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Facile Polyolefin Plastics Hydrogenolysis Catalyzed by a Surface Electrophilic d0 Hydride
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Researchers demonstrated that polyolefin plastics — a major fraction of single-use plastic waste — can be chemically broken down using a zirconium catalyst on a highly acidic support material. Catalytic hydrogenolysis of polyolefins is a promising approach to chemical recycling that could reduce the amount of plastic entering the environment as microplastics.
Polyolefins comprise a major fraction of single-use plastics and yet their catalytic deconstruction/recycling has proven challenging due to their inert hydrocarbon connectivities. Here an electrophilic earth-abundant single-site organozirconium catalyst chemisorbed on a highly Brønsted acidic support and characterized by a broad array of experimental and theoretical techniques, is shown to mediate the rapid hydrogenolytic cleavage of molecular and macromolecular saturated hydrocarbons under mild conditions. For n-hexadecane, hydrogenolysis to light hydrocarbons proceeds with an activity of 690 mol n-hexadecane · mol Zr-1 · h-1 at 150°C/2.5 atm H2 pressure. Under similar solventless conditions, polyethylene, polyethylene-co- 1-octene, isotactic polypropylene, and a post-consumer sandwich bag are rapidly hydrogenolyzed to low molecular mass hydrocarbons via a turnover-limiting C-C scission pathway involving ßalkyl transfer rather than more common σ-bond metathesis.
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This review examines recent scientific advances in catalytic chemical recycling of polyolefins such as polyethylene and polypropylene, which account for nearly 50% of all plastic production by mass. Researchers highlight catalytic processes that can break down polyolefin waste at lower temperatures than pyrolysis, with the goal of upcycling discarded plastics into functional chemicals rather than sending them to landfill.
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