Reversible and Selective Interconversion of Hydrogen and Carbon Dioxide into Formate by a Semiartificial Formate Hydrogenlyase Mimic.
Reversible and Selective Interconversion of Hydrogen and Carbon Dioxide into Formate by a Semiartificial Formate Hydrogenlyase Mimic.
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通过半人工甲酸氢解酶模拟物将氢气和二氧化碳可逆且选择性地相互转化为甲酸。
DOI：
10.1021/jacs.9b09575
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发表时间：
2019
影响因子：
15
通讯作者：
Sokol KP
中科院分区：
文献类型：
--
作者：
Sokol KP
生物甲酸氢解酶（FHL）复合体连接甲酸脱氢酶（FDH）和氢酶（H2酶），在大肠杆菌中通过混合酸发酵从甲酸产生H2和CO2。在这里，我们描述了一个电化学和胶体半人工FHL系统，由固定在导电氧化铟锡（ITO）作为电子继电器的FDH和H2酶。这些体外系统受益于高活性酶对的有效连接，并允许甲酸在环境温度和压力下可逆转化为H2和CO2。该混合系统提供了一个模板的合成催化剂的设计和超越FHL络合物在体内储存和释放H2的需求相互转换CO2/H2和甲酸以最小的偏差在任何一个方向。
The biological formate hydrogenlyase (FHL) complex links a formate dehydrogenase (FDH) to a hydrogenase (H2ase) and produces H2and CO2from formate via mixed-acid fermentation inEscherichia coli. Here, we describe an electrochemical and a colloidal semiartificial FHL system that consists of an FDH and a H2ase immobilized on conductive indium tin oxide (ITO) as an electron relay. Thesein vitrosystems benefit from the efficient wiring of a highly active enzyme pair and allow for the reversible conversion of formate to H2and CO2under ambient temperature and pressure. The hybrid systems provide a template for the design of synthetic catalysts and surpass the FHL complexin vivoby storing and releasing H2on demand by interconverting CO2/H2and formate with minimal bias in either direction.