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聚乙烯在Co-MCM-41催化剂上氧化升级为长链二酸

Oxidative Upcycling of Polyethylene to Long Chain Diacid over Co-MCM-41 Catalyst.

作者信息

Zhang Qiang, He Jiajia, Wei Xiangyue, Shen Chengfeng, Ye Pengbo, An Wenli, Liu Xuehui, Li Haoze, Xu Shimei, Su Zhishan, Wang Yu-Zhong

机构信息

The Collaborative Innovation Center for Eco-Friendly and Fire-Safety Polymeric Materials (MoE), State Key Laboratory of Polymer Materials Engineering, National Engineering Laboratory of Eco-Friendly Polymeric Materials (Sichuan), College of Chemistry, Sichuan University, Chengdu, 610064, China.

Key Laboratory of Green Chemistry and Technology, Ministry of Education, College of Chemistry Sichuan University, Chengdu, Sichuan, 610064, P.R. China.

出版信息

Angew Chem Int Ed Engl. 2024 Aug 12;63(33):e202407510. doi: 10.1002/anie.202407510. Epub 2024 Jul 10.

Abstract

Plastic pollution is an emerging global threat due to lack of effective methods for transforming waste plastics into useful resources. Here, we demonstrate a direct oxidative upcycling of polyethylene into high-value and high-volume saturated dicarboxylic acids in high carbon yield of 85.9 % in which the carbon yield of long chain dicarboxylic (C10-C20) acids can reach 58.9% over cobalt-doped MCM-41 molecular sieves, in the absence of any solvent or precious metal catalyst. The distribution of the dicarboxylic acids can be controllably adjusted from short-chain (C4-C10) to long-chain ones (C10-C20) through changing cobalt loading of MCM-41 under nanoconfinement. Highly and sparsely dispersed cobalt along with confined space of mesoporous structure enables complete degradation of polyethylene and high selectivity of dicarboxylic acid in mild condition. So far, this is the first report on highly selective one-step preparation of long chain dicarboxylic acids. The approach provides an attractive solution to tackle plastic pollution and a promising alternative route to long chain diacids.

摘要

由于缺乏将废塑料转化为有用资源的有效方法,塑料污染正成为一种新出现的全球威胁。在此,我们展示了一种将聚乙烯直接氧化升级循环为高价值、高产量饱和二元羧酸的方法,其碳产率高达85.9%,其中在无任何溶剂或贵金属催化剂的情况下,钴掺杂的MCM-41分子筛上长链二元羧酸(C10-C20)的碳产率可达58.9%。通过在纳米限域条件下改变MCM-41的钴负载量,二元羧酸的分布可从短链(C4-C10)可控地调节为长链(C10-C20)。高度分散且稀疏分布的钴以及介孔结构的限域空间使得聚乙烯在温和条件下能完全降解,且二元羧酸具有高选择性。到目前为止,这是关于高选择性一步制备长链二元羧酸的首次报道。该方法为解决塑料污染提供了一个有吸引力的方案,也是长链二酸一条有前景的替代路线。

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