Laboratory of Functionalized Molecular Solids, Ministry of Education, Anhui Key Laboratory of Chemo/Biosensing, Laboratory of Optical Probes and Bioelectrocatalysis (LOPAB), College of Chemistry and Materials Science, Anhui Normal University , Wuhu 241000, P.R. China.
ACS Appl Mater Interfaces. 2017 Nov 22;9(46):40978-40986. doi: 10.1021/acsami.7b12295. Epub 2017 Nov 7.
The efficient immobilization of enzymes on favorable supporting materials to design enzyme electrodes endowed with specific catalysis performances such as deep oxidation of biofuels, and direct electron transfer (DET)-type bioelectrocatalysis is highly desired for fabricating enzymatic biofuel cells (BFCs). In this study, carbon nanodots (CNDs) have been used as the immobilizing matrixes and electron relays of enzymes to construct (NAD)-dependent dehydrogenase cascades-based bioanode for the deep oxidation of methanol and DET-type laccase-based biocathode for oxygen reduction to water. At the bioanode, multiplex enzymes including alcohol dehydrogenase, aldehyde dehydrogenase, and formate dehydrogenase are coimmobilized on CNDs electrode which is previously coated with in situ polymerized methylene blue as the electrocatalyst for oxidizing NADH to NAD. At the biocathode, fungal laccase is directly cast on CNDs and facilitated DET reaction is allowed. As a result, a novel membrane-less methanol/O BFC has been assembled and displays a high open-circuit voltage of 0.71(±0.02) V and a maximum power density of 68.7 (±0.4) μW cm. These investigated features imply that CNDs may act as new conductive architectures to elaborate enzyme electrodes for further bioelectrochemical applications.
为了设计具有特定催化性能的酶电极,如生物燃料的深度氧化和直接电子转移(DET)型生物电化学催化,将酶有效地固定在有利的支撑材料上是非常理想的,这对于制造酶生物燃料电池(BFC)至关重要。在这项研究中,碳纳米点(CND)被用作酶的固定基质和电子中继体,构建基于(NAD)依赖性脱氢酶级联的生物阳极,用于甲醇的深度氧化,以及基于 DET 型漆酶的生物阴极,用于氧还原为水。在生物阳极上,将包括醇脱氢酶、醛脱氢酶和甲酸脱氢酶在内的多种酶共固定在先前涂有原位聚合亚甲基蓝的 CNDs 电极上,作为将 NADH 氧化为 NAD 的电催化剂。在生物阴极上,真菌漆酶直接浇铸在 CNDs 上,并允许进行 DET 反应。结果,组装了一种新型无膜甲醇/O BFC,其开路电压高达 0.71(±0.02)V,最大功率密度为 68.7(±0.4)μW cm。这些研究结果表明,CND 可以作为新的导电结构来精心设计酶电极,以进一步应用于生物电化学领域。