A Ziegler-type spherical cap model reveals early stage ethylene polymerization growth versus catalyst fragmentation relationships

Koen W. Bossers, Laurens D. B. Mandemaker, Nikolaos Nikolopoulos, Yuanshuai Liu, Marcus Rohnke, Peter Peinder, Bas J. P. Terlingen, Felix Walther, Joren M. Dorresteijn, Thomas Hartman and Bert M. Weckhuysen ()
Additional contact information
Koen W. Bossers: Utrecht University
Laurens D. B. Mandemaker: Utrecht University
Nikolaos Nikolopoulos: Utrecht University
Yuanshuai Liu: Utrecht University
Marcus Rohnke: Justus Liebig University
Peter Peinder: VibSpec, Haaftenlaan 28
Bas J. P. Terlingen: Utrecht University
Felix Walther: Justus Liebig University
Joren M. Dorresteijn: Utrecht University
Thomas Hartman: Utrecht University
Bert M. Weckhuysen: Utrecht University

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract Polyolefin catalysts are characterized by their hierarchically complex nature, which complicates studies on the interplay between the catalyst and formed polymer phases. Here, the missing link in the morphology gap between planar model systems and industrially relevant spherical catalyst particles is introduced through the use of a spherical cap Ziegler-type catalyst model system for the polymerization of ethylene. More specifically, a moisture-stable LaOCl framework with enhanced imaging contrast has been designed to support the TiCl4 pre-active site, which could mimic the behaviour of the highly hygroscopic and industrially used MgCl2 framework. As a function of polymerization time, the fragmentation behaviour of the LaOCl framework changed from a mixture of the shrinking core (i.e., peeling off small polyethylene fragments at the surface) and continuous bisection (i.e., internal cleavage of the framework) into dominantly a continuous bisection model, which is linked to the evolution of the estimated polyethylene volume and the fraction of crystalline polyethylene formed. The combination of the spherical cap model system and the used advanced micro-spectroscopy toolbox, opens the route for high-throughput screening of catalyst functions with industrially relevant morphologies on the nano-scale.

Date: 2022
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DOI: 10.1038/s41467-022-32635-z

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