Chemistry, Ames Laboratory
Journal or Book Title
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.
Tennakoon, Akalanka; Wu, Xun; Paterson, Alexander L.; Patnaik, Smita; Pei, Yuchen; LaPointe, Anne M.; Ammal, Salai C.; Hackler, Ryan A.; Heyden, Andreas; Slowing, Igor I.; Coates, Geoffrey W.; Delferro, Massimiliano; Peters, Baron; Huang, Wenyu; Sadow, Aaron D.; and Perras, Frédéric A., "Catalytic upcycling of high-density polyethylene via a processive mechanism" (2020). Chemistry Publications. 1263.