Polyethylene Terephthalate Deconstruction Catalyzed by a Carbon-Supported Single-Site Molybdenum-Dioxo Complex
Polyethylene Terephthalate Deconstruction Catalyzed by a Carbon-Supported Single-Site Molybdenum-Dioxo Complex
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DOI：
10.1002/anie.202007423
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发表时间：
2020-09-15
影响因子：
16.6
通讯作者：
Marks, Tobin J.
中科院分区：
文献类型：
--
作者：
Kratish, Yosi;Li, Jiaqi;Marks, Tobin J.
聚对苯二甲酸乙二醇酯(PET)在碳负载的单位二氧化钼催化剂上选择性解聚为对苯二甲酸(PTA)和乙烯。在氢气气氛下，无溶剂反应效率最高。该催化剂具有很高的稳定性，可以多次循环使用而不会失去活性。废弃的饮料瓶PET或PET+PP混合物(模拟瓶子+盖子)在260℃下进行完全的PET分解和定量的PTA分离。对模型双酯1，2-乙二醇二苯甲酸酯的机理研究表明，该反应是通过最初的逆氢-烷氧基化/β-C-O断裂和随后的苯甲酸乙烯酯中间体的氢解进行的。
Polyethylene terephthalate (PET) is selectively depolymerized by a carbon-supported single-site molybdenum-dioxo catalyst to terephthalic acid (PTA) and ethylene. The solventless reactions are most efficient under 1 atmosphere of H-2. The catalyst exhibits high stability and can be recycled multiple times without loss of activity. Waste beverage bottle PET or a PET + polypropylene (PP) mixture (simulating the bottle + cap) proceeds at 260 degrees C with complete PET deconstruction and quantitative PTA isolation. Mechanistic studies with a model diester, 1,2-ethanediol dibenzoate, suggest the reaction proceeds by initial retro-hydroalkoxylation/beta-C-O scission and subsequent hydrogenolysis of the vinyl benzoate intermediate.