Fundamental Studies of the Construction of Biocatalyst-Based Super-Bio-Fuel Cells

生物电化学燃料电池是一种利用生物催化剂代替金属催化剂（pt）的新型燃料电池系统。我们首次证明了胆红素氧化酶是一种很有前途的酶催化剂，可以在中性pH下与介质化合物进行生物阴极反应，实现双氧四电子还原为水。我们还发现胆红素氧化酶直接接受来自几种碳电极的电子，产生相当大的阴极电流，将氧还原为水。2)首次构建了以胆红素氧化酶和普通脱硫弧菌细胞为生物催化剂，在生理pH下工作的基于生物电催化的二氢/二氧燃料电池。3)分别以pqq依赖性葡萄糖脱氢酶和脱氢酶为催化剂的生物阳极反应，成功地与以胆红素氧化酶为基础的生物阴极反应相结合，构建了葡萄糖和nadh的生物燃料电池。4)提出了一种新的制氢系统，该系统使用葡萄糖或乙醇等催化试剂进行电解制氢。当普通脱硫弧菌在生物阴极催化质子电催化还原与葡萄糖脱氢酶在生物阳极催化葡萄糖氧化相结合时，可以以很小的过电位实现氢的电解生产。5)利用蓝藻和产水氧化酶的光合生物电化学电池通过阳极室的照明产生光电流。这是一种理想的光电池，依靠简单的化学反应：2H_2+O_2=2H2O。但是，生物催化剂的稳定性和光能转化效率低等问题仍然存在。

Basic researches have been done of a bioelectrochemical fuel cells, which is a new fuel cell system utilizing biocatalysts in place of metal catalysts such as Pt.1)We have first demonstrated that bilirubin oxidase is a promising enzyme catalyst to achieve four electron reductions of dioxygen to water at neutral pH in the biocathode reaction with a mediator compound. We have also discovered that bilirubin oxidase directly accept electrons from several kinds of carbon electrodes to produce cathodic current of significan magnitude for the reduction of oxygen to water.2)We have for the first time constructed a bioelectrocatalysis-based dihydrogen/dioxygen fuel cell operating at physiological pH, in which bilirubin oxidase enzyme and desulfovibrio vulgaris bacterial cells are used as biocatalysts.3)Bio-anode reactions using PQQ-dependent glucose dehydrogenase and diaphorase as catalysts, respectively, have successfully combined with the bilirubin oxidase-based bio-cathode reaction to construct bio fuel cells for glucose and NADH.4)A new hydrogen production system has been proposed which uses a scarifying reagent such as glucose or ethanol in electrolytic hydrogen production. Electrolytic production of hydrogen can be achieved with very small overpotential when desulfovibrio vulgaris catalyzed electrocatalytic reduction of proton at a biocathode is combined with e.g. glucose dehydrogenase catalyzed oxidation of glucose at a bioanode.5)Photosynthetic bioelectrochemical cell utilizing cyanobacteria and water-generating oxidase produces photocurrent by the illumination of the anode compartment. This is a kind of ideal photo cell relying on the simple chemical reaction : 2H_2+O_2=2H2O. However, the stability of the biocatalysts and the low conversion efficiency of light energy remain to be serious problems.