DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Upcycling of polyethylene to gasoline through a self-supplied hydrogen strategy in a layered self-pillared zeolite

Journal Article · · Nature Chemistry
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [3];  [4];  [1];  [5];  [1];  [1];  [4];  [6]; ORCiD logo [7];  [7];  [7];  [7];  [8];  [8]; ORCiD logo [8];  [9];  [9] more »;  [9]; ORCiD logo [10];  [10]; ORCiD logo [10]; ORCiD logo [11]; ORCiD logo [11]; ORCiD logo [11];  [4]; ORCiD logo [12] « less
  1. Chinese Academy of Sciences (CAS), Beijing (China); University of Chinese Academy of Sciences, Beijing (China)
  2. Beijing Normal University, Beijing (China)
  3. Peking University, Beijing (China); University of Manchester (United Kingdom)
  4. East China Normal University (ECNU), Shanghai (China)
  5. Chinese Academy of Sciences (CAS), Beijing (China)
  6. Institute of High Energy Physics (IHEP), Dongguan (China). China Spallation Neutron Source (CSNS)
  7. Chinese Academy of Sciences (CAS), Beijing (China). Institute of High Energy Physics (IHEP)
  8. Chinese Academy of Sciences (CAS), Beijing (China). Institute of Chemistry
  9. SINOPEC Research Institute of Petroleum Processing (RIPP), Beijing (China)
  10. Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
  11. Harwell Science and Innovation Campus, Didcot (United Kingdom). Diamond Light Source, Ltd.
  12. Chinese Academy of Sciences (CAS), Beijing (China). Institute of Chemistry; University of Chinese Academy of Sciences, Beijing (China); East China Normal University (ECNU), Shanghai (China); Institute of Eco-Chongming, Shanghai (China)

Conversion of plastic wastes to valuable carbon resources without using noble metal catalysts or external hydrogen remains a challenging task. Here we report a layered self-pillared zeolite that enables the conversion of polyethylene to gasoline with a remarkable selectivity of 99% and yields of >80% in 4 h at 240 °C. The liquid product is primarily composed of branched alkanes (selectivity of 72%), affording a high research octane number of 88.0 that is comparable to commercial gasoline (86.6). In situ inelastic neutron scattering, small-angle neutron scattering, solid-state nuclear magnetic resonance, X-ray absorption spectroscopy and isotope-labelling experiments reveal that the activation of polyethylene is promoted by the open framework tri-coordinated Al sites of the zeolite, followed by β-scission and isomerization on Brönsted acids sites, accompanied by hydride transfer over open framework tri-coordinated Al sites through a self-supplied hydrogen pathway to yield selectivity to branched alkanes. This study shows the potential of layered zeolite materials in enabling the upcycling of plastic wastes.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Laboratory Directed Research and Development (LDRD) Program; National Natural Science Foundation of China (NSFC); Engineering and Physical Sciences Research Council (EPSRC)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
2471533
Journal Information:
Nature Chemistry, Journal Name: Nature Chemistry Journal Issue: 6 Vol. 16; ISSN 1755-4330
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (44)

Plastic Waste Conversion over a Refinery Waste Catalyst journal June 2021
Unravelling the Reactivity of Framework Lewis Acid Sites towards Methanol Activation on H‐ZSM‐5 Zeolite with Solid‐State NMR Spectroscopy journal September 2022
FT-IR Studies on Light Olefin Skeletal Isomerization Catalysis journal October 1998
Isomerization and hydrocracking of C9 through C16 n-alkanes on Pt/HZSM-5 zeolite journal October 1983
aCLIMAX 4.0.1, The new version of the software for analyzing and interpreting INS spectra journal March 2004
The Haag–Dessau mechanism of protolytic cracking of alkanes journal April 2000
Conversion of polyethylene waste to short chain hydrocarbons under mild temperature and hydrogen pressure with metal-free and metal-loaded MFI zeolites journal December 2023
Catalyst: Design Challenges for the Future of Plastics Recycling journal December 2016
Plasticenta: First evidence of microplastics in human placenta journal January 2021
On the origin of the difference between type A and type B skeletal isomerization of alkenes catalyzed by zeolites: The crucial input of ab initio molecular dynamics journal May 2019
Viscosity of heavy n -alkanes and diffusion of gases therein based on molecular dynamics simulations and empirical correlations journal December 2015
Polypropylene Plastic Waste Conversion to Lubricants over Ru/TiO 2 Catalysts journal June 2021
Disordered, Sub-Nanometer Ru Structures on CeO2 are Highly Efficient and Selective Catalysts in Polymer Upcycling by Hydrogenolysis journal April 2022
Hydrogenolysis of Polypropylene and Mixed Polyolefin Plastic Waste over Ru/C to Produce Liquid Alkanes journal July 2021
Acid Strength Controlled Reaction Pathways for the Catalytic Cracking of 1-Pentene to Propene over ZSM-5 journal June 2015
Catalytic Degradation of High-Density Polyethylene over Different Zeolitic Structures journal March 2000
Local structure of sodium aluminosilicate glass: an ab initio molecular orbital study journal September 1993
Coking-Resistant Polyethylene Upcycling Modulated by Zeolite Micropore Diffusion journal August 2022
Conversion of Polyolefin Waste to Liquid Alkanes with Ru-Based Catalysts under Mild Conditions journal December 2020
Polyethylene Hydrogenolysis at Mild Conditions over Ruthenium on Tungstated Zirconia journal August 2021
Efficient solvent- and hydrogen-free upcycling of high-density polyethylene into separable cyclic hydrocarbons journal June 2023
Chemical recycling of waste plastics for new materials production journal June 2017
Critical advances and future opportunities in upcycling commodity polymers journal March 2022
Depolymerization of plastics by means of electrified spatiotemporal heating journal April 2023
Recovering waste plastics using shape-selective nano-scale reactors as catalysts journal January 2019
Catalytic upcycling of high-density polyethylene via a processive mechanism journal October 2020
Zeolites as catalysts in oil refining journal January 2014
Design of Lewis-acid centres in zeolitic matrices for the conversion of renewables journal January 2015
Structure of the water ice surface studied by x-ray absorption spectroscopy at the O K-edge journal December 2002
Electronic structure analysis of via x-ray absorption near-edge structure at the Si K, and O K edges journal September 1998
alpha-Al2O3 (0001) Surfaces: Atomic and Electronic Structure journal February 1994
Efficient and selective degradation of polyethylenes into liquid fuels and waxes under mild conditions journal June 2016
Production, use, and fate of all plastics ever made journal July 2017
Plastic waste to fuels by hydrocracking at mild conditions journal April 2021
Synthesis of Self-Pillared Zeolite Nanosheets by Repetitive Branching journal June 2012
Predicted growth in plastic waste exceeds efforts to mitigate plastic pollution journal September 2020
The global odyssey of plastic pollution journal June 2020
Polyethylene upcycling to long-chain alkylaromatics by tandem hydrogenolysis/aromatization journal October 2020
Toward polymer upcycling—adding value and tackling circularity journal July 2021
The global threat from plastic pollution journal July 2021
Chemically recyclable thermoplastics from reversible-deactivation polymerization of cyclic acetals journal August 2021
Mixed plastics waste valorization through tandem chemical oxidation and biological funneling journal October 2022
Catalytic deconstruction of waste polyethylene with ethylene to form propylene journal September 2022
Low-temperature upcycling of polyolefins into liquid alkanes via tandem cracking-alkylation journal February 2023