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Issue 40, 2012
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Morphogen-driven self-construction of covalent films built from polyelectrolytes and homobifunctional spacers: buildup and pH response

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Abstract

Self-construction of films using polyelectrolytes bearing complementary chemical groups is a recent emerging concept in the coating field. Herein, we describe the one-pot morphogen film self-construction through formation of covalent bonds between polyelectrolytes and homobifunctional spacers by Huisgen click-chemistry. One-pot solution of poly(acrylic acid) bearing alkyne groups (PAA-Alk), bisazides ethylene glycol (Az-EGn-Az) spacers and CuSO4 was brought into contact with a gold electrode. Cu(I), the morphogen, was generated electrochemically from Cu(II) at the electrode/one-pot solution interface. The PAA-Alk/Az-EGn-Az film buildup was investigated by varying the length of the EGn spacer (n = 2, 13 and 50) leading to different growth rates. By increasing the pH of the solution, a reversible swelling of the films (up to 400% for n = 13 or 50) is obtained due to electrostatic repulsion between PAA chains. Further investigations on film swelling were performed by using PAA-Alk and an original bisazide spacer based on two pyrene units connected by a triamine spacer (Az-bispyrene-Az). This spacer has the property to adopt an extended conformation under acidic conditions and a “stacked” conformation under basic conditions, which both can be monitored by fluorimetry. Despite the mechanical tension due to film swelling at basic pH, bispyrene spacers adopt a stacked conformation. This allowed us to monitor the pH within PAA-Alk/Az-bispyrene-Az films. The pH remains fairly stable and below the pKa of PAA when the pH of the contacting solution varies from pH 5 to pH 7 and increases above pH 8, which explains why film swelling takes place essentially above pH 8.

Graphical abstract: Morphogen-driven self-construction of covalent films built from polyelectrolytes and homobifunctional spacers: buildup and pH response

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Supplementary files

Article information


Submitted
01 Jun 2012
Accepted
03 Aug 2012
First published
24 Aug 2012

Soft Matter, 2012,8, 10336-10343
Article type
Paper

Morphogen-driven self-construction of covalent films built from polyelectrolytes and homobifunctional spacers: buildup and pH response

G. Rydzek, P. Polavarapu, C. Rios, J. Tisserant, J. Voegel, B. Senger, P. Lavalle, B. Frisch, P. Schaaf, F. Boulmedais and L. Jierry, Soft Matter, 2012, 8, 10336
DOI: 10.1039/C2SM26272J

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