Morphology-tuned MnOx/TiO2 nanocatalysts for recycling PET plastic waste using biomass-derived ethylene glycol†

IF 5.1 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Nanoscale Pub Date : 2025-02-10 DOI:10.1039/D4NR05373G
Bhattu Swapna, Madam Bobby Barnabas, Pragya Moni Gogoi, Pankaj Bharali, Giridhar Madras and Putla Sudarsanam
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Abstract

This study presents a decisive role of TiO2 morphology on the catalytic activity of MnOx/TiO2 nanomaterials for the chemical recycling of PET waste bottles using biomass-derived ethylene glycol to produce a valuable monomer, bis(2-hydroxyethyl) terephthalate (BHET). Three types of MnOx/TiO2 nanocatalysts were prepared by varying the TiO2 morphology (nanosheets: NS, nanotubes: NT, and nanorods: NR). The combination of MnOx nanoparticles and TiO2 nanorods (MnOx/TiO2-NR) showed significantly enhanced catalytic activity in PET glycolysis, with a 91% isolated yield of BHET at 190 °C in 3 h, whereas 74% and 82% yields of BHET were attained with MnOx/TiO2-NS and MnOx/TiO2-NT nanocatalysts, respectively. The morphology of TiO2 and the uniform dispersion of MnOx on TiO2-NR were confirmed by electron microscopic analysis. The MnOx/TiO2-NR catalyst contains optimum basic sites, which play a key role, along with surface hydroxyl species and Mn3+/Mn2+ species, in activating ethylene glycol and PET/its oligomers towards BHET formation. The excellent stability of the MnOx/TiO2-NR nanocatalyst, as confirmed by the hot-filtration test, good catalytic reusability up to four cycles, non-toxic nature, and the low cost of the MnOx/TiO2 materials indicate the practical feasibility of the developed catalytic protocol for the plastic recycling industry.

Abstract Image

形貌调谐MnOx/TiO2纳米催化剂用于生物质衍生乙二醇回收PET塑料废物
本研究展示了TiO2的形态对MnOx/TiO2纳米材料催化活性的决定性作用,该纳米材料用于化学回收PET废弃瓶,利用生物质衍生的乙二醇生产有价值的单体,双(2-羟乙基)对苯二甲酸乙二醇酯(BHET)。通过改变TiO2的形态(纳米片:NS,纳米管:NT,纳米棒:NR),制备了三种MnOx/TiO2纳米催化剂。MnOx纳米颗粒和TiO2纳米棒(MnOx/TiO2- nr)的组合在PET糖酵解过程中表现出显著增强的催化活性,在190℃条件下3 h分离得到BHET的产率为91%,而MnOx/TiO2- ns和MnOx/TiO2- nt纳米催化剂分别获得了74%和82%的BHET产率。电镜分析证实了TiO2的形貌和MnOx在TiO2- nr上的均匀分散。MnOx/TiO2-NR催化剂含有最佳碱性位点,与表面羟基和Mn3+/Mn2+物质一起,在激活乙二醇和PET/其低聚物形成BHET方面发挥了关键作用。热过滤试验证实,MnOx/TiO2- nr纳米催化剂具有优异的稳定性,催化可重复使用4次,MnOx/TiO2材料的无毒性和低成本表明,所开发的催化方案在塑料回收行业具有实际可行性。
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来源期刊
Nanoscale
Nanoscale CHEMISTRY, MULTIDISCIPLINARY-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
12.10
自引率
3.00%
发文量
1628
审稿时长
1.6 months
期刊介绍: Nanoscale is a high-impact international journal, publishing high-quality research across nanoscience and nanotechnology. Nanoscale publishes a full mix of research articles on experimental and theoretical work, including reviews, communications, and full papers.Highly interdisciplinary, this journal appeals to scientists, researchers and professionals interested in nanoscience and nanotechnology, quantum materials and quantum technology, including the areas of physics, chemistry, biology, medicine, materials, energy/environment, information technology, detection science, healthcare and drug discovery, and electronics.
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