Reversible Interconversion of CO2 and Formate by a Molybdenum-Containing Formate Dehydrogenase

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• 作者：Arnau Bassegoda ; Christopher Madden ; David W. Wakerley ; Erwin Reisner ; Judy Hirst
• 刊名：Journal of the American Chemical Society
• 出版年：2014
• 出版时间：November 5, 2014
• 年：2014
• 卷：136
• 期：44
• 页码：15473-15476
• 全文大小：247K
• ISSN：1520-5126

文摘

CO₂ and formate are rapidly, selectively, and efficiently interconverted by tungsten-containing formate dehydrogenases that surpass current synthetic catalysts. However, their mechanism of catalysis is unknown, and no tractable system is available for study. Here, we describe the catalytic properties of the molybdenum-containing formate dehydrogenase H from the model organism Escherichia coli (EcFDH-H). We use protein film voltammetry to demonstrate that EcFDH-H is a highly active, reversible electrocatalyst. In each voltammogram a single point of zero net current denotes the CO₂ reduction potential that varies with pH according to the Nernst equation. By quantifying formate production we show that electrocatalytic CO₂ reduction is specific. Our results reveal the capabilities of a Mo-containing catalyst for reversible CO₂ reduction and establish EcFDH-H as an attractive model system for mechanistic investigations and a template for the development of synthetic catalysts.