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

IF 2.9 3区化学 Q3 CHEMISTRY, PHYSICAL

Physical Chemistry Chemical Physics Pub Date : 2025-01-15 DOI:10.1039/D4CP03758H

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

引用次数: 0

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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溶液化学计量学对预成核FeS团簇热力学稳定性的影响

硫化铁（FeS）形成的重要性延伸到“生命起源”理论、工业应用和不必要的结垢形成。然而，FeS成核的初始阶段，特别是溶液组成的影响，仍然不清楚。通常，溶液中的铁和硫化物成分的化学计量与形成的颗粒中的不同。本研究使用从头算方法计算了含有过量Fe（II）或S（-II）的水态FeS预成核簇。结果表明，含有额外S（-II）的团簇更容易形成，这意味着在富S（-II）的环境中，与富Fe（II）的环境相比，FeS颗粒的成核速度更快。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Physical Chemistry Chemical Physics 化学-物理：原子、分子和化学物理

CiteScore

5.50

自引率

9.10%

发文量

2675

审稿时长

2.0 months

期刊介绍： Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.