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首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Reversible interconversion of carbon dioxide and formate by an electroactive enzyme
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Reversible interconversion of carbon dioxide and formate by an electroactive enzyme

机译：电活性酶可逆转化二氧化碳和甲酸

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Carbon dioxide (CO_2) is a kinetically and thermodynamically stable molecule. It is easily formed by the oxidation of organic molecules, during combustion or respiration, but is difficult to reduce. The production of reduced carbon compounds from CO_2 is an attractive proposition, because carbon-neutral energy sources could be used to generate fuel resources and sequester CO_2 from the atmosphere. However, available methods for the electrochemical reduction of CO_2 require excessive overpotentials (are energetically wasteful) and produce mixtures of products. Here, we show that a tungsten-containing formate dehydrogenase enzyme (FDH1) adsorbed to an electrode surface catalyzes the efficient electrochemical reduction of CO_2 to formate. Electrocatalysis by FDH1 is thermodynamically reversible-only small overpotentials are required, and the point of zero net catalytic current defines the reduction potential. It occurs under thoroughly mild conditions, and formate is the only product. Both as a homogeneous catalyst and on the electrode, FDH1 catalyzes CO_2 reduction with a rate more than two orders of magnitude faster than that of any known catalyst for the same reaction. Formate oxidation is more than five times faster than CO_2 reduction. Thermodynamically, formate and hydrogen are oxidized at similar potentials, so formate is a viable energy source in its own right as well as an industrially important feedstock and a stable intermediate in the conversion of CO_2 to methanol and methane. FDH1 demonstrates the feasibility of interconverting CO_2 and formate electrochemically, and it is a template for the development of robust synthetic catalysts suitable for practical applications.
机译：二氧化碳（CO_2）是一种动力学和热力学稳定的分子。它在燃烧或呼吸过程中很容易通过有机分子的氧化而形成，但很难还原。由CO_2生产还原碳化合物是一个有吸引力的提议，因为碳中性能源可用于产生燃料资源并从大气中隔离CO_2。然而，用于电化学还原CO 2的可用方法需要过度的过电势（在能量上是浪费的）并产生产物的混合物。在这里，我们表明吸附到电极表面的含钨甲酸脱氢酶（FDH1）催化了CO_2高效甲酸还原成甲酸。 FDH1的电催化是热力学可逆的，仅需要很小的超电势，并且零净催化电流的点定义了还原电势。它在完全温和的条件下发生，甲酸是唯一的产物。无论是作为均相催化剂还是在电极上，FDH1催化的CO_2还原速度均比相同反应中任何已知催化剂的还原速度快两个数量级。甲酸酯氧化比CO_2还原快五倍以上。在热力学上，甲酸和氢以相似的电势被氧化，因此甲酸本身就是一种可行的能源，同时也是工业上重要的原料，也是将CO_2转化为甲醇和甲烷的稳定中间体。 FDH1证明了电化学转化CO_2和甲酸的可行性，并且它是开发适用于实际应用的坚固合成催化剂的模板。

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