Iron-Sulfur Clusters

We are motivated to prepare new iron-sulfur clusters, because these are important biological cofactors that can perform amazing reactions like N2 and CO2 reduction, and because they have unusual electronic structures that are a challenge to modern chemistry. In our work, we have prepared numerous unusual clusters and a few of them are shown below.

A current topic of research is iron-nickel-sulfur clusters, which are motivated by the active site of CO dehydrogenase, an enzyme that efficiently interconverts CO2 and CO. We are exploring the feasibility of unprecedented metal geometries and oxidation states, with the goal of understanding what is possible in the natural system.

Relevant Publications

Majed S. Fataftah, Daniel W. N. Wilson, Zachary Mathe, Theodore J. Gerard, Brandon Q. Mercado, Serena DeBeer, Patrick L. Holland
Inserting Three-Coordinate Nickel into [4Fe-4S] Clusters
ACS Cent. Sci.  202410, 1910-1919.  
Samuel H. Newman-Stonebraker, Theodore J. Gerard, Patrick L. Holland
Opportunities for insight into the mechanism of efficient CO2/CO interconversion at a nickel-iron cluster in CO dehydrogenase
Chem  202410, 1655-1667.  
Daniel W. N. Wilson, Majed S. Fataftah, Zachary Mathe, Brandon Q. Mercado, Serena DeBeer, Patrick L. Holland
Three-Coordinate Nickel and Metal-Metal Interactions in a Heterometallic Iron-Sulfur Cluster
J. Am. Chem. Soc.  2024146, 4013–4025.  
Daniel E. DeRosha, Vijay G. Chilkuri, Casey Van Stappen, Eckhard Bill, Brandon Q. Mercado, Serena DeBeer, Frank Neese, Patrick L. Holland
Planar three-coordinate iron sulfide in a synthetic [4Fe-3S] cluster with biomimetic reactivity  
Nature Chem.  201911, 1019-1025.  
Daniel E. DeRosha, Nicholas A. Arnet, Brandon Q. Mercado, and Patrick L. Holland
A [2Fe-1S] Complex that Affords Access to Bimetallic and Higher Nuclearity Iron-Sulfur Clusters
Inorg. Chem.  201958, 8829-8834.  
Wenwen Yao, Prabhuodeyara M. Gurubasavaraj, Patrick L. Holland
All-Ferrous Iron-Sulfur Clusters
Struct. Bonding  2014160, 1-37.