Enzyme Containing Redox Polymer Networks for Biosensors or Biofuel Cells: A Photochemical Approach
Enzyme Containing Redox Polymer Networks for Biosensors or Biofuel Cells: A Photochemical Approach
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DOI：
10.1021/la9037183
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发表时间：
2010-04-20
期刊：
影响因子：
3.9
通讯作者：
Ruehe, Juergen
中科院分区：
文献类型：
--
作者：
Bunte, Christine;Prucker, Oswald;Ruehe, Juergen
一种光化学方法产生（微结构）氧化还原水凝胶NOM纳入酶，并评估其在生物传感器和生物燃料电池应用的潜力。为此，聚（二甲基丙烯酰胺）聚合物含有电活性二茂铁部分和光反应性二苯甲酮基团的合成和沉积在电极表面上的薄膜。在用UV光短时间照射后，聚合物层交联并变得牢固地粘附到玻璃碳电极上。如果在涂覆之前将葡萄糖氧化酶混合到聚合物溶液中，则获得具有非常高的催化电流响应的葡萄糖氧化电极。研究了多价离子和蛋白质对电催化膜性能的影响。结果表明，二价HPO_（42-）与氧化还原基团之间的相互作用可显著缩短氧化还原电极的寿命，而在一价离子和还原形式的介体存在下，氧化还原电极是相当稳定的.在氧化还原聚合物网络上涂覆薄的共价连接的聚（二甲基丙烯酰胺）保护层可以大大减少蛋白质在表面上的吸附，并提高电极在生理环境中的长期稳定性。因为蛋白质吸附在未保护的表面上是生物电极失效的主要原因之一。这一方面有望有助于设计更生物稳定的传感器和燃料电池。
A photochemical approach to the generation of (microstructured) redox hydrogels NOM incorporated enzymes is presented and evaluated with respect to its potential in biosensor and biofuel cell applications. For this, poly(dimethylacrylamide) polymers containing both electroactive ferrocene moieties and photoreactive benzophenone groups are synthesized and deposited as thin films on electrode surfaces. Upon short irradiation with UV light, the polymer layer cross links and becomes firmly adhered to the glassy carbon electrodes. If glucose oxidase is mixed into the polymer solution prior to coating, then glucose-oxidizing electrodes with very high catalytic current responses are obtained. The influence of multivalent ions and proteins on the performance or the electrocatalytic films is studied. It is found that the interaction between bivalent HPO42- and the oxidized redox moieties can shorten the lifetime of the redox electrodes significantly whereas the same electrodes are quite stable in the presence of monovalent ions and the reduced form of the mediator. Coating a thin, covalently attached poly(dimethylacrylamide) protective layer onto the redox polymer networks can greatly reduce the adsorption of proteins onto the surfaces and improve the long-term stability of the electrodes in physiological environments. Because the adsorption of proteins onto unprotected surfaces is one of the major causes of bioelectrode failure. this aspect is expected to contribute to the design of more biostable sensors and fuel cells.