Biomedical Sciences, Health and Society, Malmö University, 20560 Malmö, Sweden ; A.N. Bach Institute of Biochemistry, 119071 Moscow, Russia.
Division of Solid State Physics and The Nanometer Structure Consortium (nmC@LU), Lund University, 22100 Lund, Sweden.
Beilstein J Nanotechnol. 2015 Jun 22;6:1377-84. doi: 10.3762/bjnano.6.142. eCollection 2015.
Here we detail high performance, enzymatic electrodes for oxygen bio-electroreduction, which can be easily and reproducibly fabricated with industry-scale throughput. Planar and nanostructured electrodes were built on biocompatible, flexible polymer sheets, while nanoimprint lithography was used for electrode nanostructuring. To the best of our knowledge, this is one of the first reports concerning the usage of nanoimprint lithography for amperometric bioelectronic devices. The enzyme (Myrothecium verrucaria bilirubin oxidase) was immobilised on planar (control) and artificially nanostructured, gold electrodes by direct physical adsorption. The detailed electrochemical investigation of bioelectrodes was performed and the following parameters were obtained: open circuit voltage of approximately 0.75 V, and maximum bio-electrocatalytic current densities of 18 µA/cm(2) and 58 µA/cm(2) in air-saturated buffers versus 48 µA/cm(2) and 186 µA/cm(2) in oxygen-saturated buffers for planar and nanostructured electrodes, respectively. The half-deactivation times of planar and nanostructured biocathodes were measured to be 2 h and 14 h, respectively. The comparison of standard heterogeneous and bio-electrocatalytic rate constants showed that the improved bio-electrocatalytic performance of the nanostructured biocathodes compared to planar biodevices is due to the increased surface area of the nanostructured electrodes, whereas their improved operational stability is attributed to stabilisation of the enzyme inside nanocavities.
我们详细介绍了高性能、酶促氧气生物电还原电极，这些电极可以通过工业规模的高通量生产方法来轻松、可重复地制造。平面和纳米结构电极构建在生物相容性、柔性聚合物片上，同时使用纳米压印光刻技术进行电极纳米结构化处理。据我们所知，这是首次报道纳米压印光刻术在安培生物电子设备中的应用之一。酶（Myrothecium verrucaria 胆红素氧化酶）通过直接物理吸附固定在平面（对照）和人工纳米结构化的金电极上。对生物电极进行了详细的电化学研究，并获得了以下参数：开路电压约为 0.75 V，在空气饱和缓冲液中，平面和纳米结构化电极的最大生物电催化电流密度分别为 18 µA/cm(2)和 58 µA/cm(2)，在氧气饱和缓冲液中，分别为 48 µA/cm(2)和 186 µA/cm(2)。平面和纳米结构化生物阴极的半失活时间分别测量为 2 h 和 14 h。标准非均相和生物电催化速率常数的比较表明，与平面生物器件相比，纳米结构化生物阴极的改进的生物电催化性能归因于纳米结构化电极的表面积增加，而其改进的操作稳定性归因于纳米腔内部酶的稳定化。
