PACMAN:基于晶体图卷积网络的纳米多孔材料鲁棒部分原子电荷预测器

IF 5.5 1区 化学 Q2 CHEMISTRY, PHYSICAL
Guobin Zhao,  and , Yongchul G. Chung*, 
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引用次数: 0

摘要

我们报告了一种快速简便的方法(PACMAN),该方法基于从量子金属有机框架(QMOF)数据库获得的 180 万个高保真部分原子电荷数据训练的图卷积网络(GCN),用于分配金属有机框架(MOF)和共价有机框架(COF)晶体结构的部分原子电荷。所开发的模型性能卓越,其平均绝对误差 (MAE) 为 0.0055 e(测试集性能),同时与 DDEC6、Bader 和 CM5 电荷保持一致,适用于不同化学性质和拓扑结构的 MOFs 和 COFs。我们发现,新方法准确地分配了含离子纳米多孔材料的部分原子电荷,这在以前的机器学习(ML)模型中是不可能实现的。与文献中报道的其他 ML 模型相比,基于 PACMAN 和原始 DDEC6 电荷的 CO2 和 N2 吸收的大规范蒙特卡罗(GCMC)模拟结果和水的亨利定律常数的 Widom 粒子插入计算结果显示出极佳的一致性。新方法的运行时间分析表明,可在 10 秒内获得多达 500 个原子的 MOF 和 COF 结构的部分原子电荷。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

PACMAN: A Robust Partial Atomic Charge Predicter for Nanoporous Materials Based on Crystal Graph Convolution Networks

PACMAN: A Robust Partial Atomic Charge Predicter for Nanoporous Materials Based on Crystal Graph Convolution Networks

PACMAN: A Robust Partial Atomic Charge Predicter for Nanoporous Materials Based on Crystal Graph Convolution Networks

We report a fast and easy method (PACMAN) to assign partial atomic charges on metal–organic framework (MOF) and covalent–organic framework (COF) crystal structures based on graph convolution networks (GCNs) trained on >1.8 million high-fidelity partial atomic charge data obtained from the Quantum Metal–Organic Framework (QMOF) database. The developed model shows outstanding performance, achieving a mean absolute error (MAE) of 0.0055 e (test set performance) while maintaining consistency with DDEC6, Bader, and CM5 charges across diverse chemistry and topologies of MOFs and COFs. We find that the new method accurately assigns partial atomic charges for ion-containing nanoporous materials, which has not been possible in previous machine learning (ML) models. Grand canonical Monte Carlo (GCMC) simulation results for CO2 and N2 uptakes and the Widom particle insertion calculation for Henry’s law constant of water results based on PACMAN and the original DDEC6 charges show excellent agreements compared to other ML models reported in the literature. The runtime analysis of the new method demonstrates that the partial atomic charges of MOF and COF structures with up to 500 atoms can be obtained in less than 10 s. An easy-to-use web interface has been developed to facilitate the adoption of the developed model.

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来源期刊
Journal of Chemical Theory and Computation
Journal of Chemical Theory and Computation 化学-物理:原子、分子和化学物理
CiteScore
9.90
自引率
16.40%
发文量
568
审稿时长
1 months
期刊介绍: The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.
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