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基于机器学习的用于可控烯烃共聚的茂金属催化剂设计

Machine-Learning-Based Design of Metallocene Catalysts for Controlled Olefin Copolymerization.

作者信息

Kim Yongjun, Kim Yeonjoon, Kim Hyeonsu, Kang Sungwoo, Kim Jaewook, Lee Kyunghoon, Jeong Wook, Lee Won Jong, Ryu Ho, Kim Kyungwoo, Kim Woo Youn

机构信息

Department of Chemistry, KAIST, 291 Daehak-ro, Yuseong-gu, Daejeon, 34141, Republic of Korea.

Department of Chemistry, Pukyong National University, 45 Yongso-ro, Nam-gu, Busan, 48513, Republic of Korea.

出版信息

Chemistry. 2025 Jun 6;31(32):e202500316. doi: 10.1002/chem.202500316. Epub 2025 May 7.

DOI:10.1002/chem.202500316
PMID:40331399
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12144874/
Abstract

Polyolefins are versatile materials for various purposes, but their functionality should be fine-tuned for target applications including the mitigation of adverse environmental impacts. Producing such polymers with desired properties requires catalysts that can control polymerization at an atomistic level. However, complex reaction mechanisms and very limited experimental data make it difficult to design new efficient catalysts using conventional computational and data-driven approaches. Here, we present a pragmatic strategy based on data-efficient predictive models combined with a genetic algorithm to design new catalysts for controlled ethylene/hexene copolymerization. By deriving the chemically intuitive descriptors from the mechanistic analysis of the polymerization, we achieved the promising predictive models with small data applicable to various core structures and different experimental conditions, respectively. We screened catalysts through a virtual screening scheme combining a genetic algorithm and predictive models using chemically intuitive descriptors and considered their synthesizability through the manual inspections of experts. As a result, we successfully designed nine catalysts with desired comonomer ratios and diverse core structures.

摘要

聚烯烃是用于各种目的的通用材料,但其功能应针对包括减轻不利环境影响在内的目标应用进行微调。生产具有所需性能的此类聚合物需要能够在原子水平上控制聚合反应的催化剂。然而,复杂的反应机制和非常有限的实验数据使得使用传统的计算和数据驱动方法设计新型高效催化剂变得困难。在此,我们提出了一种基于数据高效预测模型并结合遗传算法的实用策略,以设计用于可控乙烯/己烯共聚的新型催化剂。通过从聚合反应的机理分析中得出化学直观描述符,我们分别针对适用于各种核心结构和不同实验条件的小数据实现了有前景的预测模型。我们通过结合遗传算法和使用化学直观描述符的预测模型的虚拟筛选方案筛选催化剂,并通过专家的人工检查考虑它们的可合成性。结果,我们成功设计了九种具有所需共聚单体比例和不同核心结构的催化剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d0f0/12144874/ed3c51c2e145/CHEM-31-e202500316-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d0f0/12144874/b0f13fbaf310/CHEM-31-e202500316-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d0f0/12144874/308c0fad8b26/CHEM-31-e202500316-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d0f0/12144874/d19908843632/CHEM-31-e202500316-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d0f0/12144874/ea9844fdc775/CHEM-31-e202500316-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d0f0/12144874/9613ad31897e/CHEM-31-e202500316-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d0f0/12144874/ed3c51c2e145/CHEM-31-e202500316-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d0f0/12144874/b0f13fbaf310/CHEM-31-e202500316-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d0f0/12144874/308c0fad8b26/CHEM-31-e202500316-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d0f0/12144874/d19908843632/CHEM-31-e202500316-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d0f0/12144874/ea9844fdc775/CHEM-31-e202500316-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d0f0/12144874/9613ad31897e/CHEM-31-e202500316-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d0f0/12144874/ed3c51c2e145/CHEM-31-e202500316-g007.jpg

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Computational Methods Enable the Prediction of Improved Catalysts for Nickel-Catalyzed Cross-Electrophile Coupling.
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