Assessment of transport phenomena in catalyst effectiveness for chemical polyolefin recycling

Since the dawn of agitated brewing in the Paleolithic era, effective mixing has enabled efficient reactions. Emerging catalytic chemical polyolefin recycling processes present unique challenges, considering that the polymer melt has a viscosity three orders of magnitude higher than that of honey. The lack of protocols to achieve effective mixing may have resulted in suboptimal catalyst effectiveness. In this study, we have tackled the hydrogenolysis of commercial-grade high-density polyethylene and polypropylene to show how different stirring strategies can create differences of up to 85% and 40% in catalyst effectiveness and selectivity, respectively. The reaction develops near the H2–melt interface, with the extension of the interface and access to catalyst particles the main performance drivers. Leveraging computational fluid dynamics simulations, we have identified a power number of 15,000–40,000 to maximize the catalyst effectiveness factor and optimize stirring parameters. This temperature- and pressure-independent model holds across a viscosity range of 1–1,000 Pa s. Temperature gradients may quickly become relevant for reactor scale-up. The importance of optimizing the contact between catalyst particles, hydrogen and plastic melt in polyolefin chemical recycling has been overlooked, leading to suboptimal performance. The authors develop a criterion based on the dimensionless power number to optimize catalyst effectiveness. Stirring conditions can now be selected to treat commercial-grade polyethylene and polypropylene.