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Abstract:

Solid state nanochannels modified with supramolecular architectures are a new and interesting class of stimuli-responsive nanofluidic element. Their fundamental understanding requires describing the behavior of soft-materials in confined geometries and its responses to changes in solution conditions. Here, a nanochannel modified with a polyelectrolyte brush is studied with a molecular theory that incorporates the conformational behavior of the polymers, electrostatic, van der Waals, and repulsive interactions coupled with the ability of the polymer segments to regulate their charge through acid-base equilibrium. The theory predicts pH-dependent ionic conductivity in excellent agreement with experimental observations. The polymer chains undergo large conformational changes triggered by variations in the outer solution environment and the conductivity of the device is shown to be controlled by the charge state of the polymer. The degree of polymer charge is largely affected by charge regulation and nanoconfinement effects. The molecular calculations show that the apparent pKa inside the pore departs from that in solution when increasing the curvature of the nanochannel. © 2010 American Chemical Society.

Registro:

Documento: Artículo
Título:Responsive polymers end-tethered in solid-state nanochannels: When nanoconfinement really matters
Autor:Tagliazucchi, M.; Azzaroni, O.; Szleifer, I.
Filiación:INQUIMAE, CONICET, Universidad de Buenos Aires, C1428EHA, Argentina
Instituto de Investigaciones Fisicoquiěmicas Teoěricas y Aplicadas (INIFTA), CONICET, Universidad Nacional de la Plata, CC 16 Suc.4, (1900) La Plata, Argentina
Department of Biomedical Engineering, Chemistry of Life Processes Institute, Northwestern University, Evanston, IL 60208, United States
Palabras clave:Acid-base equilibria; Charge regulation; Charge state; Confined geometries; Conformational behavior; Conformational change; Experimental observation; Molecular calculations; Molecular theory; Nano channels; Nanoconfinement effects; Nanoconfinements; PH-dependent; Polyelectrolyte brushes; Polymer chains; Polymer segments; Repulsive interactions; Responsive polymer; Solution conditions; Stimuli-responsive; Supramolecular architectures; Van der waals; Van der Waals forces; Polymers; nanochannel; polyelectrolyte; polymer; article; chemical interaction; conformational transition; geometry; ion conductance; nanoanalysis; nanofluidics; pH; solid state; static electricity; stimulus response; supramolecular chemistry; Electric Conductivity; Electrolytes; Hydrogen-Ion Concentration; Molecular Conformation; Nanostructures; Nanotechnology; Polyvinyls
Año:2010
Volumen:132
Número:35
Página de inicio:12404
Página de fin:12411
DOI: http://dx.doi.org/10.1021/ja104152g
Título revista:Journal of the American Chemical Society
Título revista abreviado:J. Am. Chem. Soc.
ISSN:00027863
CODEN:JACSA
CAS:Electrolytes; Polyvinyls; poly(4-vinylpyridine), 25232-41-1
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00027863_v132_n35_p12404_Tagliazucchi

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Citas:

---------- APA ----------
Tagliazucchi, M., Azzaroni, O. & Szleifer, I. (2010) . Responsive polymers end-tethered in solid-state nanochannels: When nanoconfinement really matters. Journal of the American Chemical Society, 132(35), 12404-12411.
http://dx.doi.org/10.1021/ja104152g
---------- CHICAGO ----------
Tagliazucchi, M., Azzaroni, O., Szleifer, I. "Responsive polymers end-tethered in solid-state nanochannels: When nanoconfinement really matters" . Journal of the American Chemical Society 132, no. 35 (2010) : 12404-12411.
http://dx.doi.org/10.1021/ja104152g
---------- MLA ----------
Tagliazucchi, M., Azzaroni, O., Szleifer, I. "Responsive polymers end-tethered in solid-state nanochannels: When nanoconfinement really matters" . Journal of the American Chemical Society, vol. 132, no. 35, 2010, pp. 12404-12411.
http://dx.doi.org/10.1021/ja104152g
---------- VANCOUVER ----------
Tagliazucchi, M., Azzaroni, O., Szleifer, I. Responsive polymers end-tethered in solid-state nanochannels: When nanoconfinement really matters. J. Am. Chem. Soc. 2010;132(35):12404-12411.
http://dx.doi.org/10.1021/ja104152g