Influence of solution stoichiometry on the thermodynamic stability of prenucleation FeS clusters

Vincent F.D. Peters; Janou A. Koskamp; Devis Di Tommaso; Mariette Wolthers

doi:10.1039/d4cp03758h

Influence of solution stoichiometry on the thermodynamic stability of prenucleation FeS clusters

Vincent F.D. Peters, Janou A. Koskamp, Devis Di Tommaso, Mariette Wolthers^*

^*Corresponding author for this work

Queen Mary University of London

Research output: Contribution to journal › Article › Academic › peer-review

Abstract

The significance of iron sulphide (FeS) formation extends to "origin of life" theories, industrial applications, and unwanted scale formation. However, the initial stages of FeS nucleation, particularly the impact of solution composition, remain unclear. Often, the iron and sulphide components' stoichiometry in solution differs from that in formed particles. This study uses ab initio methods to computationally examine aqueous FeS prenucleation clusters with excess Fe(II) or S(-II). The results suggest that clusters with additional S(-II) are more likely to form, implying faster nucleation of FeS particles in S(-II)-rich environments compared to Fe(II)-rich ones.

Original language	English
Pages (from-to)	3115-3123
Number of pages	9
Journal	Physical Chemistry Chemical Physics
Volume	27
Issue number	6
Early online date	20 Jan 2025
DOIs	https://doi.org/10.1039/d4cp03758h
Publication status	Published - 14 Feb 2025

Bibliographical note

Publisher Copyright:
© 2025 The Royal Society of Chemistry.

Funding

We thank A. Muthuperiyanayagam and A. Zivkovic for help with the ab initio calculations and A. Karami for discussions on FeS formation. This project has received funding to M. W., V. F. D. P., and J. A. K from the European Research Council (ERC) under the European Unions Horizon 2020 research and innovation programme (grant agreement no. 819588).

Funders	Funder number
European Research Council (ERC) under the European Unions Horizon 2020 research and innovation programme	819588

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Influence of solution stoichiometry on the thermodynamic stability of prenucleation FeS clustersFinal published version, 834 KBLicence: CC BY-NC

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abstract = "The significance of iron sulphide (FeS) formation extends to {"}origin of life{"} theories, industrial applications, and unwanted scale formation. However, the initial stages of FeS nucleation, particularly the impact of solution composition, remain unclear. Often, the iron and sulphide components' stoichiometry in solution differs from that in formed particles. This study uses ab initio methods to computationally examine aqueous FeS prenucleation clusters with excess Fe(II) or S(-II). The results suggest that clusters with additional S(-II) are more likely to form, implying faster nucleation of FeS particles in S(-II)-rich environments compared to Fe(II)-rich ones. ",

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Influence of solution stoichiometry on the thermodynamic stability of prenucleation FeS clusters

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