التفاصيل البيبلوغرافية
| العنوان: |
Machine Learning Models for Predicting Zirconocene Properties and Barriers |
| المؤلفون: |
Justin K. Kirkland, Jugal Kumawat, Maliheh Shaban Tameh, Tyson Tolman, Allison C. Lambert, Graham R. Lief, Qing Yang, Daniel H. Ess |
| سنة النشر: |
2024 |
| مصطلحات موضوعية: |
Biophysics, Biochemistry, Molecular Biology, Science Policy, Biological Sciences not elsewhere classified, Chemical Sciences not elsewhere classified, Information Systems not elsewhere classified, predicting zirconocene properties, naturally emerge showing, machine learning algorithm, ligand aromatic carbons, feature importance analysis, calculated zirconocene properties, aromatic ligand framework, machine learning models, despite robust models, performance significantly depends, barriers zr metallocenes, models depends, transition states, smooth overlap, quantitative accuracy, persistence images, moderate influence, ethylene polymerization, energy structures, direct connections, coulomb matrices, chemical descriptors, bonding hapticity |
| الوصف: |
Zr metallocenes have significant potential to be highly tunable polyethylene catalysts through modification of the aromatic ligand framework. Here we report the development of multiple machine learning models using a large library (>700 systems) of DFT-calculated zirconocene properties and barriers for ethylene polymerization. We show that very accurate machine learning models are possible for HOMO–LUMO gaps of precatalysts but the performance significantly depends on the machine learning algorithm and type of featurization, such as fingerprints, Coulomb matrices, smooth overlap of atomic positions, or persistence images. Surprisingly, the description of the bonding hapticity, the number of direct connections between Zr and the ligand aromatic carbons, only has a moderate influence on the performance of most models. Despite robust models for HOMO–LUMO gaps, these types of machine learning models based on structure connectivity type features perform poorly in predicting ethylene migratory insertion barrier heights. Therefore, we developed several relatively robust and accurate machine learning models for barrier heights that are based on quantum-chemical descriptors (QCDs). The quantitative accuracy of these models depends on which potential energy surface structure QCDs were harvested from. This revealed a Hammett-type principle to naturally emerge showing that QCDs from the π-coordination complexes provide much better descriptions of the transition states than other potential-energy structures. Feature importance analysis of the QCDs provides several fundamental principles that influence zirconocene catalyst reactivity. |
| نوع الوثيقة: |
dataset |
| اللغة: |
unknown |
| العلاقة: |
https://figshare.com/articles/dataset/Machine_Learning_Models_for_Predicting_Zirconocene_Properties_and_Barriers/25047824Test |
| DOI: |
10.1021/acs.jcim.3c01575.s005 |
| الإتاحة: |
https://doi.org/10.1021/acs.jcim.3c01575.s005Test
https://figshare.com/articles/dataset/Machine_Learning_Models_for_Predicting_Zirconocene_Properties_and_Barriers/25047824Test |
| حقوق: |
CC BY-NC 4.0 |
| رقم الانضمام: |
edsbas.89E2E71A |
| قاعدة البيانات: |
BASE |
