Integration of Polyaniline/Poly(acrylic acid) Films and Redox Enzymes on Electrode Supports: An in Situ Electrochemical/Surface Plasmon Resonance Study of the Bioelectrocatalyzed Oxidation of Glucose or Lactate in the Integrated Bioelectrocatalytic Systems

作者：Oleg A. Raitman, Eugenii Yu. Katz, Andreas F. Bückmann, Itamar Willner · 发表于：Journal of the American Chemical Society · 年份：2002 · DOI：10.1021/ja012680r · 被引用次数：263 · 研究领域：Conducting polymers and applications、Electrochemical sensors and biosensors、Analytical Chemistry and Sensors

Electropolymerization of aniline in the presence of poly(acrylic acid) on Au electrodes yields a polyaniline/poly(acrylic acid) composite film, exhibiting reversible redox functions in aqueous solutions at pH = 7.0. In situ electrochemical-SPR measurements are used to identify the dynamics of swelling and shrinking of the polymer film upon the oxidation of the polyaniline (PAn) to its oxidized state (PAn(2+)) and the reduction of the oxidized polymer (PAn(2+)) back to its reduced state (PAn), respectively. Covalent attachment of N(6)-(2-aminoethyl)-flavin adenin dinucleotide (amino-FAD, 1) to the carboxylic groups of the composite polyaniline/poly(acrylic acid) film followed by the reconstitution of apoglucose oxidase on the functional polymer yields an electrically contacted glucose oxidase of unprecedented electrical communication efficiency with the electrode: electron-transfer turnover rate approximately 1000 s(-1) at 30 degrees C. In situ electrochemical-SPR analyses are used to characterize the bioelectrocatalytic functions of the biomaterial-polymer interface. The current responses of the bioelectrocatalytic system increase as the glucose concentrations are elevated. Similarly, the SPR spectra of the system are controlled by the concentration of glucose. The glucose concentration controls the steady-state concentration ratio of PAn/PAn(2+) in the film composition. Therefore, the SPR spectrum of the film measured upon its electrochemical oxidation is shifted from the sp...