文摘
Here, we report on a novel, versatile approach for the preparation of mediated enzyme electrodes, demonstrated using cross-linked films of glucose oxidase and a range of functionalised osmium complexes on graphite electrodes. Response of enzyme electrodes are optimised by evaluation of glucose response as a function of variation in ratios of [Os(2,2-bipyridine)2(4-aminomethyl pyridine)Cl]+ redox mediator, polyallylamine support and glucose oxidase enzyme cross-linked using a di-epoxide reagent in films on graphite. Lowering of the redox potential required to mediate glucose oxidation is achieved by synthesis of complexes using (4,4-dimethyl-2,2-bipyridine) or (4,4-dimethoxy-2,2-bipyridine) as a ligand instead of (2,2-bipyridine). Enzyme electrodes prepared using the complexes based on dimethoxy- or dimethyl-substituted bipyridines provide glucose oxidation current densities of 30 and 70?μA?cm? at 0.2 and 0.35?V applied potential compared to 120?μA?cm? at 0.45?V for the initial enzyme electrode, under pseudo-physiological conditions in 5?mM glucose, with stability of signals proving inadequate for long-term operation. Current output and stability may be improved by selection of alternate anchoring and cross-linking methodology, to provide enzyme electrodes capable for application to long-term glucose biosensors and anodes in enzymatic fuel cells. Figure Glucose enzyme electrodes for application as biosensors or anodes in enzymatic fuel cells prepared by crosslinking films of osmium complex, glucose oxidase and polymer support on graphite electrodes.