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Reversible interconversion of CO2 and formate by a molybdenum-containing formate dehydrogenase.


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Authors

Bassegoda, Arnau 
Madden, Christopher 
Wakerley, David W 

Abstract

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.

Description

Keywords

Carbon Dioxide, Formate Dehydrogenases, Formates, Molybdenum

Journal Title

J Am Chem Soc

Conference Name

Journal ISSN

0002-7863
1520-5126

Volume Title

136

Publisher

American Chemical Society (ACS)
Sponsorship
Biotechnology and Biological Sciences Research Council (BB/J000124/1)
Engineering and Physical Sciences Research Council (EP/H00338X/2)
Biotechnology and Biological Sciences Research Council (BB/I026367/1)
Medical Research Council (MC_U105663141)