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A redox-sensitive nanofluidic diode based on nicotinamide-modified asymmetric nanopores

Ali, Mubarak and Ahmed, Ishtiaq and Ramirez, Patricio and Nasir, Saima and Mafe, Salvador and Niemeyer, Christof M. and Ensinger, Wolfgang (2017):
A redox-sensitive nanofluidic diode based on nicotinamide-modified asymmetric nanopores.
In: Sensors and Actuators B: Chemical, 240Elsevier Science Publishing, pp. 895-902, ISSN 0925-4005,
DOI: 10.1016/j.snb.2016.09.061,
[Online-Edition: https://doi.org/10.1016/j.snb.2016.09.061],
[Article]

Abstract

We demonstrate a redox-sensitive nanofluidic diode whose ion rectification is modulated by the oxidation and reduction of chemical moieties incorporated on its surface. To achieve this goal, we have first synthesized the chemical compounds 1-(4-aminobutyl)-3-carbamoylpyridin-1-ium (Nic-BuNH2) and 3-carbamoyl-1-(2,4-dinitrophenyl)pyridinium (Nic-DNP). Then, the surface of track-etched single asymmetric nanopores is decorated with the redox-sensitive Nic-BuNH2 and Nic-DNP molecules using carbodiimide coupling chemistry and Zincke reaction, respectively. The success of the modification reactions is monitored through the changes in the current-voltage (I-V) curves prior to and after pore functionalization. Upon exposing the modified pore to solutions of hydrogen peroxide (oxidizing agent) and sodium dithionite (reducing agent) the surface charge is reversibly modulated from positive to neutral, leading to measurable changes in the electronic readout of ion current passing through the nanopore. On oxidation, the quaternary nicotinamide units impart positive charge to the pore surface, resulting in the ion current rectification (anion-selective pore). On the contrary, the complementary reduced dihydronicotinamide moieties resulted in the loss of surface charge and ohmic behaviour (non-selective pore). The experimental results are further theoretically described by using Poisson-Nernst-Planck equations.

Item Type: Article
Erschienen: 2017
Creators: Ali, Mubarak and Ahmed, Ishtiaq and Ramirez, Patricio and Nasir, Saima and Mafe, Salvador and Niemeyer, Christof M. and Ensinger, Wolfgang
Title: A redox-sensitive nanofluidic diode based on nicotinamide-modified asymmetric nanopores
Language: English
Abstract:

We demonstrate a redox-sensitive nanofluidic diode whose ion rectification is modulated by the oxidation and reduction of chemical moieties incorporated on its surface. To achieve this goal, we have first synthesized the chemical compounds 1-(4-aminobutyl)-3-carbamoylpyridin-1-ium (Nic-BuNH2) and 3-carbamoyl-1-(2,4-dinitrophenyl)pyridinium (Nic-DNP). Then, the surface of track-etched single asymmetric nanopores is decorated with the redox-sensitive Nic-BuNH2 and Nic-DNP molecules using carbodiimide coupling chemistry and Zincke reaction, respectively. The success of the modification reactions is monitored through the changes in the current-voltage (I-V) curves prior to and after pore functionalization. Upon exposing the modified pore to solutions of hydrogen peroxide (oxidizing agent) and sodium dithionite (reducing agent) the surface charge is reversibly modulated from positive to neutral, leading to measurable changes in the electronic readout of ion current passing through the nanopore. On oxidation, the quaternary nicotinamide units impart positive charge to the pore surface, resulting in the ion current rectification (anion-selective pore). On the contrary, the complementary reduced dihydronicotinamide moieties resulted in the loss of surface charge and ohmic behaviour (non-selective pore). The experimental results are further theoretically described by using Poisson-Nernst-Planck equations.

Journal or Publication Title: Sensors and Actuators B: Chemical
Volume: 240
Publisher: Elsevier Science Publishing
Uncontrolled Keywords: Synthetic nanopores, Redox reaction, Nicotinamide, Current rectification, Surface functionalization, Track-etching
Divisions: 11 Department of Materials and Earth Sciences
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences > Material Science > Material Analytics
Date Deposited: 20 Sep 2016 05:42
DOI: 10.1016/j.snb.2016.09.061
Official URL: https://doi.org/10.1016/j.snb.2016.09.061
Funders: M.A., S.N. and W.E. acknowledge the funding from the Hessen State Ministry of Higher Education, Research and the Arts, Germany, under the LOEWE project iNAPO., P. R. and S. M. acknowledge financial support by the Generalitat Valenciana (Program of Excellence Prometeo/GV/0069), the Spanish Ministry of Economic Affairs and Competitiveness (MAT2015-65011-P), and FEDER., I.A. and C.M.N. acknowledge financial support through the Helmholtz programme BioInterfaces in Technology and Medicine.
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