Quantitative Electrocatalytic Upcycling of Polyethylene Terephthalate Plastic and Its Oligomer with a Cobalt-Based One-Dimensional Coordination Polymer Having Open Metal Sites along with Coproduction of Hydrogen,ACS Catalysis

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Quantitative Electrocatalytic Upcycling of Polyethylene Terephthalate Plastic and Its Oligomer with a Cobalt-Based One-Dimensional Coordination Polymer Having Open Metal Sites along with Coproduction of Hydrogen
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-12-20 , DOI: 10.1021/acscatal.2c05270
Snehanjali Behera ₁ , Soumitra Dinda ₁ , Rajat Saha ₂ , Biswajit Mondal ₁

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Polyethylene terephthalate (PET) is the most used polymer, but its natural degradation kinetics is sluggish; therefore, its disposal poses an environmental threat. Here, we demonstrate electrocatalytic PET upcycling with full recyclability with a cobalt containing one-dimensional (1D) coordination polymer as an electrocatalyst that can operate at a low onset potential of 1.27 V vs. RHE, affording terephthalic acid (TPA) in 100% yield and potassium diformate (KDF) with ∼80% selectivity as isolated products, along with the coproduction of hydrogen. The mechanistic analysis, as obtained from systematic studies with PET, its oligomer, and monomer revealed a pathway for a side reaction generating carbonate (CO₃^2–) that follows a formate oxidation instead of an oxalate oxidation pathway. The catalytic performance and the mechanistic insight gained from the study, are useful in developing the PET upcycling technologies with maximized formate/KDF production.

中文翻译：

聚对苯二甲酸乙二醇酯塑料及其低聚物与具有开放金属位点的钴基一维配位聚合物的定量电催化升级循环并联产氢气

聚对苯二甲酸乙二醇酯 (PET) 是最常用的聚合物，但其自然降解动力学缓慢；因此，它的处置会对环境造成威胁。在这里，我们展示了具有完全可回收性的电催化 PET 升级回收，使用含钴的一维 (1D) 配位聚合物作为电催化剂，可以在相对于 RHE 1.27 V 的低起始电位下运行，以 100% 的收率提供对苯二甲酸 (TPA)和二甲酸钾 (KDF) 作为分离产物具有约 80% 的选择性，以及氢气的联产。从对 PET、其低聚物和单体的系统研究中获得的机理分析揭示了副反应生成碳酸盐 (CO ₃^2–) 遵循甲酸盐氧化而不是草酸盐氧化途径。从研究中获得的催化性能和机理洞察力有助于开发 PET 升级回收技术，最大限度地提高甲酸盐/KDF 的产量。

更新日期：2022-12-20

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