通过相对预测提升热稳定性模型鲁棒性,适用于不一致实验数据。
Differential Learning for Robust Prediction of Thermal Stability with Application to Energetic Materials
- 训练模型预测分子对的热稳定性差异,而非绝对值。
- 在异质数据集上排名准确率超85%,优于传统回归方法。
- 揭示键解离焓是热稳定性关键决定因素,适合材料安全设计。
预测含能材料在处理和储存过程中的热稳定性对设计安全可靠材料至关重要。然而,由于实验协议与分析方法差异,不同实验室测得的数据波动大,难以训练可靠预测模型。本文提出差分学习:不预测绝对分解温度,而是训练消息传递神经网络预测分子对之间的相对稳定性差异。该方法降低系统误差影响,在同一异质数据集上实现超过85%的化合物排序准确率,显著优于传统回归方法。为理解预测机制,我们对比了神经网络与基于从头算计算和化学信息学软件生成描述符的可解释模型,发现键解离焓是热稳定性排序的关键决定因素,深化了对热分解复杂化学的理解。该差分学习框架可泛化至图神经网络及传统描述符方法。结果表明,学习相对属性是应对噪声实验数据的有效策略,可直接应用于材料设计中以指导安全规程制定。
原文摘要 · Abstract (English)
Predicting thermal stability during handling and storage is essential for the design of safe and reliable energetic materials. However, experimental measurements vary significantly across laboratories due to differences in protocols and analysis methods, making it difficult to train reliable predictive models. We address this challenge through differential learning. Rather than predicting absolute decomposition temperatures, we instead train message passing neural networks to predict relative differences between pairs of molecules. This approach reduces sensitivity to systematic experimental errors and achieves >85% accuracy in ranking compounds by thermal stability, outperforming conventional regression methods on the same heterogeneous dataset. To understand what drives these predictions, we compare neural network models with interpretable alternatives built from descriptors derived from ab initio calculations and cheminformatics software. This analysis identifies bond dissociation enthalpy as a key determinant of thermal stability rankings, providing further insight into the complex chemistry of thermal decomposition. The differential learning framework generalizes across model architectures, from graph neural networks to classical descriptor-based approaches. Our results demonstrate that learning relative properties rather than absolute values offers a practical solution for modeling noisy experimental data, with direct applications in materials design where thermal stability predictions inform safety protocols.
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