Jenkins Peter A, Boland Susan, Kavanagh Paul, Leech Dónal
School of Chemistry, National University of Ireland, Galway, University Road, Galway, Ireland.
Bioelectrochemistry. 2009 Sep;76(1-2):162-8. doi: 10.1016/j.bioelechem.2009.04.008. Epub 2009 May 5.
We are interested in investigating the applications of biocatalytic mediated reduction of oxygen by oxygenases in films on electrode surfaces, as such reactions can form the basis for biosensors or biocatalytic fuel cell development. Here we present approaches aimed at improving the stability and signal output of such films. These include selection of oxygen reducing biocatalysts which are active under physiological conditions and development of redox mediators which offer the opportunity to tailor the mediator to each enzyme. It was found that for each enzyme Melanocarpus albomyces laccase (MaL), Trametes hirsutus laccase (ThL) or bilirubin oxidase (MvBOD) it was the biocatalytic films mediated by Os(2,2'-bipyridine)(2)Cl.PVI that not only generated the highest current densities compared to Os(4,4'-dimethyl-2,2'-bipyridine)(2)Cl.PVI and Os(4,4'-dichloro-2,2'-bipyridine)(2)Cl.PVI, but also proved to be the most stable over 48 h. Under physiological conditions electrodes constructed from MvBOD generated the highest initial current densities for each of the osmium redox polymers, however these films proved to be the least stable over 48 h. Stability could be improved using surface pre-treatment.
我们有兴趣研究电极表面薄膜中氧化酶介导的生物催化还原氧的应用，因为此类反应可为生物传感器或生物催化燃料电池的开发奠定基础。在此，我们介绍旨在提高此类薄膜稳定性和信号输出的方法。这些方法包括选择在生理条件下具有活性的氧还原生物催化剂，以及开发氧化还原介质，从而有机会针对每种酶定制介质。结果发现，对于每种酶，即黑孢块菌漆酶（MaL）、糙皮侧耳漆酶（ThL）或胆红素氧化酶（MvBOD），由Os(2,2'-联吡啶)(2)Cl.PVI介导的生物催化膜不仅与Os(4,4'-二甲基-2,2'-联吡啶)(2)Cl.PVI和Os(4,4'-二氯-2,2'-联吡啶)(2)Cl.PVI相比产生了最高的电流密度，而且在48小时内被证明是最稳定的。在生理条件下，由MvBOD构建的电极在每种锇氧化还原聚合物中产生了最高的初始电流密度，然而这些膜在48小时内被证明是最不稳定的。使用表面预处理可以提高稳定性。
