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

NATURE CHEMISTRY(2024)

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摘要
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 degrees 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 beta-scission and isomerization on Br & ouml;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.
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