The HydG Enzyme Generates an Fe(CO)2(CN) Synthon in Assembly of the FeFe Hydrogenase H-Cluster
Science, 2014•science.org
Three iron-sulfur proteins–HydE, HydF, and HydG–play a key role in the synthesis of the
[2Fe] H component of the catalytic H-cluster of FeFe hydrogenase. The radical S-adenosyl-l-
methionine enzyme HydG lyses free tyrosine to produce p-cresol and the CO and CN−
ligands of the [2Fe] H cluster. Here, we applied stopped-flow Fourier transform infrared and
electron-nuclear double resonance spectroscopies to probe the formation of HydG-bound
Fe-containing species bearing CO and CN− ligands with spectroscopic signatures that …
[2Fe] H component of the catalytic H-cluster of FeFe hydrogenase. The radical S-adenosyl-l-
methionine enzyme HydG lyses free tyrosine to produce p-cresol and the CO and CN−
ligands of the [2Fe] H cluster. Here, we applied stopped-flow Fourier transform infrared and
electron-nuclear double resonance spectroscopies to probe the formation of HydG-bound
Fe-containing species bearing CO and CN− ligands with spectroscopic signatures that …
Three iron-sulfur proteins–HydE, HydF, and HydG–play a key role in the synthesis of the [2Fe]H component of the catalytic H-cluster of FeFe hydrogenase. The radical S-adenosyl-l-methionine enzyme HydG lyses free tyrosine to produce p-cresol and the CO and CN− ligands of the [2Fe]H cluster. Here, we applied stopped-flow Fourier transform infrared and electron-nuclear double resonance spectroscopies to probe the formation of HydG-bound Fe-containing species bearing CO and CN− ligands with spectroscopic signatures that evolve on the 1- to 1000-second time scale. Through study of the 13C, 15N, and 57Fe isotopologs of these intermediates and products, we identify the final HydG-bound species as an organometallic Fe(CO)2(CN) synthon that is ultimately transferred to apohydrogenase to form the [2Fe]H component of the H-cluster.
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