Elucidating the Hydrolysis and Polymerization Reactions of Al3+-Solvated Molecules by Reactive Molecular Dynamics Simulation

IF 2.3 3区 化学 Q3 CHEMISTRY, PHYSICAL International Journal of Quantum Chemistry Pub Date : 2024-09-16 DOI:10.1002/qua.27483
Feng Liu, Qi Zhao, Yuguo Xia, Xiuling Jiao, Dairong Chen
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Abstract

Utilizing the reactive molecular dynamics (ReaxFF MD) simulation, we conducted a comprehensive study on the impact of basicity (OH/Al3+ ratio), concentration, and temperature on the hydrolysis and polymerization reactions of Al3+-solvated molecules. Through simulations, we analyzed the structural changes, energy fluctuations of the system, and the evolution patterns of reaction products under different parameters, which were subsequently validated by experimental data. The research results indicate that hydroxide ions in the solution directly influence the breakage of OH bonds in the coordinating water molecules of solvated aluminum ions. This, in turn, affects the number of H2O and OH ions coordinated with Al3+, leading to changes in hydrolysis products. Additionally, the number of OH ions surrounding Al3+ affects the electrostatic repulsion, making it easier for polymerization reactions to occur as the system approaches the point of zero charge. On the other hand, an increase in concentration and temperature enhances the frequency of cluster collisions, thus contributing to an increase in polymerization degree. The experimental results align closely with our simulated predictions. As the pH value increases, the particle size exhibits a trend of first increasing and then decreasing, reaching a maximum at the point of zero charge. Simultaneously, an increase in concentration also prompts an increase in particle size. The combination of these empirical results with simulations enhances the credibility and reliability of our model's predictive capabilities. This study not only expands our understanding of the relevant chemical reaction processes but also provides important theoretical support for practical applications in related fields.

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通过反应分子动力学模拟阐明 Al3+ 溶剂分子的水解和聚合反应
利用反应分子动力学(ReaxFF MD)模拟,我们全面研究了碱度(OH-/Al3+ 比)、浓度和温度对 Al3+ 溶剂分子水解和聚合反应的影响。通过模拟,我们分析了不同参数下体系的结构变化、能量波动以及反应产物的演化规律,并随后通过实验数据进行了验证。研究结果表明,溶液中的氢氧根离子直接影响溶解铝离子配位水分子中 OH 键的断裂。这反过来又会影响与 Al3+ 配位的 H2O 和 OH- 离子的数量,从而导致水解产物的变化。此外,Al3+ 周围 OH- 离子的数量也会影响静电斥力,从而在体系接近零电荷点时更容易发生聚合反应。另一方面,浓度和温度的增加会提高团簇碰撞的频率,从而有助于提高聚合度。实验结果与我们的模拟预测非常吻合。随着 pH 值的增加,粒径呈现先增大后减小的趋势,并在零电荷点达到最大值。同时,浓度的增加也会促使粒径增大。这些经验结果与模拟相结合,增强了我们模型预测能力的可信度和可靠性。这项研究不仅拓展了我们对相关化学反应过程的理解,还为相关领域的实际应用提供了重要的理论支持。
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来源期刊
International Journal of Quantum Chemistry
International Journal of Quantum Chemistry 化学-数学跨学科应用
CiteScore
4.70
自引率
4.50%
发文量
185
审稿时长
2 months
期刊介绍: Since its first formulation quantum chemistry has provided the conceptual and terminological framework necessary to understand atoms, molecules and the condensed matter. Over the past decades synergistic advances in the methodological developments, software and hardware have transformed quantum chemistry in a truly interdisciplinary science that has expanded beyond its traditional core of molecular sciences to fields as diverse as chemistry and catalysis, biophysics, nanotechnology and material science.
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