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arXiv 2602.23142cs.LG
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二元混合物中扩散系数预测的张量补全方法

Prediction of Diffusion Coefficients in Mixtures with Tensor Completion

Laboratory of Engineering Thermodynamics, RPTU Kaiserslautern(工程热力学实验室,科隆大学)

Zeno Romero, Kerstin Münnemann, Hans Hasse, Fabian Jirasek

AI总结:

本文提出一种混合张量补全方法,用于预测二元混合物中无限稀释温度依赖的扩散系数,结合实验数据和贝叶斯框架提升预测精度。

摘要:

预测混合物中的扩散系数对于许多应用至关重要,因为实验数据仍然稀缺,而机器学习(ML)提供了有前景的替代方案。在ML模型中,矩阵补全方法(MCMs)已被证明在预测热物理性质,包括二元混合物中的扩散系数方面是有效的。然而,MCMs仅限于单温度预测,其准确性强烈依赖于每个感兴趣的温度的高质量实验数据的可用性。在本工作中,我们通过提出一种混合张量补全方法(TCM)来解决这一挑战,用于预测二元混合物中无限稀释温度依赖的扩散系数。TCM采用Tucker分解,并在298 K、313 K和333 K的二元系统中无限稀释扩散系数的实验数据上联合训练。半经验SEGWE模型的预测作为贝叶斯训练框架中的先验知识。TCM然后线性外推到268 K到378 K之间的任何温度,其预测精度显著优于现有模型。为了进一步提高预测性能,实验数据库通过主动学习(AL)策略扩展,通过脉冲场梯度(PFG)NMR测量获取新的扩散数据。在298 K、313 K和333 K下测量了19种溶质+溶剂系统的无限稀释扩散系数。将这些结果纳入TCM中,显著提高了其预测精度。这些发现突显了结合数据高效ML方法与自适应实验来推进传输性质预测模型的潜力。

英文摘要:

Predicting diffusion coefficients in mixtures is crucial for many applications, as experimental data remain scarce, and machine learning (ML) offers promising alternatives to established semi-empirical models. Among ML models, matrix completion methods (MCMs) have proven effective in predicting thermophysical properties, including diffusion coefficients in binary mixtures. However, MCMs are restricted to single-temperature predictions, and their accuracy depends strongly on the availability of high-quality experimental data for each temperature of interest. In this work, we address this challenge by presenting a hybrid tensor completion method (TCM) for predicting temperature-dependent diffusion coefficients at infinite dilution in binary mixtures. The TCM employs a Tucker decomposition and is jointly trained on experimental data for diffusion coefficients at infinite dilution in binary systems at 298 K, 313 K, and 333 K. Predictions from the semi-empirical SEGWE model serve as prior knowledge within a Bayesian training framework. The TCM then extrapolates linearly to any temperature between 268 K and 378 K, achieving markedly improved prediction accuracy compared to established models across all studied temperatures. To further enhance predictive performance, the experimental database was expanded using active learning (AL) strategies for targeted acquisition of new diffusion data by pulsed-field gradient (PFG) NMR measurements. Diffusion coefficients at infinite dilution in 19 solute + solvent systems were measured at 298 K, 313 K, and 333 K. Incorporating these results yields a substantial improvement in the TCM's predictive accuracy. These findings highlight the potential of combining data-efficient ML methods with adaptive experimentation to advance predictive modeling of transport properties.

机构、总结、中文摘要均由AI分析而来,可能存在错误,请以论文正文为准。

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