Properties of the tetravalent actinide series in aqueous phase from a microscopic simulation self-consistent engine.,Physical Chemistry Chemical Physics

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Properties of the tetravalent actinide series in aqueous phase from a microscopic simulation self-consistent engine.
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2020-01-14 , DOI: 10.1039/c9cp04912f
Eléonor Acher ₁ , Michel Masella , Valérie Vallet , Florent Réal

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In the context of nuclear fuel recycling and environmental issues, the understanding of the properties of radio-elements with various approaches remains a challenge regarding their dangerousness. Moreover, experimentally, some issues are also of importance; first, it is imperative to work at sufficiently high concentrations to reach the sensitivities of the analytical tools, however this condition often leads to precipitation for some of them; second, stabilizing specific oxidation states of some actinides remains a challenge, thus making it difficult to extract general trends across the actinide series. Complementary to experiments, modeling can be used to unbiasedly probe the actinide's properties in an aquatic environment and offers a predictive tool. We report the first molecular dynamics simulations based on homogeneously built force fields for the whole series of the tetravalent actinides in aqueous phase from ThIV to BkIV and including PuIV. The force fields used to model the interactions among the constituents include polarization and charge donation microscopic effects. They are built from a self-consistent iterative ab initio based engine that can be included in future developments as an element of a potential machine learning procedure devoted to generating accurate force fields. The comparison of our simulated hydrated actinide properties to available experimental data shows the model robustness and the relevance of our parameter assignment engine. Moreover, our simulated structural, dynamical and evolution of the hydration free energy data show that, apart from AmIV and CmIV, the actinide properties change progressively along the series.

中文翻译：

微观模拟自洽发动机在水相中四价act系元素的性质。

在核燃料循环利用和环境问题的背景下，以各种方法了解无线电元素的特性仍然是对其危险性的挑战。而且，从实验上讲，一些问题也很重要。首先，必须在足够高的浓度下工作以达到分析工具的灵敏度，但是这种情况通常会导致其中一些沉淀。其次，稳定某些act系元素的特定氧化态仍然是一个挑战，因此很难提取across系元素系列的总体趋势。作为实验的补充，建模可以用于在水生环境中无偏探测probe系元素的性质，并提供一种预测工具。我们报告了基于均一的力场的第一分子动力学模拟，该力场是从ThIV到BkIV以及包括PuIV的水相中整个系列的四价act系元素的。用于模拟成分之间相互作用的力场包括极化和电荷捐赠微观效应。它们是基于一个自洽的，从头开始的迭代引擎构建的，可以作为未来机器学习过程的组成部分，将其包含在未来的发展中，该过程专门用于生成精确的力场。将我们模拟的水合act系元素性质与可用的实验数据进行比较，结果表明了模型的鲁棒性和参数分配引擎的相关性。此外，我们对水合自由能数据的模拟结构，动力学和演化表明，除了AmIV和CmIV以外，

更新日期：2020-01-14

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