Design of an Os Complex-Modified Hydrogel with Optimized Redox Potential for Biosensors and Biofuel Cells

作者：Pinyou Piyanut; Ruff Adrian; Poeller Sascha; Ma Su; Ludwig Roland; Schuhmann Wolfgang

来源：Chemistry - A European Journal, 2016, 22(15): 5319-5326.

DOI：10.1002/chem.201504591

• biosensors
• hydrogel
• osmium
• polymers
• redox chemistry

Multistep synthesis and electrochemical characterization of an Os complex-modified redox hydrogel exhibiting a redox potential approximate to+30mV (vs. Ag/AgCl 3m KCl) is demonstrated. The careful selection of bipyridine-based ligands bearing N,N-dimethylamino moieties and an amino-linker for the covalent attachment to the polymer backbone ensures the formation of a stable redox polymer with an envisaged redox potential close to 0V. Most importantly, the formation of an octahedral N6-coordination sphere around the Os central atoms provides improved stability concomitantly with the low formal potential, a low reorganization energy during the Os3+/2+ redox conversion and a negligible impact on oxygen reduction. By wiring a variety of enzymes such as pyrroloquinoline quinone (PQQ)-dependent glucose dehydrogenase, flavin adenine dinucleotide (FAD)-dependent glucose dehydrogenase and the FAD-dependent dehydrogenase domain of cellobiose dehydrogenase, low-potential glucose biosensors could be obtained with negligible co-oxidation of common interfering compounds such as uric acid or ascorbic acid. In combination with a bilirubin oxidase-based biocathode, enzymatic biofuel cells with open-circuit voltages of up to 0.54V were obtained.

• 出版日期2016-4-4