Fast and Accurate Ring Strain Energy Predictions with Machine Learning and Application in Strain-Promoted Reactions

利用机器学习快速准确地预测环应变能及其在应变促进反应中的应用

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Abstract

Ring strain energy (RSE) is crucial for understanding molecular reactivity, with broad implications in polymerization, click chemistry, drug discovery and beyond. However, quantitatively determining RSE through experiments or quantum mechanics (QM) is resource-intensive, limiting its application on a large scale. We present a machine learning (ML)-based workflow that enables the reliable and efficient prediction of RSE, entirely bypassing traditional QM calculations. Our workflow employs AIMNet2 machine learning interatomic potentials and Auto3D for the identification of low-energy conformers and RSE computation. Remarkably, it achieves an R (2) of 0.997 and a mean absolute error (MAE) of 0.896 kcal/mol when benchmarked against the ωB97M-D4/Def2-TZVPP method, while running orders of magnitude faster than DFT calculations. To demonstrate the utility of our workflow, we successfully differentiated reactive from nonreactive molecules in copper-free click chemistry, [3 + 2] cycloaddition reaction and ring-opening metathesis polymerization, underscoring its transferability to diverse molecular systems. Additionally, we compiled the RSE Atlas, a computational database encompassing 16,905 single-ring molecules, offering a valuable resource for investigating factors influencing RSE. Our approach transforms RSE into a readily computable property, facilitating its integration into reaction designs.

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