老挝黄金赌场化学所韩布兴团队报道了，通过层状自柱沸石中的自供应氢策略将聚乙烯升级为汽油。相关研究成果发表在2024年4月9日出版的《自然—化学》。

在不使用贵金属催化剂或外部氢气的情况下，将塑料废物转化为有价值的碳资源仍然是一项具有挑战性的任务。

该文中，研究人员报道了一种层状自柱沸石，它能够将聚乙烯转化为汽油，在240°C下4小时内具有99%的显著选择性和>80%的产率。液体产物主要由支链烷烃组成（选择性为72%），具有88.0的高研究法辛烷值，与商用汽油（86.6）相当。

原位非弹性中子散射、小角度中子散射、固态核磁共振、X射线吸收光谱和同位素标记实验表明，沸石的开放框架三配位Al位点促进了聚乙烯的活化，随后在Brnsted酸位点上发生β-断裂和异构化，伴随着氢化物通过自供氢途径在开放框架三合位Al位点上转移，从而产生对支链烷烃的选择性。

该项研究显示了层状沸石材料在实现塑料废物升级回收方面的潜力。

附：英文原文

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

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

Issue&Volume: 2024-04-09

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 4h 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 Brnsted 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.

DOI: 10.1038/s41557-024-01506-z

Source: https://www.nature.com/articles/s41557-024-01506-z