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A redox hydrogel protects hydrogenase from high-potential deactivation and oxygen damage

Hydrogenases are nature's efficient catalysts for both the generation of energy via oxidation of molecular ​hydrogen and the production of ​hydrogen via the reduction of protons. However, their ​O2sensitivity and deactivation at high potential limit their applications in practical devices, such as fuel cells. Here, we show that the integration of an ​O2-sensitive hydrogenase into a specifically designed viologen-based redox polymer protects the enzyme from ​O2 damage and high-potential deactivation. Electron transfer between the polymer-bound viologen moieties controls the potential applied to the active site of the hydrogenase and thus insulates the enzyme from excessive oxidative stress. Under catalytic turnover, electrons provided from the ​hydrogen oxidation reaction induce viologen-catalysed ​O2 reduction at the polymer surface, thus providing self-activated protection from ​O2. The advantages of this tandem protection are demonstrated using a single-compartment biofuel cell based on an ​O2-sensitive hydrogenase and ​H2/​O2 mixed feed under anode-limiting conditions.



http://www.nature.com/nchem/journal/v6/n9/full/nchem.2022.html

Nature Chemistry 6, 822–827 (2014) doi:10.1038/nchem.2022
发布日期:2014/09/01 发布者: 点击数: