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

Ali, Mubarak ; Ahmed, Ishtiaq ; Ramirez, Patricio ; Nasir, Saima ; Mafe, Salvador ; Niemeyer, Christof M. ; Ensinger, Wolfgang :
A redox-sensitive nanofluidic diode based on nicotinamide-modified asymmetric nanopores.
[Online-Edition: https://doi.org/10.1016/j.snb.2016.09.061]
In: Sensors and Actuators B: Chemical, 240 pp. 895-902. ISSN 09254005
[Artikel], (2017)

Offizielle URL: https://doi.org/10.1016/j.snb.2016.09.061

Kurzbeschreibung (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.

Typ des Eintrags: Artikel
Erschienen: 2017
Autor(en): Ali, Mubarak ; Ahmed, Ishtiaq ; Ramirez, Patricio ; Nasir, Saima ; Mafe, Salvador ; Niemeyer, Christof M. ; Ensinger, Wolfgang
Titel: A redox-sensitive nanofluidic diode based on nicotinamide-modified asymmetric nanopores
Sprache: Englisch
Kurzbeschreibung (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.

Titel der Zeitschrift, Zeitung oder Schriftenreihe: Sensors and Actuators B: Chemical
Band: 240
Verlag: Elsevier Science Publishing
Freie Schlagworte: Synthetic nanopores, Redox reaction, Nicotinamide, Current rectification, Surface functionalization, Track-etching
Fachbereich(e)/-gebiet(e): 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft > Fachgebiet Materialanalytik
11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft
11 Fachbereich Material- und Geowissenschaften
Hinterlegungsdatum: 11 Jul 2017 11:55
Offizielle URL: https://doi.org/10.1016/j.snb.2016.09.061
ID-Nummer: doi:10.1016/j.snb.2016.09.061
Sponsoren: 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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