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

Ziyu Cen; Xue Han; Longfei Lin; Sihai Yang; Wanying Han; Weilong Wen; Wenli Yuan; Minghua Dong; Zhiye Ma; Fang Li; Yubin Ke; Juncai Dong; Jin Zhang; Shuhu Liu; Jialiang Li; Qian Li; Ningning Wu; Junfeng Xiang; Hao Wu; Lile Cai; Yanbo Hou; Yongqiang Cheng; Luke L Daemen; Anibal J Ramirez-Cuesta; Pilar Ferrer; David C Grinter; Georg Held; Yueming Liu; Buxing Han

doi:10.1038/s41557-024-01506-z

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

Nat Chem. 2024 Apr 9. doi: 10.1038/s41557-024-01506-z. Online ahead of print.

Authors

Ziyu Cen^{1

2}, Xue Han³, Longfei Lin^{4

5}, Sihai Yang^{6

7}, Wanying Han⁸, Weilong Wen^{1

2}, Wenli Yuan¹, Minghua Dong^{1

2}, Zhiye Ma^{1

2}, Fang Li⁸, Yubin Ke⁹, Juncai Dong¹⁰, Jin Zhang¹⁰, Shuhu Liu¹⁰, Jialiang Li¹⁰, Qian Li¹¹, Ningning Wu¹¹, Junfeng Xiang¹¹, Hao Wu¹², Lile Cai¹², Yanbo Hou¹², Yongqiang Cheng¹³, Luke L Daemen¹³, Anibal J Ramirez-Cuesta¹³, Pilar Ferrer¹⁴, David C Grinter¹⁴, Georg Held¹⁴, Yueming Liu⁸, Buxing Han^{15

16

17

18}

Affiliations

¹ Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, China.
² School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, China.
³ College of Chemistry, Beijing Normal University, Beijing, China. xue.han@bnu.edu.cn.
⁴ Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, China. linlongfei@iccas.ac.cn.
⁵ School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, China. linlongfei@iccas.ac.cn.
⁶ College of Chemistry and Molecular Engineering, Beijing National Laboratory for Molecular Sciences, Peking University, Beijing, China. sihai.yang@pku.edu.cn.
⁷ Department of Chemistry, University of Manchester, Manchester, UK. sihai.yang@pku.edu.cn.
⁸ Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular and Process Engineering, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, China.
⁹ China Spallation Neutron Source, Institute of High Energy Physics, Dongguan, China.
¹⁰ Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, China.
¹¹ Center for Physicochemical Analysis Measurements, Institute of Chemistry, Chinese Academy of Sciences, Beijing, China.
¹² SINOPEC Research Institute of Petroleum Processing, Beijing, China.
¹³ Neutron Scattering Division, Neutron Sciences Directorate, Oak Ridge National Laboratory, Oak Ridge, TN, USA.
¹⁴ Diamond Light Source, Harwell Science and Innovation Campus, Didcot, UK.
¹⁵ Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, China. hanbx@iccas.ac.cn.
¹⁶ School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, China. hanbx@iccas.ac.cn.
¹⁷ Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular and Process Engineering, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, China. hanbx@iccas.ac.cn.
¹⁸ Institute of Eco-Chongming, Shanghai, China. hanbx@iccas.ac.cn.

PMID: 38594366
DOI: 10.1038/s41557-024-01506-z

Abstract

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.

Abstract

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