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

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 CaiYanbo Hou, Yongqiang Cheng, Luke L. Daemen, Anibal J. Ramirez-Cuesta, Pilar Ferrer, David C. Grinter, Georg Held, Yueming Liu, Buxing Han

Research output: Contribution to journal › Article › peer-review

73 Scopus citations

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. (Figure presented.)

Original language	English
Pages (from-to)	871-880
Number of pages	10
Journal	Nature Chemistry
Volume	16
Issue number	6
DOIs	https://doi.org/10.1038/s41557-024-01506-z
State	Published - Jun 2024

Funding

This work was supported by the National Natural Science Foundation of China (grant no. 22293012 to L.L., grant no. 22293015 to B.H., grant no. 22121002 to B.H.), Engineering and Physical Sciences Research Council (EPSRC) (grant no. EP/V056409/1 to S.Y.), the University of Manchester, Beijing National Laboratory for Molecular Sciences (BNLMS) and Peking University. We thank Beijing Synchrotron Radiation Facility, Diamond Light Source and China Spallation Neutron Source for access to the beamlines 4B7B, B07-B (SI33962) and Small Angle Neutron Diffractometer, respectively. A portion of this research used resources at the Spallation Neutron Source, a Department of Energy (DOE) Office of Science User Facility operated by Oak Ridge National Laboratory. The computing resources at Oak Ridge National Laboratory were made available through the VirtuES and the ICE-MAN projects, funded by Laboratory Directed Research and Development program and Compute and Data Environment for Science. We thank Z. Wang for the assistance during the acquisition of GD ESI mass spectra.

Access to Document

10.1038/s41557-024-01506-z

Cite this

Cen, Z., Han, X., Lin, L., Yang, S., Han, W., Wen, W., Yuan, W., Dong, M., Ma, Z., Li, F., Ke, Y., Dong, J., Zhang, J., Liu, S., Li, J., Li, Q., Wu, N., Xiang, J., Wu, H., ... Han, B. (2024). Upcycling of polyethylene to gasoline through a self-supplied hydrogen strategy in a layered self-pillared zeolite. Nature Chemistry, 16(6), 871-880. https://doi.org/10.1038/s41557-024-01506-z

@article{325db53f3d3a4bc585eb2de2c686dbdc,

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

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 Br{\"o}nsted 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. (Figure presented.)",

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

note = "Publisher Copyright: {\textcopyright} The Author(s) 2024.",

year = "2024",

month = jun,

doi = "10.1038/s41557-024-01506-z",

language = "English",

volume = "16",

pages = "871--880",

journal = "Nature Chemistry",

issn = "1755-4330",

publisher = "Nature Research",

number = "6",

}

Cen, Z, Han, X, Lin, L, Yang, S, Han, W, Wen, W, Yuan, W, Dong, M, Ma, Z, Li, F, Ke, Y, Dong, J, Zhang, J, Liu, S, Li, J, Li, Q, Wu, N, Xiang, J, Wu, H, Cai, L, Hou, Y, Cheng, Y, Daemen, LL, Ramirez-Cuesta, AJ, Ferrer, P, Grinter, DC, Held, G, Liu, Y & Han, B 2024, 'Upcycling of polyethylene to gasoline through a self-supplied hydrogen strategy in a layered self-pillared zeolite', Nature Chemistry, vol. 16, no. 6, pp. 871-880. https://doi.org/10.1038/s41557-024-01506-z

TY - JOUR

T1 - Upcycling of polyethylene to gasoline through a self-supplied hydrogen strategy in a layered self-pillared zeolite

AU - Cen, Ziyu

AU - Han, Xue

AU - Lin, Longfei

AU - Yang, Sihai

AU - Han, Wanying

AU - Wen, Weilong

AU - Yuan, Wenli

AU - Dong, Minghua

AU - Ma, Zhiye

AU - Li, Fang

AU - Ke, Yubin

AU - Dong, Juncai

AU - Zhang, Jin

AU - Liu, Shuhu

AU - Li, Jialiang

AU - Li, Qian

AU - Wu, Ningning

AU - Xiang, Junfeng

AU - Wu, Hao

AU - Cai, Lile

AU - Hou, Yanbo

AU - Cheng, Yongqiang

AU - Daemen, Luke L.

AU - Ramirez-Cuesta, Anibal J.

AU - Ferrer, Pilar

AU - Grinter, David C.

AU - Held, Georg

AU - Liu, Yueming

AU - Han, Buxing

PY - 2024/6

Y1 - 2024/6

N2 - 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. (Figure presented.)

AB - 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. (Figure presented.)

UR - https://www.scopus.com/pages/publications/85189919895

U2 - 10.1038/s41557-024-01506-z

DO - 10.1038/s41557-024-01506-z

M3 - Article

C2 - 38594366

AN - SCOPUS:85189919895

SN - 1755-4330

VL - 16

SP - 871

EP - 880

JO - Nature Chemistry

JF - Nature Chemistry

IS - 6

ER -

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

Abstract

Funding

Access to Document

Other files and links

Fingerprint

Cite this