N. Goujon, Jérémy Demarteau, Xabier Lopez de Pariza, N. Casado, H. Sardón, D. Mecerreyes
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The initial cyclic voltammetry results of the depolymerization product of PET used as a model compound show a reversible redox process, when using a 0.1 M tetrabutylammonium hexafluorophosphate/dimethyl sulfoxide electrolyte system, with a standard redox potential of −2.12 V vs. Fc/Fc+. Finally, the cycling performance of terephthalate nanoparticles was investigated using a 0.1 M TBAPF6 solution in acetonitrile as electrolyte in a three-electrode cell. The terephthalate anode electrode displays good cycling stability and performance at high C-rate (i.e., ≥5C), delivering a stable specific discharge capacity of 32.8 mAh.g−1 at a C-rate of 30 C, with a capacity retention of 94% after 100 cycles. 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引用次数: 4
摘要
每年生产超过3000万吨的聚对苯二甲酸乙酯(PET),由于机械回收过程中材料性能的恶化,所有PET瓶的回收利用率不超过60%。本文提出了一种可持续的方法,通过化学升级回收聚对苯二甲酸乙酯(PET)废物来生产具有氧化还原活性的纳米颗粒,用于储能。通过对PET解聚产物(即双羟基(2-乙基)对苯二甲酸乙酯,BHET)进行简单的甲基丙烯酸酯功能化得到的甲基丙烯酸酯-对苯二甲酸乙酯单体进行乳液聚合,制备了尺寸小于100 nm的氧化还原活性纳米颗粒。当使用0.1 M四丁基六氟磷酸铵/二甲亚砜电解质体系,标准氧化还原电位为- 2.12 V vs. Fc/Fc+时,作为模型化合物的PET解聚产物的初始循环伏安法结果表明,其氧化还原过程是可逆的。最后,以0.1 M TBAPF6溶液为电解液,在三电极电池中研究了对苯二甲酸盐纳米颗粒的循环性能。对苯二甲酸盐阳极电极在高倍率(即≥5C)下具有良好的循环稳定性和性能,稳定的比放电容量为32.8 mAh。g−1在C率为30℃时,循环100次后容量保持率为94%。然而,在较低的c速率(即≤2C)下,观察到比放电和充电容量之间的大滞后和容量衰减,这表明与对苯二甲酸酯部分相关的氧化还原反应存在一些不可逆性,特别是与氧化过程有关。
Chemical Upcycling of PET Waste towards Terephthalate Redox Nanoparticles for Energy Storage
Over 30 million ton of poly(ethylene terephthalate) (PET) is produced each year and no more than 60% of all PET bottles are reclaimed for recycling due to material property deteriorations during the mechanical recycling process. Herein, a sustainable approach is proposed to produce redox-active nanoparticles via the chemical upcycling of poly(ethylene terephthalate) (PET) waste for application in energy storage. Redox-active nanoparticles of sizes lower than 100 nm were prepared by emulsion polymerization of a methacrylic-terephthalate monomer obtained by a simple methacrylate functionalization of the depolymerization product of PET (i.e., bis-hydroxy(2-ethyl) terephthalate, BHET). The initial cyclic voltammetry results of the depolymerization product of PET used as a model compound show a reversible redox process, when using a 0.1 M tetrabutylammonium hexafluorophosphate/dimethyl sulfoxide electrolyte system, with a standard redox potential of −2.12 V vs. Fc/Fc+. Finally, the cycling performance of terephthalate nanoparticles was investigated using a 0.1 M TBAPF6 solution in acetonitrile as electrolyte in a three-electrode cell. The terephthalate anode electrode displays good cycling stability and performance at high C-rate (i.e., ≥5C), delivering a stable specific discharge capacity of 32.8 mAh.g−1 at a C-rate of 30 C, with a capacity retention of 94% after 100 cycles. However, a large hysteresis between the specific discharge and charge capacities and capacity fading are observed at lower C-rate (i.e., ≤2C), suggesting some irreversibility of redox reactions associated with the terephthalate moiety, in particular related to the oxidation process.