Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 136, Issue 44, Pages 15473-15476Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja508647u
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Funding
- Biotechnology and Biological Sciences Research Council [BB/I026367/1, BB/J000124/1]
- Medical Research Council [U105663141]
- Engineering and Physical Sciences Research Council [EP/H00338X/2]
- Biotechnology and Biological Sciences Research Council [BB/I026367/1, BB/J000124/1] Funding Source: researchfish
- Engineering and Physical Sciences Research Council [EP/H00338X/2, 1235151] Funding Source: researchfish
- Medical Research Council [MC_U105663141] Funding Source: researchfish
- BBSRC [BB/I026367/1, BB/J000124/1] Funding Source: UKRI
- EPSRC [EP/H00338X/2] Funding Source: UKRI
- MRC [MC_U105663141] Funding Source: UKRI
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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.
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