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

Author:

Cen ZiyuORCID,Han XueORCID,Lin LongfeiORCID,Yang SihaiORCID,Han Wanying,Wen Weilong,Yuan Wenli,Dong Minghua,Ma Zhiye,Li Fang,Ke Yubin,Dong JuncaiORCID,Zhang Jin,Liu Shuhu,Li Jialiang,Li Qian,Wu Ningning,Xiang JunfengORCID,Wu Hao,Cai Lile,Hou Yanbo,Cheng YongqiangORCID,Daemen Luke L.,Ramirez-Cuesta Anibal J.ORCID,Ferrer PilarORCID,Grinter David C.ORCID,Held GeorgORCID,Liu Yueming,Han BuxingORCID

Abstract

AbstractConversion 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.

Funder

RCUK | Engineering and Physical Sciences Research Council

National Science Foundation of China | National Natural Science Foundation of China-Yunnan Joint Fund

National Natural Science Foundation of China

Publisher

Springer Science and Business Media LLC

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