pH‐Switchable Bioelectrocatalysis Based on Weak Polyelectrolyte Multilayers

Weak polyelectrolytes poly(allylamine hydrochloride) (PAH) and poly(acrylic acid) (PAA) were assembled into {PAH/PAA}n layer-by-layer films on electrodes. The cyclic voltammetry (CV) response of ferrocenecarboxylic acid (Fc(COOH)) at {PAH/PAA}5 film electrodes assembled under the specific condition showed pH-sensitive “on-off” switching property. This property was further used to control the electrocatalytic oxidation of glucose by glucose oxidase (GOD) with Fc(COOH) as the electron transfer mediator, so that the pH-switchable bioelectrocatalysis could be realized. The mechanism of pH-sensitive behavior of the system was explored and believed to originate from the pH-dependent structure change of the films.

[1]  A. Turner,et al.  Ferrocene-mediated enzyme electrode for amperometric determination of glucose. , 1984, Analytical chemistry.

[2]  Itamar Willner,et al.  Magnetic control of electrocatalytic and bioelectrocatalytic processes. , 2003, Angewandte Chemie.

[3]  I. Willner,et al.  Controlling chemical reactivity at solid-solution interfaces by means of hydrophobic magnetic nanoparticles. , 2006, Langmuir : the ACS journal of surfaces and colloids.

[4]  C. Danilowicz,et al.  Effect of ionic strength on the behavior of amperometric enzyme electrodes mediated by redox hydrogels. , 1999, Analytical chemistry.

[5]  C. Barrett,et al.  Acid-base equilibria of weak polyelectrolytes in multilayer thin films , 2003 .

[6]  Zhihui Dai,et al.  Immobilization of hemoglobin on zirconium dioxide nanoparticles for preparation of a novel hydrogen peroxide biosensor. , 2004, Biosensors & bioelectronics.

[7]  Huiqin Yao,et al.  pH-switchable bioelectrocatalysis of hydrogen peroxide on layer-by-layer films assembled by concanavalin A and horseradish peroxidase with electroactive mediator in solution. , 2010, The journal of physical chemistry. B.

[8]  Naifei Hu,et al.  Dual-switchable bioelectrocatalysis synergistically controlled by pH and perchlorate concentration based on poly(4-vinylpyridine) films. , 2010, The journal of physical chemistry. B.

[9]  Evgeny Katz,et al.  Polymer Brush-Modified Electrode with Switchable and Tunable Redox Activity for Bioelectronic Applications , 2008 .

[10]  Xin Wei,et al.  Integration of enzymes and electrodes: spectroscopic and electrochemical studies of chitosan-enzyme films. , 2002, Analytical chemistry.

[11]  Katsuhiko Ariga,et al.  ASSEMBLY OF MULTICOMPONENT PROTEIN FILMS BY MEANS OF ELECTROSTATIC LAYER-BY-LAYER ADSORPTION , 1995 .

[12]  Christopher J. Barrett,et al.  pH-Dependent Loading and Release Behavior of Small Hydrophilic Molecules in Weak Polyelectrolyte Multilayer Films , 2004 .

[13]  Jian Zhou,et al.  Biochemically controlled bioelectrocatalytic interface. , 2008, Journal of the American Chemical Society.

[14]  Itamar Willner,et al.  Magneto-Switchable Bioelectrocatalysis , 2000 .

[15]  Merlin L. Bruening,et al.  Electrochemical and in Situ Ellipsometric Investigation of the Permeability and Stability of Layered Polyelectrolyte Films , 2000 .

[16]  S. Cosnier Biomolecule immobilization on electrode surfaces by entrapment or attachment to electrochemically polymerized films. A review. , 1999, Biosensors & bioelectronics.

[17]  M. Winnik,et al.  Synthesis and characterization of pyrene-labeled poly(ethylenimine) , 1998 .

[18]  Michael F. Rubner,et al.  Reversible Molecular Memory and pH-Switchable Swelling Transitions in Polyelectrolyte Multilayers , 2003 .

[19]  Gero Decher,et al.  Fuzzy Nanoassemblies: Toward Layered Polymeric Multicomposites , 1997 .

[20]  D. Glatzhofer,et al.  Effects of electrolyte and pH on the behavior of cross-linked films of ferrocene-modified poly(ethylenimine). , 2007, Langmuir : the ACS journal of surfaces and colloids.

[21]  R. Advíncula,et al.  pH-sensitive bipolar ion-permselective ultrathin films. , 2004, Journal of the American Chemical Society.

[22]  F. Caruso,et al.  Nanoporous thin films formed by salt-induced structural changes in multilayers of poly(acrylic acid) and poly(allylamine). , 2001 .

[23]  Mitsuru Akashi,et al.  Layer-by-Layer Assembly of Poly(vinyl alcohol) and Hydrophobic Polymers Based on Their Physical Adsorption on Surfaces , 2002 .

[24]  Basit Yameen,et al.  Mesoporous films and polymer brushes helping each other to modulate ionic transport in nanoconfined environments. An interesting example of synergism in functional hybrid assemblies. , 2009, Journal of the American Chemical Society.

[25]  J Wang,et al.  Screen-printable sol-gel enzyme-containing carbon inks. , 1996, Analytical chemistry.

[26]  C. Barrett,et al.  Swelling Dynamics of Multilayer Films of Weak Polyelectrolytes , 2004 .

[27]  Evgeny Katz,et al.  Biofuel cell logically controlled by antigen-antibody recognition: towards immune-regulated bioelectronic devices. , 2009, Journal of the American Chemical Society.

[28]  Huiqin Yao,et al.  pH-Sensitive "on-off" switching behavior of layer-by-layer films assembled by concanavalin A and dextran toward electroactive probes and its application in bioelectrocatalysis. , 2009, The journal of physical chemistry. B.

[29]  R. Crooks,et al.  PH-SWITCHABLE, ULTRATHIN PERMSELECTIVE MEMBRANES PREPARED FROM MULTILAYER POLYMER COMPOSITES , 1997 .

[30]  Michael F. Rubner,et al.  pH-Dependent Thickness Behavior of Sequentially Adsorbed Layers of Weak Polyelectrolytes , 2000 .

[31]  G. S. Wilson,et al.  Recent developments in faradaic bioelectrochemistry , 2000 .

[32]  Michael F. Rubner,et al.  Controlling Bilayer Composition and Surface Wettability of Sequentially Adsorbed Multilayers of Weak Polyelectrolytes , 1998 .

[33]  Shaoling Song,et al.  pH-Controllable bioelectrocatalysis based on "on-off" switching redox property of electroactive probes for spin-assembled layer-by-layer films containing branched poly(ethyleneimine). , 2010, The journal of physical chemistry. B.

[34]  Evgeny Katz,et al.  Chemical gating with nanostructured responsive polymer brushes: mixed brush versus homopolymer brush. , 2008, ACS nano.

[35]  G. Sauerbrey Verwendung von Schwingquarzen zur Wägung dünner Schichten und zur Mikrowägung , 1959 .

[36]  Jinghong Li,et al.  Composite system based on chitosan and room-temperature ionic liquid: direct electrochemistry and electrocatalysis of hemoglobin. , 2006, Biomacromolecules.

[37]  Charles R. Martin,et al.  Investigations of Potential-Dependent Fluxes of Ionic Permeates in Gold Nanotubule Membranes Prepared via the Template Method , 2001 .

[38]  N. Hu,et al.  pH-controllable bioelectrocatalysis of glucose by glucose oxidase loaded in weak polyelectrolyte layer-by-layer films with ferrocene derivative as mediator , 2010 .

[39]  Itamar Willner,et al.  Electroanalytical and Bioelectroanalytical Systems Based on Metal and Semiconductor Nanoparticles , 2004 .

[40]  C. Barrett,et al.  pH-responsive properties of multilayered poly(L-lysine)/hyaluronic acid surfaces. , 2003, Biomacromolecules.

[41]  Lei Zhai,et al.  pH-Gated Porosity Transitions of Polyelectrolyte Multilayers in Confined Geometries and Their Application as Tunable Bragg Reflectors , 2004 .

[42]  Itamar Willner,et al.  Application of a Nitrospiropyran-FAD-Reconstituted Glucose Oxidase and Charged Electron Mediators as Optobioelectronic Assemblies for the Amperometric Transduction of Recorded Optical Signals: Control of the “On”−“Off” Direction of the Photoswitch , 1997 .

[43]  C. Barrett,et al.  Swelling behavior of hyaluronic acid/polyallylamine hydrochloride multilayer films. , 2005, Biomacromolecules.

[44]  Christopher J. Barrett,et al.  Fabrication of Microporous Thin Films from Polyelectrolyte Multilayers , 2000 .

[45]  Katz,et al.  Integration of Layered Redox Proteins and Conductive Supports for Bioelectronic Applications. , 2000, Angewandte Chemie.

[46]  Allon I Hochbaum,et al.  Rational design of cytophilic and cytophobic polyelectrolyte multilayer thin films. , 2003, Biomacromolecules.

[47]  S. Armes,et al.  Stimuli-Responsive Polymer Ultrathin Films with a Binary Architecture: Combined Layer-by-Layer Polyelectrolyte and Surface-Initiated Polymerization Approach , 2008 .

[48]  Shaoling Song,et al.  "On-off" switchable bioelectrocatalysis synergistically controlled by temperature and sodium sulfate concentration based on poly(N-isopropylacrylamide) films. , 2010, The journal of physical chemistry. B.

[49]  Michael F. Rubner,et al.  Influence of the Degree of Ionization on Weak Polyelectrolyte Multilayer Assembly , 2005 .

[50]  Huiqin Yao,et al.  pH-Controllable on-off bioelectrocatalysis of bienzyme layer-by-layer films assembled by concanavalin A and glucoenzymes with an electroactive mediator. , 2010, Journal of Physical Chemistry B.

[51]  G. Sauerbrey,et al.  Use of quartz vibration for weighing thin films on a microbalance , 1959 .

[52]  Malin Eriksson,et al.  Visco-elastic and adhesive properties of adsorbed polyelectrolyte multilayers determined in situ with QCM-D and AFM measurements. , 2005, Journal of colloid and interface science.