利用偏置MACE加速MD模拟阐明水溶液中Preyssler阴离子的离子捕获与传输机制
Elucidating Ion Capture and Transport Mechanisms of Preyssler Anions in Aqueous Solutions Using Biased MACE-Accelerated MD Simulations
AI总结：
本研究利用平衡和偏置MACE加速MD模拟，揭示了Preyssler阴离子的离子捕获与传输机制，发现受限水显著调节离子相互作用并改变传输自由能景观，为调节多金属氧酸盐的离子交换与传输提供了可行途径。
摘要：
在水溶液中进行了平衡和偏置MACE加速MD模拟，以研究{P5W30} Preyssler阴离子（PA）的离子捕获与传输机制，该阴离子是具有内部空腔的扩展型多金属氧酸盐（POM）家族中最小的代表性成员。使用平衡MACE MD模拟对两种代表性的Na(H2O)@PA和Na@PA复合物进行了仔细研究，深入探讨了PA内部空腔与外部之间存在的独特原子间相互作用。我们对径向分布函数和配位数的仔细分析表明，Na(H2O)@PA中受限水的存在对包封离子与PA空腔氧原子之间的相互作用性质具有深刻的调节作用。使用充分收敛的MACE加速多重行走器良好调谐元动力学模拟，针对作为海水和盐溶液中最丰富且具代表性的离子之一的Na+，仔细研究了两种不同的缔合和解离离子传输机制。通过比较含与不含受限水的系统，发现Na(H2O)@PA中仅存在一个预包封受限水就会显著改变离子传输过程的自由能景观。研究还发现，PA中两个窗口的收缩和扩张直接影响Na+和H2O的传输。这项工作的结果具有指导意义，因为它们展示了一条可行的途径，用于调节POM分子簇及其框架在水溶液中的离子交换与传输现象。
英文摘要：
Equilibrium and biased MACE accelerated MD simulations in aqueous solutions are performed to investigate the ion capture and transport mechanisms of the {P5W30} Preyssler anion (PA) as the smallest representative member of the extended polyoxometalate (POM) family with an internal cavity. The unique interatomic interactions present in the internal cavity vs. exterior of PA are carefully investigated using equilibrium MACE MD simulations for two representative Na(H2O)@PA and Na@PA complexes. Our careful analyses of radial distribution functions and coordination numbers show that the presence of confined water in Na(H2O)@PA has profound modulating effects on the nature of the interactions of the encapsulated ion with the oxygens of the PA cavity. Using well-converged MACE-accelerated multiple walker well-tempered metadynamics simulations, two different associative and dissociative ion transport mechanisms were carefully investigated for Na+ as one of the most abundant and representative ions present in seawater and saline solutions. By comparing systems with and without confined water, it was found that the presence of only one pre-encapsulated confined water in Na(H2O)@PA dramatically changes the free energy landscape of ion transport processes. It was also found that the contraction and dilation of the two windows present in PA directly influence the Na+ and H2O transport. Results from this work are helpful as they show a viable path toward tuning the ion exchange and transport phenomena in aqueous solutions of POM molecular clusters and frameworks.
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