Catalytic recycling of PET waste bottles into a value-added amide monomer using a heterogeneous niobium pentoxide nanocatalyst†

IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Sustainable Energy & Fuels Pub Date : 2024-10-02 DOI:10.1039/D4SE01136H
Bhattu Swapna, Suresh Babu Putla, Asha Ramesh, Challapalli Subrahmanyam, Giridhar Madras and Putla Sudarsanam
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Abstract

Using a diverse heterogeneous nanocatalyst, aminolysis represents a promising approach for the chemical recycling of discarded PET waste bottles into a valuable monomer bis(2-hydroxyethyl) terephthalamide (BHETA). This study reports the solution combustion synthesis of a nanostructured Nb2O5 material for the catalytic aminolysis of PET waste bottles using ethanolamine. The Nb2O5 nanocatalyst calcined at 450 °C (Nb2O5-450) exhibited robust catalytic performance with a 92% isolated yield of the BHETA monomer and complete PET conversion under mild conditions compared with several homogeneous and heterogeneous catalysts. The Nb2O5-450 nanocatalyst has a unique morphology with both nanosheet and nanorod particles. The Nb2O5-450 nanocatalyst, possessing strong acid sites and more oxygen vacancies as estimated by NH3-TPD and O 1s XPS analyses, respectively, induced electron deficiency in the carbonyl carbon of PET. This electron-deficient characteristic facilitated the aminolysis reaction, wherein ethanolamine attacked the carbonyl carbon, initiating the reaction toward the formation of BHETA. The purity and structure of BHETA were confirmed through NMR, FT-IR, TGA/DSC, and powder XRD techniques. The 1 wt% Nb2O5 catalyst exhibited reasonably good catalytic reusability for up to five cycles. The characterization of the Nb2O5-450 nanocatalyst before and after the reaction highlighted its structural stability, affirming the sustainable nature of the catalyst for valorizing PET waste into value-added monomers.

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利用异相五氧化二铌纳米催化剂催化回收 PET 废瓶,将其转化为高附加值的酰胺单体†。
利用多种异质纳米催化剂,氨解是将废弃 PET 废瓶转化为有价值单体双(2-羟乙基)对苯二甲酰胺(BHETA)的一种很有前景的化学回收方法。本研究报告了利用乙醇胺催化氨解 PET 废瓶的纳米 Nb2O5 材料的溶液燃烧合成方法。与几种均相和异相催化剂相比,在 450 °C 煅烧的 Nb2O5 纳米催化剂(Nb2O5-450)表现出强劲的催化性能,在温和条件下,BHETA 单体的分离产率达到 92%,并实现了 PET 的完全转化。Nb2O5-450 纳米催化剂具有独特的形态,既有纳米片状颗粒,也有纳米棒状颗粒。根据 NH3-TPD 和 O 1s XPS 分析,Nb2O5-450 纳米催化剂具有强酸性位点和更多的氧空位,可诱导 PET 的羰基碳缺电子。这种缺电子特性促进了氨解反应,其中乙醇胺攻击羰基碳,引发了生成 BHETA 的反应。通过 NMR、FT-IR、TGA/DSC 和粉末 XRD 技术确认了 BHETA 的纯度和结构。1 wt% Nb2O5 催化剂表现出相当好的催化重复使用性,可循环使用长达五个周期。对 Nb2O5-450 纳米催化剂在反应前后的表征突显了其结构的稳定性,从而肯定了该催化剂在将 PET 废料转化为高附加值单体方面的可持续性。
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来源期刊
Sustainable Energy & Fuels
Sustainable Energy & Fuels Energy-Energy Engineering and Power Technology
CiteScore
10.00
自引率
3.60%
发文量
394
期刊介绍: Sustainable Energy & Fuels will publish research that contributes to the development of sustainable energy technologies with a particular emphasis on new and next-generation technologies.
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Back cover Back cover Recent advances and opportunities in perovskite-based triple-junction tandem solar cells Enhanced thermoelectric properties of Cu1.8S via the introduction of ZnS nanostructures† Back cover
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