Catalytic upcycling of high-density polyethylene via a processive mechanism

Autor: Yuchen Pei, Wenyu Huang, Alexander L. Paterson, Frédéric A. Perras, Igor I. Slowing, Geoffrey W. Coates, Baron Peters, Aaron D. Sadow, Andreas Heyden, Xun Wu, Akalanka Tennakoon, Salai Cheettu Ammal, Massimiliano Delferro, Smita Patnaik, Ryan A. Hackler, Anne M. LaPointe
Rok vydání: 2020
Předmět:
Zdroj: Nature Catalysis. 3:893-901
ISSN: 2520-1158
Popis: The overconsumption of single-use plastics is creating a global waste catastrophe, with widespread environmental, economic and health-related consequences. Here we show that the benefits of processive enzyme-catalysed conversions of biomacromolecules can be leveraged to affect the selective hydrogenolysis of high-density polyethylene into a narrow distribution of diesel and lubricant-range alkanes using an ordered, mesoporous shell/active site/core catalyst architecture that incorporates catalytic platinum sites at the base of the mesopores. Solid-state nuclear magnetic resonance revealed that long hydrocarbon macromolecules readily move within the pores of this catalyst, with a subsequent escape being inhibited by polymer–surface interactions, a behaviour that resembles the binding and translocation of macromolecules in the catalytic cleft of processive enzymes. Accordingly, the hydrogenolysis of polyethylene with this catalyst proceeds processively to yield a reliable, narrow and tunable stream of alkane products. Achieving plastic deconstruction with high selectivity is crucial for upcycling schemes, but remains challenging. Here, a processive approach for the selective hydrogenolysis of high-density polyethylene into narrow alkane fractions is introduced relying on a Pt/SiO2 catalyst encapsulated in a mesoporous silica shell.
Databáze: OpenAIRE