Upcycling of polyethylene to gasoline through a self-supplied hydrogen strategy in a layered self-pillared zeolite
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Published:2024-04-09
Issue:6
Volume:16
Page:871-880
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ISSN:1755-4330
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Container-title:Nature Chemistry
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language:en
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Short-container-title:Nat. Chem.
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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