以4-巯基苯甲酸修饰纳米金粒子作为固酶载体和导电基体构建了新型纳米结构固酶葡萄糖/O2燃料电池,其制备简单,长期使用性能稳定.利用纳米金粒子通过表面修饰基团和酶分子活性中心附近疏水结合位之间的相互作用固定葡萄糖氧化酶(GOx)和漆酶(Lac)分子,分别制备了固酶阳极—4-巯基苯甲酸功能化纳米金粒子固定葡萄糖氧化酶修饰金盘电极GOx/4-MBA@GNP/Au和固酶阴极—4-巯基苯甲酸功能化纳米金粒子固定漆酶修饰金盘电极Lac/4-MBA@GNP/Au.电化学实验结果表明,两种电极在不引入任何外加电子中介的条件下,均可以实现酶活性中心-纳米金粒子之间的直接电子迁移,而且具有较快的催化反应能力(固酶阳极和阴极的转化速率分别为1.3和0.5 s-1;催化葡萄糖氧化和氧气还原的起始电位分别为-0.23和0.76 V).评估了固酶阳极和阴极组装成的纳米结构固酶葡萄糖/O2燃料电池的能量输出性能.该燃料电池在没有Nation薄膜和阳极无N2气保护下,开路电压和最大输出能量密度分别可达0.56 V和760.0 μW/cm2,使用一周后输出能量密度仍然可以达到最初值的～88％.进一步测试结果显示,该燃料电池呈现出与游离漆酶类似的pH依赖关系和热稳定性,这些实验结果均暗示:影响整个酶燃料电池性能的关键在于漆酶基阴极催化氧还原的过程.此外,这种燃料电池的性能虽然受到共存干扰物抗坏血酸的影响,但在人类血清中测试结果显示其仍然具有较高的输出能量密度(132.0 μW/cm2,开路电压0.40V).本文研究结果给出了设计高性能葡萄糖/O2燃料电池的新思路,同时也为研究固酶燃料电池的构效关系提供了实验依据和有价值的启示.
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