title: Film Self-Assembly of Oppositely Charged Macromolecules Triggered by Electrochemistry through a Morphogenic Approach.
abstract: The development of new surface functionalization methods that are easy to use, versatile, and allow local deposition represents a real scientific challenge. Overcoming this challenge, we present here a one-pot process that consists in self-assembling, by electrochemistry on an electrode, films made of oppositely charged macromolecules. This method relies on a charge-shifting polyanion, dimethylmaleic-modified poly(allylamine) (PAHd), that undergoes hydrolysis at acidic pH, leading to an overall switching of its charge. When a mixture of the two polyanions, PAHd and poly(styrenesulfonate) (PSS), is placed in contact with an electrode, where the pH is decreased locally by electrochemistry, the transformation of PAHd into a polycation (PAH) leads to the continuous self-assembly of a nanometric PAH/PSS film by electrostatic interactions. The pH decrease is obtained by the electrochemical oxidation of hydroquinone, which produces protons locally over nanometric distances. Using a negatively charged enzyme, alkaline phosphatase (AP), instead of PSS, this one-pot process allows the creation of enzymatically active films. Under mild conditions, self-assembled PAH/AP films have an enzymatic activity which is adjustable simply by controlling the self-assembly time. The selective functionalization of microelectrode arrays by PAH/AP was achieved, opening the route toward miniaturized biosensors.
authors: Institut Charles Sadron , UPR 22, Centre National de la Recherche Scientifique, Strasbourg, France.
authors: Alexandre
authors: A
authors: Dochter
authors: Institut Charles Sadron , UPR 22, Centre National de la Recherche Scientifique, Strasbourg, France.
authors: Tony
authors: T
authors: Garnier
authors: Institut Charles Sadron , UPR 22, Centre National de la Recherche Scientifique, Strasbourg, France.
authors: Elodie
authors: E
authors: Pardieu
authors: Institut Charles Sadron , UPR 22, Centre National de la Recherche Scientifique, Strasbourg, France.
authors: Nguyet Trang Thanh
authors: NT
authors: Chau
authors: Institut Charles Sadron , UPR 22, Centre National de la Recherche Scientifique, Strasbourg, France.
authors: Clément
authors: C
authors: Maerten
authors: Institut National de la Santé et de la Recherche Médicale , Unité 1121, Strasbourg, France.|Faculté de Chirurgie Dentaire, Université de Strasbourg , Strasbourg, France.
authors: Bernard
authors: B
authors: Senger
authors: Institut Charles Sadron , UPR 22, Centre National de la Recherche Scientifique, Strasbourg, France.|Institut National de la Santé et de la Recherche Médicale , Unité 1121, Strasbourg, France.|Faculté de Chirurgie Dentaire, Université de Strasbourg , Strasbourg, France.|International Center for Frontier Research in Chemistry, Strasbourg, France.|Ecole Européenne de Chimie, Polymères et Matériaux de Strasbourg, Université de Strasbourg , Strasbourg, France.|Institut Universitaire de France , Paris, France.
authors: Pierre
authors: P
authors: Schaaf
authors: Institut Charles Sadron , UPR 22, Centre National de la Recherche Scientifique, Strasbourg, France.|International Center for Frontier Research in Chemistry, Strasbourg, France.|Ecole Européenne de Chimie, Polymères et Matériaux de Strasbourg, Université de Strasbourg , Strasbourg, France.|University of Strasbourg Institute for Advanced Study (USIAS) , Strasbourg, France.
authors: Loïc
authors: L
authors: Jierry
authors: Institut Charles Sadron , UPR 22, Centre National de la Recherche Scientifique, Strasbourg, France.|International Center for Frontier Research in Chemistry, Strasbourg, France.|University of Strasbourg Institute for Advanced Study (USIAS) , Strasbourg, France.
authors: Fouzia
authors: F
authors: Boulmedais
mesh_terms: D000499:Allylamine / Q000737:chemistry; D015374:Biosensing Techniques / Q000379:methods; D002384:Catalysis; D004563:Electrochemistry / Q000379:methods*; D004566:Electrodes; D011073:Polyamines / Q000737:chemistry; D000071228:Polyelectrolytes; D011108:Polymers / Q000737:chemistry; D011137:Polystyrenes / Q000737:chemistry
chemical_list: D000499:Allylamine; D011073:Polyamines; D000071228:Polyelectrolytes; D011108:Polymers; D011137:Polystyrenes; C003321:polystyrene sulfonic acid