Conformations of polyolefins on platinum catalysts control product distribution in plastics recycling Chemical Science RSC Publishing DOI:10 1039 D2SC04772A

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• The design of catalysts for the chemical recycling of plastic waste will benefit greatly from an intimate knowledge of the interfacial polymer–catalyst interactions that determine reactant and product distributions.
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The design of catalysts for the chemical recycling of plastic waste will benefit greatly from an intimate knowledge of the interfacial polymer–catalyst interactions that determine reactant and product distributions. Here, we investigate backbone chain length, side chain length, and concentration effects on the density and conformation of polyethylene surrogates at the interface with Pt(111) and relate them to experimental product distributions resulting from carbon–carbon bond cleavage. Using replica-exchange molecular dynamics simulations, we characterize the polymer conformations at the interface by the distributions of trains, loops, and tails and their first moments. We find that the preponderance of short chains, in the range of 20 carbon atoms, lies entirely on the Pt surface, whereas longer chains exhibit much broader distributions of conformational features. Remarkably, the average length of trains is independent of the chain length but can be tuned via the polymer–surface interaction. The degree of localization increases with the number and size of the side chains.

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Long chains can adsorb from the melt onto the Pt surface even in melt mixtures containing shorter polymer chains at high concentrations. We confirm experimentally key computational findings and demonstrate that blends may provide a strategy to reduce the selectivity for undesired light gases. The solid polymer (PE, Mw ∼4 kDa, Mn ∼1.7 kDa, Sigma-Aldrich) or a mixture of PE and icosane (TCI) was mixed with a freshly reduced catalyst and loaded in a high-pressure stainless-steel Parr reactor with a Teflon magnetic stir bar without a liner.

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