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Comprehensive Study of the Enzymatic Catalysis of the Electrochemical Oxygen Reduction Reaction (ORR) by Immobilized Copper Efflux Oxidase (CueO) From Escherichia coli

机译:固定化大肠杆菌的铜外排氧化酶(CueO)催化酶催化电化学还原氧反应(ORR)的综合研究

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摘要

In recent years, enzymatic fuel cells have experienced a great development promoted by the availability of novel biological techniques that allow the access to a large number of enzymatic catalysts. One of the most important aspects in this area is the development of biocatalysts for the oxygen reduction reaction (ORR). Laccases from the group of enzymes called blue multi-cooper oxidases have received considerable attention because of their ability to catalyze the electrochemical oxygen reduction reaction to water when immobilized on metallic or carbonaceous electrode materials. In this paper we report a comprehensive study of the electrocatalytic activity of the enzyme Copper efflux oxidase (CueO) from Escherichia coli immobilized on different electrode materials. The influence of the electrode substrate employed for protein immobilization was evaluated using glassy carbon, gold or platinum electrodes. Gold and platinum electrodes were modified using different self-assembled monolayers (SAM) able to tune the electrostatic interaction between the protein and the substrate, depending on the nature of the terminal functional group in the SAM. The effects of protein immobilization time, electrode potential, solution pH and temperature, protein and O2 concentration have been carefully investigated. Finally, direct electron transfer (DET) was investigated in the presence of the following inhibitors: fluoride (F), chloride (Cl) and azide (N3-).
机译:近年来,酶燃料电池已经经历了巨大的发展,这是由于可获得允许使用大量酶催化剂的新型生物技术的推动。该领域最重要的方面之一是氧还原反应(ORR)的生物催化剂的开发。来自漆酶的被称为蓝色多库珀氧化酶的漆酶由于固定在金属或碳质电极材料上时具有催化水的电化学氧还原反应的能力而备受关注。在本文中,我们报告了固定在不同电极材料上的大肠杆菌铜外排氧化酶(CueO)的电催化活性的综合研究。使用玻璃碳,金或铂电极评估用于蛋白质固定的电极基材的影响。金和铂电极使用不同的自组装单分子层(SAM)进行修饰,这取决于SAM中末端官能团的性质,可调节蛋白质和底物之间的静电相互作用。仔细研究了蛋白质固定时间,电极电势,溶液pH和温度,蛋白质和O2浓度的影响。最后,在以下抑制剂的存在下研究了直接电子转移(DET):氟化物(F -),氯化物(Cl -)和叠氮化物( N 3 - )。

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