Nitrogen-Doped Graphene: The Influence of Doping Level on the Charge-Transfer Resistance and Apparent Heterogeneous Electron Transfer Rate

Three nitrogen-doped graphene samples were synthesized by the hydrothermal method using urea as doping/reducing agent for graphene oxide (GO), previously dispersed in water. The mixture was poured into an autoclave and placed in the oven at 160 °C for 3, 8 and 12 h. The samples were corresp...

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Main Authors: Maria Coros, Codruta Varodi, Florina Pogacean, Emese Gal, Stela M. Pruneanu
Format: Article
Language:English
Published: MDPI AG 2020-03-01
Series:Sensors
Subjects:
Online Access:https://www.mdpi.com/1424-8220/20/7/1815
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author Maria Coros
Codruta Varodi
Florina Pogacean
Emese Gal
Stela M. Pruneanu
author_facet Maria Coros
Codruta Varodi
Florina Pogacean
Emese Gal
Stela M. Pruneanu
author_sort Maria Coros
collection DOAJ
description Three nitrogen-doped graphene samples were synthesized by the hydrothermal method using urea as doping/reducing agent for graphene oxide (GO), previously dispersed in water. The mixture was poured into an autoclave and placed in the oven at 160 &#176;C for 3, 8 and 12 h. The samples were correspondingly denoted NGr-1, NGr-2 and NGr-3. The effect of the reaction time on the morphology, structure and electrochemical properties of the resulting materials was thoroughly investigated using scanning electron microscopy (SEM) Raman spectroscopy, X-ray powder diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), elemental analysis, Cyclic Voltammetry (CV) and electrochemical impedance spectroscopy (EIS). For NGr-1 and NGr-2, the nitrogen concentration obtained from elemental analysis was around 6.36 wt%. In the case of NGr-3, a slightly higher concentration of 6.85 wt% was obtained. The electrochemical studies performed with NGr modified electrodes proved that the charge-transfer resistance (R<sub>ct</sub>) and the apparent heterogeneous electron transfer rate constant (K<sub>app</sub>) depend not only on the nitrogen doping level but also on the type of nitrogen atoms found at the surface (pyrrolic-N, pyridinic-N or graphitic-N). In our case, the NGr-1 sample which has the lowest doping level and the highest concentration of pyrrolic-N among all nitrogen-doped samples exhibits the best electrochemical parameters: a very small R<sub>ct </sub>(38.3 &#937;), a large K<sub>app </sub>(13.9 &#215; 10<sup>&#8722;2</sup> cm/s) and the best electrochemical response towards 8-hydroxy-2&#8242;-deoxyguanosine detection (8-OHdG).
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spelling doaj.art-4f00a48588a44913a4919bdd540a98612022-12-22T03:18:49ZengMDPI AGSensors1424-82202020-03-01207181510.3390/s20071815s20071815Nitrogen-Doped Graphene: The Influence of Doping Level on the Charge-Transfer Resistance and Apparent Heterogeneous Electron Transfer RateMaria Coros0Codruta Varodi1Florina Pogacean2Emese Gal3Stela M. Pruneanu4National Institute for Research and Development of Isotopic and Molecular Technologies, Donat Street, No. 67-103, 400293 Cluj-Napoca, RomaniaNational Institute for Research and Development of Isotopic and Molecular Technologies, Donat Street, No. 67-103, 400293 Cluj-Napoca, RomaniaNational Institute for Research and Development of Isotopic and Molecular Technologies, Donat Street, No. 67-103, 400293 Cluj-Napoca, RomaniaDepartment of Chemistry and Chemical Engineering, Hungarian Line of Study, Babes-Bolyai University, 11 Arany János St., 400028 Cluj-Napoca, RomaniaNational Institute for Research and Development of Isotopic and Molecular Technologies, Donat Street, No. 67-103, 400293 Cluj-Napoca, RomaniaThree nitrogen-doped graphene samples were synthesized by the hydrothermal method using urea as doping/reducing agent for graphene oxide (GO), previously dispersed in water. The mixture was poured into an autoclave and placed in the oven at 160 &#176;C for 3, 8 and 12 h. The samples were correspondingly denoted NGr-1, NGr-2 and NGr-3. The effect of the reaction time on the morphology, structure and electrochemical properties of the resulting materials was thoroughly investigated using scanning electron microscopy (SEM) Raman spectroscopy, X-ray powder diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), elemental analysis, Cyclic Voltammetry (CV) and electrochemical impedance spectroscopy (EIS). For NGr-1 and NGr-2, the nitrogen concentration obtained from elemental analysis was around 6.36 wt%. In the case of NGr-3, a slightly higher concentration of 6.85 wt% was obtained. The electrochemical studies performed with NGr modified electrodes proved that the charge-transfer resistance (R<sub>ct</sub>) and the apparent heterogeneous electron transfer rate constant (K<sub>app</sub>) depend not only on the nitrogen doping level but also on the type of nitrogen atoms found at the surface (pyrrolic-N, pyridinic-N or graphitic-N). In our case, the NGr-1 sample which has the lowest doping level and the highest concentration of pyrrolic-N among all nitrogen-doped samples exhibits the best electrochemical parameters: a very small R<sub>ct </sub>(38.3 &#937;), a large K<sub>app </sub>(13.9 &#215; 10<sup>&#8722;2</sup> cm/s) and the best electrochemical response towards 8-hydroxy-2&#8242;-deoxyguanosine detection (8-OHdG).https://www.mdpi.com/1424-8220/20/7/1815nitrogen-doped graphenecharge-transfer resistanceapparent heterogeneous electron transfer ratemodified electrodesdetection of 8-ohdg
spellingShingle Maria Coros
Codruta Varodi
Florina Pogacean
Emese Gal
Stela M. Pruneanu
Nitrogen-Doped Graphene: The Influence of Doping Level on the Charge-Transfer Resistance and Apparent Heterogeneous Electron Transfer Rate
Sensors
nitrogen-doped graphene
charge-transfer resistance
apparent heterogeneous electron transfer rate
modified electrodes
detection of 8-ohdg
title Nitrogen-Doped Graphene: The Influence of Doping Level on the Charge-Transfer Resistance and Apparent Heterogeneous Electron Transfer Rate
title_full Nitrogen-Doped Graphene: The Influence of Doping Level on the Charge-Transfer Resistance and Apparent Heterogeneous Electron Transfer Rate
title_fullStr Nitrogen-Doped Graphene: The Influence of Doping Level on the Charge-Transfer Resistance and Apparent Heterogeneous Electron Transfer Rate
title_full_unstemmed Nitrogen-Doped Graphene: The Influence of Doping Level on the Charge-Transfer Resistance and Apparent Heterogeneous Electron Transfer Rate
title_short Nitrogen-Doped Graphene: The Influence of Doping Level on the Charge-Transfer Resistance and Apparent Heterogeneous Electron Transfer Rate
title_sort nitrogen doped graphene the influence of doping level on the charge transfer resistance and apparent heterogeneous electron transfer rate
topic nitrogen-doped graphene
charge-transfer resistance
apparent heterogeneous electron transfer rate
modified electrodes
detection of 8-ohdg
url https://www.mdpi.com/1424-8220/20/7/1815
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AT florinapogacean nitrogendopedgraphenetheinfluenceofdopinglevelonthechargetransferresistanceandapparentheterogeneouselectrontransferrate
AT emesegal nitrogendopedgraphenetheinfluenceofdopinglevelonthechargetransferresistanceandapparentheterogeneouselectrontransferrate
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