Molecular field analysis in half-titanocene complexes: computational study towards data-driven optimization of single-site olefin polymerization catalysts

• Published in: Catalysis science & technology 2024-05, Vol.14 (9), p.2434-244
• Main Authors: Yamaguchi, Shigeru, Kikuchi, Takahiro, Tanaka, Kenichi, Takamiya, Ikuko
• Format: Article
• ISSN: 2044-4753; 2044-4761
• DOI: 10.1039/d4cy00241e

We performed molecular field analysis using computed data of half-titanocene-catalyzed olefin polymerization. The activation energies of ethylene insertion, propylene insertion, and the energy differences between ethylene insertion and β-hydrogen transfer calculated with DFT methods were employed as target variables for regression analysis. Molecular fields (voxel data) calculated from corresponding transition-state structures were used as descriptors. The structural information visualized based on the molecular field-based regression analysis provided a catalyst design guideline. A phosphinimide catalyst designed following the guideline showed enhanced computed free energy values. According to a previous report, the designed catalyst exhibited higher activity and polymer molecular weight in ethylene polymerization compared to a high performance phosphinimide catalyst in the training samples. The control of multiple reaction outcomes in olefin polymerization has been demonstrated through data-driven catalyst optimization based on molecular field analysis, using data collected from DFT-based transition-state calculations.