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用于抑制甲烷化和生产液体燃料的原子级钌上的位点选择性聚烯烃氢解反应

Site-Selective Polyolefin Hydrogenolysis on Atomic Ru for Methanation Suppression and Liquid Fuel Production.

作者信息

Chu Mingyu, Wang Xianpeng, Wang Xuchun, Lou Xiangxi, Zhang Congyang, Cao Muhan, Wang Lu, Li Youyong, Liu Sibao, Sham Tsun-Kong, Zhang Qiao, Chen Jinxing

机构信息

Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices, Soochow University, Suzhou 215123, P. R. China.

Department of Chemistry, University of Western Ontario, London, Ontario N6A 5B7, Canada.

出版信息

Research (Wash D C). 2023;6:0032. doi: 10.34133/research.0032. Epub 2023 Jan 13.

Abstract

Catalytic hydrogenolysis of end-of-life polyolefins can produce value-added liquid fuels and therefore holds great promises in plastic waste reuse and environmental remediation. The major challenge limiting the recycling economic benefit is the severe methanation (usually >20%) induced by terminal C-C cleavage and fragmentation in polyolefin chains. Here, we overcome this challenge by demonstrating that Ru single-atom catalyst can effectively suppress methanation by inhibiting terminal C-C cleavage and preventing chain fragmentation that typically occurs on multi-Ru sites. The Ru single-atom catalyst supported on CeO shows an ultralow CH yield of 2.2% and a liquid fuel yield of over 94.5% with a production rate of 314.93 g g h at 250 °C for 6 h. Such remarkable catalytic activity and selectivity of Ru single-atom catalyst in polyolefin hydrogenolysis offer immense opportunities for plastic upcycling.

摘要

废旧聚烯烃的催化氢解能够生产高附加值的液体燃料,因此在塑料废物再利用和环境修复方面具有巨大潜力。限制回收经济效益的主要挑战是聚烯烃链中端基C-C键断裂和碎片化引发的严重甲烷化现象(通常>20%)。在此,我们通过证明Ru单原子催化剂能够有效抑制端基C-C键断裂并防止通常在多个Ru位点发生的链碎片化,从而克服了这一挑战。负载在CeO上的Ru单原子催化剂在250℃下反应6小时,CH产率超低,仅为2.2%,液体燃料产率超过94.5%,生产率为314.93 g g h。Ru单原子催化剂在聚烯烃氢解中如此显著的催化活性和选择性为塑料升级回收提供了巨大机遇。

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