Mechanism of Ni, Fe-Containing Carbon Monoxide Dehydrogenases

Ni, Fe-containing carbon monoxide dehydrogenases (CODHs) catalyze the reversible oxidation of CO with water to CO2, two protons and 2 electrons, e.g. allowing bacteria and archaea to convert CO2 to CO, which is condensed with a methyl-cation and CoA to acetyl-CoA or conversely use CO as a source of electrons. Because CODHs require no overpotential in reducing CO2, the active site Ni, Fe-cluster of CODHs serves as a model for the design of chemical catalysts. In our project we want to (I) resolve open mecanistic questions of Ni, Fe-CODHs, like the early steps of CO and CO2 binding for which we initiate XFEL measurements. Furthermore, we want to correlate the electronic and spatial structure linking the rich spectroscopic data on CODHs to defined structure of cluster C by combining single crystal EPR spectroscopy with X-ray diffraction. We also want to (II) investigate the substrate spectrum of the new enzyme, CooS-V, gain insight into its potential physiological role by investigating the enzyme with potential substrates in-vitro, in-vivo and in-crystalllo. By extending the range of investigated enzymes, we want to gain insights not only on the structure and mechanism, but also the diversity and evolution of CODHs.

Principal investigators
Dobbek, Holger Prof. Dr. rer. nat. (Details) (Structural Biology / Biochemistry)

Participating organisational units of HU Berlin

DFG: Sachbeihilfe

Duration of project
Start date: 07/2019
End date: 06/2023

Research Areas

Last updated on 2022-07-09 at 19:09