Catalytic upcycling of high-density polyethylene via a processive mechanism

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.; Perras, Frédéric A.

doi:10.1038/s41929-020-00519-4

Catalytic upcycling of high-density polyethylene via a processive mechanism

Journal Article · Mon Oct 12 00:00:00 UTC 2020 · Nature Catalysis

DOI:https://doi.org/10.1038/s41929-020-00519-4· OSTI ID:1700695

^[1]; Wu, Xun ^[1]; ^[1]; Patnaik, Smita ^[1]; Pei, Yuchen ^[1]; ^[2]; ^[3]; Hackler, Ryan A. ^[4]; Heyden, Andreas ^[3]; ^[1]; ^[2]; ^[4]; Peters, Baron ^[5]; ^[1]; ^[1]; ^[1]

Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
Cornell Univ., Ithaca, NY (United States)
Univ. of South Carolina, Columbia, SC (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Univ. of Illinois at Urbana-Champaign, IL (United States)

The overconsumption of single-use plastics is creating a global waste catastrophe, with widespread environmental, economic and health-related consequences. In this work 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.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division

Grant/Contract Number:: AC02-06CH11357; AC02-07CH11358

OSTI ID:: 1700695

Alternate ID(s):: OSTI ID: 1706641
OSTI ID: 1712698

Report Number(s):: IS--J-10,271; IS--J-10,293

Journal Information:: Nature Catalysis, Journal Name: Nature Catalysis Journal Issue: 11 Vol. 3; ISSN 2520-1158

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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