ArticleJournal of the American Chemical Society2026
Nickel(I) in an All-Ferric NiFeS Cluster.
Article in Journal of the American Chemical Society, 2026. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.
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5 authors.
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Abstract
Anaerobic carbon monoxide dehydrogenase (CODH) enzymes interconvert CO2 and CO under mild conditions and with near perfect selectivity. The CODH active site, termed the C-cluster, is a [NiFe3S4]-Feu cluster that can reside in several different oxidation states. Despite decades of research, the electronic structure of the C-cluster remains unresolved, and the metal oxidation states are ambiguous. In this study, we interrogate a series of synthetic clusters with [NiFe3S4]3+/2+/1+ cores in multiple oxidation states as models of the C-cluster cubane core. Each cluster is characterized using crystallography, spectroscopy, magnetism, and computations. The most oxidized cluster, [NiFe3S4]3+, is best described as having Ni2+ and three Fe3+ sites. Remarkably, X-ray absorption spectroscopy (XAS) data show that reduction to the [NiFe3S4]2+ state results in reduction of nickel to Ni1+, even though nearby Fe3+ sites are present. The fully oxidized Fe3+3 subsite can be reduced only after nickel has reached the Ni1+ state. These results demonstrate that Ni1+ is a readily accessible oxidation state in FeS clusters that are topologically relevant to the CODH C-cluster.
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