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Noncovalent Approach toward the Construction of Nanofluidic Diodes with pH-Reversible Rectifying Properties: Insights from Theory and Experiment

Pérez-Mitta, Gonzalo and Albesa, Alberto and Gilles, Facundo M. and Toimil-Molares, María Eugenia and Trautmann, Christina and Azzaroni, Omar (2017):
Noncovalent Approach toward the Construction of Nanofluidic Diodes with pH-Reversible Rectifying Properties: Insights from Theory and Experiment.
In: The Journal of Physical Chemistry C, American Chemical Society Publications, pp. 9070-9076, 121, (16), ISSN 1932-7447, DOI: 10.1021/acs.jpcc.7b01639, [Online-Edition: https://doi.org/10.1021/acs.jpcc.7b01639],
[Article]

Abstract

In this paper, the fabrication of a biomimetic nanofluidic diode whose ionic transport characteristics can be completely modulated with the proton concentration in solution is demonstrated. The fabrication procedure involves the electrostatic assembly of poly(allylamine hydrochloride) (PAH) into a track-etched conical nanochannel. A fully reversible, zwitterionic-like behavior with important implications for the supramolecular interactions of the PAH within confined spaces was observed. The experimental design constitutes a facile venue for the fabrication of functional nanofluidic devices and paves the way for a number of applications in nanofluidics and biosensing. Furthermore, in order to explain the experimental results and to obtain physicochemical information about the system, theoretical modeling using a continuous model based on Poisson–Nernst–Planck equations and a stochastic model using Monte Carlo simulations were performed. Good agreement between experiments and theory was found.

Item Type: Article
Erschienen: 2017
Creators: Pérez-Mitta, Gonzalo and Albesa, Alberto and Gilles, Facundo M. and Toimil-Molares, María Eugenia and Trautmann, Christina and Azzaroni, Omar
Title: Noncovalent Approach toward the Construction of Nanofluidic Diodes with pH-Reversible Rectifying Properties: Insights from Theory and Experiment
Language: English
Abstract:

In this paper, the fabrication of a biomimetic nanofluidic diode whose ionic transport characteristics can be completely modulated with the proton concentration in solution is demonstrated. The fabrication procedure involves the electrostatic assembly of poly(allylamine hydrochloride) (PAH) into a track-etched conical nanochannel. A fully reversible, zwitterionic-like behavior with important implications for the supramolecular interactions of the PAH within confined spaces was observed. The experimental design constitutes a facile venue for the fabrication of functional nanofluidic devices and paves the way for a number of applications in nanofluidics and biosensing. Furthermore, in order to explain the experimental results and to obtain physicochemical information about the system, theoretical modeling using a continuous model based on Poisson–Nernst–Planck equations and a stochastic model using Monte Carlo simulations were performed. Good agreement between experiments and theory was found.

Journal or Publication Title: The Journal of Physical Chemistry C
Volume: 121
Number: 16
Publisher: American Chemical Society Publications
Divisions: 11 Department of Materials and Earth Sciences > Material Science > Ion-Beam-Modified Materials
11 Department of Materials and Earth Sciences > Material Science
11 Department of Materials and Earth Sciences
Date Deposited: 29 Dec 2017 10:16
DOI: 10.1021/acs.jpcc.7b01639
Official URL: https://doi.org/10.1021/acs.jpcc.7b01639
Funders: We acknowledge financial support from ANPCyT (PICT 2010-2554, PICT-2013-0905 and PPL 2011-003) and from the Deutsche Forschungsgemeinschaft (DFG-FOR 1583)., M.E.T.-M and C.T. acknowledge support by the LOEWE project iNAPO funded by the Hessen State Ministry of Higher Education, Research and Arts. G.P.-M. and F.M.G. acknowledge CONICET for a doctoral fellowship.
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