Active Learning Guided Optimization of Frontal Ring-Opening Metathesis Polymerization via Alkylidene Modification

IF 5.2 Q1 POLYMER SCIENCE ACS Macro Letters Pub Date : 2025-04-11 DOI:10.1021/acsmacrolett.5c00136

Ignacio Arretche, Jacob J. Lessard, Parmeet Kaur, Mya G. Mills, Abbie J. Kim, Hannah J. Liu, Julian C. Cooper, Randy H. Ewoldt, Jeffrey S. Moore, Sameh Tawfick

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Abstract

Frontal ring-opening metathesis polymerization (FROMP) offers an energy-efficient method for manufacturing high-performance thermoset resins. However, the background reaction attributed to ring-opening metathesis polymerization (ROMP) results in a complex trade-off between the resin shelf life─necessary for practical manufacturability─and the front velocity. Here, we study the influence of alkylidene ligand selection in Grubbs’ second-generation Ru-initiators on the kinetics of FROMP and background ROMP. We reveal that ligand identity differentially affects FROMP and background ROMP reactivity, enabling tunable control over pot life and front speed. Leveraging this insight, we use active learning with multiobjective Bayesian optimization to efficiently explore the FROMP resin design space and identify superior resin formulations. This work advances the rational design of FROMP resins, expanding the range of accessible formulations and accelerating the discovery of high-performance materials for energy-efficient manufacturing applications.

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主动学习引导下烷基烯改性正面开环复分解聚合的优化

正面开环复分解聚合（FROMP）为制造高性能热固性树脂提供了一种节能的方法。然而，归因于开环复分解聚合（ROMP）的背景反应导致树脂货架寿命（实际可制造性所必需的）和前速度之间的复杂权衡。本文研究了Grubbs第二代ru引发剂中烷基基配体的选择对FROMP和背景ROMP动力学的影响。我们发现配体的同一性对FROMP和背景ROMP反应性有不同的影响，从而可以对锅寿命和前端速度进行可调控制。利用这一见解，我们使用主动学习和多目标贝叶斯优化来有效地探索FROMP树脂设计空间并确定优越的树脂配方。这项工作推进了FROMP树脂的合理设计，扩大了可获得配方的范围，并加速了节能制造应用的高性能材料的发现。

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来源期刊

ACS Macro Letters 化学-

CiteScore

10.40

自引率

3.40%

发文量

209

审稿时长

1 months

期刊介绍： ACS Macro Letters publishes research in all areas of contemporary soft matter science in which macromolecules play a key role, including nanotechnology, self-assembly, supramolecular chemistry, biomaterials, energy generation and storage, and renewable/sustainable materials. Submissions to ACS Macro Letters should justify clearly the rapid disclosure of the key elements of the study. The scope of the journal includes high-impact research of broad interest in all areas of polymer science and engineering, including cross-disciplinary research that interfaces with polymer science. With the launch of ACS Macro Letters, all Communications that were formerly published in Macromolecules and Biomacromolecules will be published as Letters in ACS Macro Letters.