Supramolecular multilayer structures of wired redox enzyme electrodes

被引:33
作者
Calvo, EJ
Danilowicz, CB
Wolosiuk, A
机构
[1] Univ Buenos Aires, Fac Ciencias Exactas & Nat, Dept Quim Organ, INQUIMAE, AR-1428 Buenos Aires, DF, Argentina
[2] Harvard Univ, Dept Phys, Cambridge, MA 02138 USA
[3] Univ Illinois, Dept Mat Sci & Engn, Urbana, IL 61801 USA
关键词
D O I
10.1039/b500528k
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Supramolecular multilayer structures comprised of glucose oxidase (GOx), and Os complex derivatised poly( allylamine) (PAH-Os) have been built by alternate layer-by-layer (LBL) electrostatic adsorption in a self-assembly process. The resulting modified electrodes with integrated mediator were tested as reagentless glucose biosensors. The enzyme kinetic parameters and the surface concentration of "wired'' enzyme Gamma(E) have been obtained by analysis of the catalytic current dependence on glucose concentrations for the ping-pong mechanism of glucose oxidation. An average osmium volume concentration was estimated by integration of the redox charge in the absence of glucose and the ellipsometric thickness. The total enzyme surface concentration was measured with a quartz crystal microbalance (QCM) during each adsoption step and the fraction of "wired'' enzyme and the bimolecular rate constant for FADH(2) oxidation by the redox polymer for the different multilayers. The catalytic current increases with the number of LBL layers because the increase in the enzyme loading while the efficiency of enzyme FADH2 oxidation by the Os redox polymer, except for the first dipping cycle remains almost constant at about 2 x 10(4) M-1 s(-1).
引用
收藏
页码:1800 / 1806
页数:7
相关论文
共 55 条
[31]   Electrostatic immobilization of glucose oxidase in a weak acid, polyelectrolyte hyperbranched ultrathin film on gold: Fabrication, characterization, and enzymatic activity [J].
Franchina, JG ;
Lackowski, WM ;
Dermody, DL ;
Crooks, RM ;
Bergbreiter, DE ;
Sirkar, K ;
Russell, RJ ;
Pishko, MV .
ANALYTICAL CHEMISTRY, 1999, 71 (15) :3133-3139
[32]   REDOX POLYMER-FILMS CONTAINING ENZYMES .1. A REDOX-CONDUCTING EPOXY CEMENT - SYNTHESIS, CHARACTERIZATION, AND ELECTROCATALYTIC OXIDATION OF HYDROQUINONE [J].
GREGG, BA ;
HELLER, A .
JOURNAL OF PHYSICAL CHEMISTRY, 1991, 95 (15) :5970-5975
[33]   Use of mixed self-assembled monolayers in a study of the effect of the microenvironment on immobilized glucose oxidase [J].
Guiomar, AJ ;
Guthrie, JT ;
Evans, SD .
LANGMUIR, 1999, 15 (04) :1198-1207
[34]   CRYSTAL-STRUCTURE OF GLUCOSE-OXIDASE FROM ASPERGILLUS-NIGER REFINED AT 2 .3 ANGSTROM RESOLUTION [J].
HECHT, HJ ;
KALISZ, HM ;
HENDLE, J ;
SCHMID, RD ;
SCHOMBURG, D .
JOURNAL OF MOLECULAR BIOLOGY, 1993, 229 (01) :153-172
[35]   ELECTRICAL WIRING OF REDOX ENZYMES [J].
HELLER, A .
ACCOUNTS OF CHEMICAL RESEARCH, 1990, 23 (05) :128-134
[36]   Layer-by-layer self-assembly of glucose oxidase with a poly(allylamine)ferrocene redox mediator [J].
Hodak, J ;
Etchenique, R ;
Calvo, EJ ;
Singhal, K ;
Bartlett, PN .
LANGMUIR, 1997, 13 (10) :2708-2716
[37]   A non-compartmentalized glucose|O2 biofuel cell by bioengineered electrode surfaces [J].
Katz, E ;
Willner, I ;
Kotlyar, AB .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1999, 479 (01) :64-68
[38]   Glucose oxidase electrodes via reconstitution of the apo-enzyme:: tailoring of novel glucose biosensors [J].
Katz, E ;
Riklin, A ;
Heleg-Shabtai, V ;
Willner, I ;
Bückmann, AF .
ANALYTICA CHIMICA ACTA, 1999, 385 (1-3) :45-58
[39]   DIRECT ELECTRON-TRANSFER TO ESCHERICHIA-COLI FUMARATE REDUCTASE IN SELF-ASSEMBLED ALKANETHIOL MONOLAYERS ON GOLD ELECTRODES [J].
KINNEAR, KT ;
MONBOUQUETTE, HG .
LANGMUIR, 1993, 9 (09) :2255-2257
[40]   Kinetic control by the substrate and the cosubstrate in electrochemically monitored redox enzymatic immobilized systems.: Catalytic responses in cyclic voltammetry and steady state techniques [J].
Limoges, B ;
Moiroux, J ;
Savéant, JM .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2002, 521 (1-2) :8-15