Accurate control of the covalent functionalization of single-walled carbon nanotubes for the electro-enzymatically controlled oxidation of biomolecules
Single-walled carbon nanotubes (SWCNTs) were functionalized by ferrocene through ethyleneglycol chains of different lengths (FcETGn) and the functionalized SWCNTs (f-SWCNTs) were characterized by different complementary analytical techniques. In particular, high-resolution scanning electron transmis...
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doaj-54dc3a5d0904408e9f171dbe139b207a2020-11-25T00:44:00ZengBeilstein-InstitutBeilstein Journal of Nanotechnology2190-42862018-10-01912750276210.3762/bjnano.9.2572190-4286-9-257Accurate control of the covalent functionalization of single-walled carbon nanotubes for the electro-enzymatically controlled oxidation of biomoleculesNaoual Allali0Veronika Urbanova1Mathieu Etienne2Xavier Devaux3Martine Mallet4Brigitte Vigolo5Jean-Joseph Adjizian6Chris P. Ewels7Sven Oberg8Alexander V. Soldatov9Edward McRae10Yves Fort11Manuel Dossot12Victor Mamane13LCPME, UMR CNRS-Université de Lorraine 7564, 405 rue de Vandoeuvre, F-54602 Villers-lès-Nancy, FranceLCPME, UMR CNRS-Université de Lorraine 7564, 405 rue de Vandoeuvre, F-54602 Villers-lès-Nancy, FranceLCPME, UMR CNRS-Université de Lorraine 7564, 405 rue de Vandoeuvre, F-54602 Villers-lès-Nancy, FranceIJL, UMR CNRS-Université de Lorraine 7198, Parc de Saurupt - CS 50840, 54011 Nancy Cedex, FranceLCPME, UMR CNRS-Université de Lorraine 7564, 405 rue de Vandoeuvre, F-54602 Villers-lès-Nancy, FranceIJL, UMR CNRS-Université de Lorraine 7198, Campus Victor Grignard, Faculté des Sciences et Technologies, 54506 Vandoeuvre-lès-Nancy Cedex, FranceIMN, UMR CNRS-Université de Nantes 6502IMN, UMR CNRS-Université de Nantes 6502Department of Engineering Sciences and Mathematics, Lulea Technical University, SwedenDepartment of Engineering Sciences and Mathematics, Lulea Technical University, SwedenIJL, UMR CNRS-Université de Lorraine 7198, Campus Victor Grignard, Faculté des Sciences et Technologies, 54506 Vandoeuvre-lès-Nancy Cedex, FranceSRSMC, UMR CNRS-Université de Lorraine 7565, Campus Victor Grignard, Faculté des Sciences et Technologies, F-54506 Vandoeuvre-lès-Nancy, FranceLCPME, UMR CNRS-Université de Lorraine 7564, 405 rue de Vandoeuvre, F-54602 Villers-lès-Nancy, FranceSRSMC, UMR CNRS-Université de Lorraine 7565, Campus Victor Grignard, Faculté des Sciences et Technologies, F-54506 Vandoeuvre-lès-Nancy, FranceSingle-walled carbon nanotubes (SWCNTs) were functionalized by ferrocene through ethyleneglycol chains of different lengths (FcETGn) and the functionalized SWCNTs (f-SWCNTs) were characterized by different complementary analytical techniques. In particular, high-resolution scanning electron transmission microscopy (HRSTEM) and electron energy loss spectroscopy (EELS) analyses support that the outer tubes of the carbon-nanotube bundles were covalently grafted with FcETGn groups. This result confirms that the electrocatalytic effect observed during the oxidation of the reduced form of nicotinamide adenine dinucleotide (NADH) co-factor by the f-SWCNTs is due to the presence of grafted ferrocene derivatives playing the role of a mediator. This work clearly proves that residual impurities present in our SWCNT sample (below 5 wt. %) play no role in the electrocatalytic oxidation of NADH. Moreover, molecular dynamic simulations confirm the essential role of the PEG linker in the efficiency of the bioelectrochemical device in water, due to the favorable interaction between the ETG units and water molecules that prevents π-stacking of the ferrocene unit on the surface of the CNTs. This system can be applied to biosensing, as exemplified for glucose detection. The well-controlled and well-characterized functionalization of essentially clean SWCNTs enabled us to establish the maximum level of impurity content, below which the f-SWCNT intrinsic electrochemical activity is not jeopardized.https://doi.org/10.3762/bjnano.9.257biosensingcarbon nanotubescovalent functionalizationelectrocatalysisferrocene |
collection |
DOAJ |
language |
English |
format |
Article |
sources |
DOAJ |
author |
Naoual Allali Veronika Urbanova Mathieu Etienne Xavier Devaux Martine Mallet Brigitte Vigolo Jean-Joseph Adjizian Chris P. Ewels Sven Oberg Alexander V. Soldatov Edward McRae Yves Fort Manuel Dossot Victor Mamane |
spellingShingle |
Naoual Allali Veronika Urbanova Mathieu Etienne Xavier Devaux Martine Mallet Brigitte Vigolo Jean-Joseph Adjizian Chris P. Ewels Sven Oberg Alexander V. Soldatov Edward McRae Yves Fort Manuel Dossot Victor Mamane Accurate control of the covalent functionalization of single-walled carbon nanotubes for the electro-enzymatically controlled oxidation of biomolecules Beilstein Journal of Nanotechnology biosensing carbon nanotubes covalent functionalization electrocatalysis ferrocene |
author_facet |
Naoual Allali Veronika Urbanova Mathieu Etienne Xavier Devaux Martine Mallet Brigitte Vigolo Jean-Joseph Adjizian Chris P. Ewels Sven Oberg Alexander V. Soldatov Edward McRae Yves Fort Manuel Dossot Victor Mamane |
author_sort |
Naoual Allali |
title |
Accurate control of the covalent functionalization of single-walled carbon nanotubes for the electro-enzymatically controlled oxidation of biomolecules |
title_short |
Accurate control of the covalent functionalization of single-walled carbon nanotubes for the electro-enzymatically controlled oxidation of biomolecules |
title_full |
Accurate control of the covalent functionalization of single-walled carbon nanotubes for the electro-enzymatically controlled oxidation of biomolecules |
title_fullStr |
Accurate control of the covalent functionalization of single-walled carbon nanotubes for the electro-enzymatically controlled oxidation of biomolecules |
title_full_unstemmed |
Accurate control of the covalent functionalization of single-walled carbon nanotubes for the electro-enzymatically controlled oxidation of biomolecules |
title_sort |
accurate control of the covalent functionalization of single-walled carbon nanotubes for the electro-enzymatically controlled oxidation of biomolecules |
publisher |
Beilstein-Institut |
series |
Beilstein Journal of Nanotechnology |
issn |
2190-4286 |
publishDate |
2018-10-01 |
description |
Single-walled carbon nanotubes (SWCNTs) were functionalized by ferrocene through ethyleneglycol chains of different lengths (FcETGn) and the functionalized SWCNTs (f-SWCNTs) were characterized by different complementary analytical techniques. In particular, high-resolution scanning electron transmission microscopy (HRSTEM) and electron energy loss spectroscopy (EELS) analyses support that the outer tubes of the carbon-nanotube bundles were covalently grafted with FcETGn groups. This result confirms that the electrocatalytic effect observed during the oxidation of the reduced form of nicotinamide adenine dinucleotide (NADH) co-factor by the f-SWCNTs is due to the presence of grafted ferrocene derivatives playing the role of a mediator. This work clearly proves that residual impurities present in our SWCNT sample (below 5 wt. %) play no role in the electrocatalytic oxidation of NADH. Moreover, molecular dynamic simulations confirm the essential role of the PEG linker in the efficiency of the bioelectrochemical device in water, due to the favorable interaction between the ETG units and water molecules that prevents π-stacking of the ferrocene unit on the surface of the CNTs. This system can be applied to biosensing, as exemplified for glucose detection. The well-controlled and well-characterized functionalization of essentially clean SWCNTs enabled us to establish the maximum level of impurity content, below which the f-SWCNT intrinsic electrochemical activity is not jeopardized. |
topic |
biosensing carbon nanotubes covalent functionalization electrocatalysis ferrocene |
url |
https://doi.org/10.3762/bjnano.9.257 |
work_keys_str_mv |
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