Abstract
Iron–sulfur clusters serve unique roles in biochemistry, geochemistry, and renewable energy technologies. However, a full theoretical understanding of their structures and properties is still lacking. To facilitate large-scale reactive molecular dynamics simulations of iron–sulfur clusters in aqueous environments, a ReaxFF reactive force field is developed, based on an extensive set of quantum chemical calculations. This force field compares favorably with the reference calculations on gas-phase species and significantly improves on a previous ReaxFF parametrization. We employ the new potential to study the stability and reactivity of iron–sulfur clusters in explicit water with constant-temperature reactive molecular dynamics. The aqueous species exhibit a dynamic, temperature-dependent behavior, in good agreement with previous much more costly ab initio simulations.
Highlights
Iron−sulfur clusters (FexSy) are ubiquitous in nature and play important roles in biochemistry and geochemistry.[1]
To facilitate large-scale dynamic studies of iron−sulfur clusters in aqueous environments, we report on the development of a new ReaxFF reactive force field designed for FexSy clusters that are coordinated to H2O molecules
The new force field was utilized in reactive molecular dynamics simulations in explicit water to test the parametrization and to provide insights into the structure and stability of Fe−S clusters in water
Summary
Iron−sulfur clusters (FexSy) are ubiquitous in nature and play important roles in biochemistry and geochemistry.[1]. There has been a surge of interest in these systems due to their exceptional chemical properties. As such, they are emerging as novel biomimetic templates,[6] sustainable batteries,[7] and catalysts.[8] For example, a recently synthesized [4Fe−3S] planar cluster, which features an iron center with three bonds to sulfides, has been used to reduce hydrazine, a natural substrate of nitrogenase.[6] Iron−sulfur clusters are considered as leading candidates for promoting prebiotic organic synthesis on early Earth.[9] Central to the theories of the origin of life is the water environment in which the clusters undergo structural transformations,[8] act as catalytic centers for synthesis of new organic bonds,[10] and form nucleation sites for minerals such as pyrite and mackinawite.[4]
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