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Reactivation of standard [NiFe]-hydrogenase and bioelectrochemical catalysis of proton reduction and hydrogen oxidation in a mediated-electron-transfer system
Bioelectrochemistry ( IF 4.8 ) Pub Date : 2018-05-05 , DOI: 10.1016/j.bioelechem.2018.05.003
Saeko Shiraiwa , Keisei So , Yu Sugimoto , Yuki Kitazumi , Osamu Shirai , Koji Nishikawa , Yoshiki Higuchi , Kenji Kano

Standard [NiFe]-hydrogenase from Desulfovibrio vulgaris Miyazaki F (DvMF-H2ase) catalyzes the uptake and production of hydrogen (H2) and is a promising biocatalyst for future energy devices. However, DvMF-H2ase experiences oxidative inactivation under oxidative stress to generate Ni-A and Ni-B states. It takes a long time to reactivate the Ni-A state by chemical reduction, whereas the Ni-B state is quickly reactivated under reducing conditions. Oxidative inhibition limits the application of DvMF-H2ase in practical devices. In this research, we constructed a mediated-electron-transfer system by co-immobilizing DvMF-H2ase and a viologen redox polymer (VP) on electrodes. The system can avoid oxidative inactivation into the Ni-B state at high electrode potentials and rapidly reactivate the Ni-A state by electrochemical reduction of VP. H2 oxidation and H+ reduction were realized by adjusting the pH from a thermodynamic viewpoint. Using carbon felt as a working-electrode material, high current densities—up to (200 ± 70) and −(100 ± 9) mA cm−3 for the H2-oxidation and H+-reduction reactions, respectively—were attained.



中文翻译:

介导电子转移系统中标准[NiFe]-加氢酶的活化和质子还原和氢氧化的生物电化学催化

宫崎骏(Desulfovibrio vulgaris Miyazaki F)的标准[NiFe]-加氢酶(Dv MF-H 2酶)催化氢(H 2)的吸收和产生,是未来能源设备的有前途的生物催化剂。但是,Dv MF-H 2酶在氧化应激下会发生氧化失活,从而产生Ni-A和Ni-B态。通过化学还原使Ni-A状态重新活化需要很长时间,而在还原条件下Ni-B状态迅速被重新活化。氧化抑制作用限制了Dv MF-H 2酶在实际设备中的应用。在这项研究中,我们通过协同作用构建了介导的电子转移系统-将Dv MF-H 2酶和紫精氧化还原聚合物(VP)固定在电极上。该系统可以避免在高电极电势下将氧化失活成Ni-B态,并通过VP的电化学还原迅速使Ni-A态再活化。从热力学的观点出发,通过调节pH来实现H 2的氧化和H +的还原。使用碳毡作为工作电极材料,可获得高电流密度-分别达到H 2-氧化和H +-还原反应的(200±70)和-(100±9)mA cm -3

更新日期:2018-05-05
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