Title
Catalytic upcycling of high-density polyethylene via a processive mechanism
Publication Date
10-12-2020
Department
Ames Laboratory; Chemistry
Campus Units
Ames Laboratory, Chemistry
OSTI ID+
1700695
Report Number
IS-J 10271
DOI
10.1038/s41929-020-00519-4
Journal Title
Nature Catalysis
Abstract
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.
DOE Contract Number(s)
AC02-07CH11358; AC02-06CH11357
Language
en
Publisher
Iowa State University Digital Repository, Ames IA (United States)