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利用掺杂氮介孔材料(NDMPC)和羧甲基壳聚糖(CMCH)机械共混的纳米复合物作为固酶载体,以滴涂-干燥法分别制备了固定漆酶(Lac)阴极和固定葡萄糖氧化酶阳极,组装了有Nafion离子交换膜的葡萄糖/O2酶燃料电池.固定漆酶电极作为燃料电池阴极和氧电化学传感器的性能以结合旋转圆盘电极技术的循环伏安法、线性扫描伏安(LSV)法以及计时电流法进行表征,同时使用紫外-可见分光光度法和石墨炉原子吸收光谱法研究酶分子在电极表面的构型和估算电极表面载体对酶的担载量.测试结果表明:固酶阴极在无电子中介体时可以实现漆酶活性中心T1与导电基体之间的直接电子迁移(表观电子迁移速率为0.013 s–1),而且具有较小的氧还原超电势(150 m V).通过进一步定量比较分子内电子传递速率(1000 s–1)、底物转化速率(0.023 s–1)以及前述酶-导电基体间电子迁移速率,可以发现此电极催化氧还原循环受制于酶-电极之间的电子迁移过程;这种电极对氧的传感性能良好:低检测限(0.04μmol dm–3)、高灵敏度(12.1μAμmol–1 dm3)和良好的对氧亲和力(KM=8.2μmol dm–3),这种固酶阴极还具有良好的重现性、长期使用性、热稳定性和pH耐受性.组装的生物燃料电池的开路电压为0.38 V,最大能量输出密度为19.2μW cm–2,最佳工作条件下使用3周后输出功率密度仍可保持初始值的60%以上.
The immobilized laccase (Lac) cathode was immobilized on the laccase-immobilized laccase using the nanocomposite mechanically doped with nitrogen-doped mesoporous materials (NDMPC) and carboxymethyl chitosan (CMCH) Glucose Oxidase Anode with Glucose / O2 Enzyme Fuel Cell with Nafion Ion Exchange Membrane Immobilized Laccase Electrode as Fuel Cell Cathode and Oxygen Electrochemical Sensor Performance Cyclic voltammetry coupled with rotating disk electrode technology, linear scan Voltammetry (LSV) and chronoamperometry were used to characterize the structure of the enzyme on the surface of the electrode and UV-visible spectrophotometry and graphite furnace atomic absorption spectrometry were used to estimate the amount of enzyme supported on the electrode surface. The results showed that the direct electron transport (apparent electron transport rate of 0.013 s-1) between laccase active center T1 and the conductive matrix could be achieved in the absence of the electron mediator by the enzyme-immobilized cathode, and had a smaller oxygen reduction potential (150 mV) .Through further quantitative comparison of intramolecular electron transfer rate (1000 s-1), substrate conversion rate (0.023 s-1) and the above electron transfer rate between the enzyme and the conductive matrix, The catalytic oxygen reduction cycle is governed by the electron-transport between the enzyme and the electrode; this electrode has good oxygen sensing performance: low detection limit (0.04 μmol dm-3), high sensitivity (12.1 μA μmol-1 dm3) and good The enzyme-immobilized cathode has also good reproducibility, long-term use, thermal stability and pH tolerance for oxygen affinity (KM = 8.2 μmol dm-3). The assembled biofuel cell has an open circuit voltage of 0.38 V , The maximum energy output density of 19.2μW cm-2, the best working conditions for 3 weeks after the output power density can still maintain the initial value of more than 60%.