Photothermal Catalytic Polyester Upcycling over Cobalt Single‐Site Catalyst
Photothermal Catalytic Polyester Upcycling over Cobalt Single‐Site Catalyst
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DOI：
10.1002/adfm.202210283
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发表时间：
2022-10
影响因子：
19
通讯作者：
Yu Liu;Xuchun Wang;Qingye Li;Tianran Yan;Xiangxi Lou;Congyang Zhang;Muhan Cao;Liang Zhang
中科院分区：
文献类型：
--
作者：
Yu Liu;Xuchun Wang;Qingye Li;Tianran Yan;Xiangxi Lou;Congyang Zhang;Muhan Cao;Liang Zhang
利用可再生太阳能将废塑料光热催化转化为燃料和/或原料，可以同时实现太阳能到化学物质的转化、资源可持续性和环境修复。然而，构建具有强光吸收和高催化活性的光热催化剂仍然是一个巨大的挑战。在这项工作中，集成的钴单中心催化剂（Co SSC）具有强光热转化、高催化活性和稳定性，用于催化聚酯的糖酵解。独特的配位不饱和Co-O5单中心可以与聚酯中的羰基配位，从而促进亲核加成消除过程。因此，Co SSCs 的时空产率比一般催化剂高一个数量级。此外，在相同条件下，光热催化的聚对苯二甲酸乙二醇酯（PET）转化率和对苯二甲酸双（2-羟乙基）酯产率分别比热催化高5.4和6.6倍，这得益于局部加热效应。技术经济分析表明，光热催化回收105吨废PET，消耗电能146.4GW·h，少排放CO2 7.44×104吨。因此，高效光热催化塑料回收系统对于废旧塑料资源化具有重要意义。
Photothermal catalytic conversion of waste plastics into fuels and/or feedstocks using renewable solar energy can achieve solar‐to‐chemical conversion, resource sustainability, and environmental remediation simultaneously. However, the construction of photothermal catalysts with strong light absorption and high catalytic activity remains a great challenge. In this work, integrated cobalt single‐site catalysts (Co SSCs), coupled with strong photothermal conversion, high catalytic activity, and stability, are employed to catalyze the glycolysis of polyesters. The unique coordination‐unsaturated CoO5 single‐site can coordinate with the carbonyl groups in polyester, thus boosting the nucleophilic addition elimination processes. As a result, the space‐time yield of Co SSCs is an order of magnitude higher than that of general catalysts. In addition, the polyethylene terephthalate (PET) conversion and bis(2‐hydroxyethyl) terephthalate yield in photothermal catalysis are 5.4 and 6.6 times higher than those of thermal catalysis under the same conditions, which are contributed by the localized heating effect. Technical economic analysis shows that the recycling of 105 tons of waste PET by photothermal catalysis consumes 146.4 GW·h electrical energy and misses 7.44 × 104 tons of CO2 emission. Therefore, a high‐efficient photothermal catalytic plastic recycling system is of great significance for waste plastic valorization.