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将聚对苯二甲酸乙二酯和一氧化碳催化转化为高价值化学品。

Catalytic Transformation of PET and CO into High-Value Chemicals.

作者信息

Li Yinwen, Wang Meng, Liu Xingwu, Hu Chaoquan, Xiao Dequan, Ma Ding

机构信息

Beijing National Laboratory for Molecular Sciences, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, P. R. China.

State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences Taiyuan, Shanxi, 030001, P. R. China.

出版信息

Angew Chem Int Ed Engl. 2022 Mar 1;61(10):e202117205. doi: 10.1002/anie.202117205. Epub 2022 Jan 24.

Abstract

Polyethylene terephthalate (PET) and CO , two chemical wastes that urgently need to be transformed in the environment, are converted simultaneously in a one-pot catalytic process through the synergistic coupling of three reactions: CO hydrogenation, PET methanolysis and dimethyl terephthalate (DMT) hydrogenation. More interestingly, the chemical equilibria of both reactions were shifted forward due to a revealed dual-promotion effect, leading to significantly enhanced PET depolymerization. The overall methanol yield from CO hydrogenation exceeded the original thermodynamic equilibrium limit since the methanol was in situ consumed in the PET methanolysis. The degradation of PET by a stoichiometric ratio of methanol was significantly enhanced because the primary product, DMT was hydrogenated to dimethyl cyclohexanedicarboxylate (DMCD) or p-xylene (PX). This synergistic catalytic process provides an effective way to simultaneously recycle two wastes, polyesters and CO , for producing high-value chemicals.

摘要

聚对苯二甲酸乙二酯(PET)和一氧化碳(CO)是两种急需在环境中转化的化学废物,它们通过一氧化碳加氢、PET甲醇解和对苯二甲酸二甲酯(DMT)加氢这三个反应的协同耦合,在一锅催化过程中同时被转化。更有趣的是,由于揭示出的双重促进作用,两个反应的化学平衡都正向移动,导致PET解聚显著增强。由于甲醇在PET甲醇解中被原位消耗,一氧化碳加氢产生的甲醇总产率超过了原来的热力学平衡极限。由于初级产物DMT被氢化为环己烷二甲酸二甲酯(DMCD)或对二甲苯(PX),按化学计量比的甲醇对PET的降解显著增强。这种协同催化过程为同时回收两种废物——聚酯和一氧化碳,以生产高价值化学品提供了一种有效方法。

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