analytiques, UMR 5280 CNRS, Université de Lyon, Université Claude Bernard Lyon 1, F-69100 Villeurbanne, France. carole.farre@univ-lyon1.fr.
11
Institut des Sciences Analytiques, UMR 5280 CNRS, Université de Lyon, Université Claude Bernard Lyon 1, F-69100 Villeurbanne, France. carole.chaix-bauvais@univ-lyon1.fr.
12
Mines Saint-Etienne, Université de Lyon, UMR 5307 CNRS, Centre SMS, F-42023 Saint-Etienne, France. barnier@emse.fr.
13
Institut des Sciences Analytiques, UMR 5280 CNRS, Université de Lyon, Université Claude Bernard Lyon 1, F-69100 Villeurbanne, France. Nicole.Jaffrezic@univ-lyon1.fr.
14
Laboratoire Hubert Curien, UMR 5516 CNRS, Université de Lyon, Université Jean Monnet, F-42000 Saint-Étienne, France. Florence.Garrelie@univ-st-etienne.fr.
15
Laboratoire Hubert Curien, UMR 5516 CNRS, Université de Lyon, Université Jean Monnet, F-42000 Saint-Étienne, France. christophe.donnet@univ-st-etienne.fr.

Abstract

Graphene-based materials are widely studied to enable significant improvements in electroanalytical devices requiring new generations of robust, sensitive and low-cost electrodes. In this paper, we present a direct one-step route to synthetize a functional nitrogen-doped graphene film onto a Ni-covered silicon electrode substrate heated at high temperature, by pulsed laser deposition of carbon in the presence of a surrounding nitrogen atmosphere, with no post-deposition transfer of the film. With the ferrocene methanol system, the functionalized electrode exhibits excellent reversibility, close to the theoretical value of 59 mV, and very high sensitivity to hydrogen peroxide oxidation. Our electroanalytical results were correlated with the composition and nanoarchitecture of the N-doped graphene film containing 1.75 at % of nitrogen and identified as a few-layer defected and textured graphene film containing a balanced mixture of graphitic-N and pyrrolic-N chemical functions. The absence of nitrogen dopant in the graphene film considerably degraded some electroanalytical performances. Heat treatment extended beyond the high temperature graphene synthesis did not significantly improve any of the performances. This work contributes to a better understanding of the electrochemical mechanisms of doped graphene-based electrodes obtained by a direct and controlled synthesis process.

KEYWORDS:

electrochemical analysis; graphene; nitrogen-doped graphene; oxygen peroxide oxidation; pulse laser deposition

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