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ReportsCarbon Dioxide Activation at the Ni,Fe-Cluster of Anaerobic Carbon Monoxide DehydrogenaseAnaerobic CO dehydrogenases catalyze the reversible oxidation of CO to CO2 at a complex Ni-, Fe-, and S-containing metal center called cluster C. We report crystal structures of CO dehydrogenase II from Carboxydothermus hydrogenoformans in three different states. In a reduced state, exogenous CO2 supplied in solution is bound and reductively activated by cluster C. In the intermediate structure, CO2 acts as a bridging ligand between Ni and the asymmetrically coordinated Fe, where it completes the square-planar coordination of the Ni ion. It replaces a water/hydroxo ligand bound to the Fe ion in the other two states. The structures define the mechanism of CO oxidation and CO2 reduction at the Ni-Fe site of cluster C. Laboratorium Proteinkristallographie and Forschungszentrum für Bio-Makromoleküle, Universität Bayreuth, D-95440 Bayreuth, Germany. * To whom correspondence should be addressed. E-mail: holger.dobbek{at}uni-bayreuth.de
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Science. ISSN 0036-8075 (print), 1095-9203 (online)
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