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<p>Upgrading plastic wastes into high-value carbon materials such as carbon nanotubes (CNTs) is an efficient strategy for the sustainable development. Herein, Zr-Al and Zr-Mn supports with an atom ratio of 7:3 and 5:5 were prepared via the co-precipitation method using citric acid as the precipitant, and used to fabricate Fe-based catalysts (Fe/Zr7Al3, Fe/Zr5Al5, Fe/Zr7Mn3 and Fe/Zr5Mn5) via the impregnation method. Then, the Fe-based catalysts were used in CNTs synthesis from PE (polyethylene) via the thermo-catalytic process on a two-stage fixed reactor. The supports as well as the fresh and spent catalysts were characterized in detail by SEM, XRD, N<sub>2</sub> physisorption, H<sub>2</sub>-TPR, TG-DSC, Raman, etc. It was found that CNTs yield was in an order of Fe/Zr5Al5 (451.0&#xa0;mg/g) &gt; Fe/Zr7Al3 (367.8&#xa0;mg/g) &gt; Fe/Zr7Mn3 (284.3&#xa0;mg/g) &gt; Fe/Zr5Mn5 (51.6&#xa0;mg/g). Compared with Fe/Zr5Al5 and Fe/Zr5Mn5, the CNTs obtained by Fe/Zr7Al3 and Fe/Zr7Mn3 exhibited the well-grown structure: The CNTs on Fe/Zr7Al3 was in an elongated and waved shape with smooth external surface and an average diameter of 30.5&#xa0;nm; the CNTs on Fe/Zr7Mn3 was longer and straighter than that of Fe/Zr7Al3, and had a smoother external surface and a larger average diameter of 55.5&#xa0;nm. In addition, the unique capability of Fe/Zr7Al3 and Fe/Zr7Mn3 was effective in regulating the morphology, quality and quantity of CNTs synthesis from n-hexane. This can be attributed to different crystal structure and reducibility of Zr-Al and Zr-Mn supports that tailored the metal-support interaction of Fe-based catalysts, which regulated the reaction pathways for hydrocarbon transformation, and thus CNTs growth with different morphology, quality and quantity.</p> Graphical abstract <p></p>

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Fabricating Zr-Al and Zr-Mn Supports for Fe-based Catalysts To Regulate CNTs Growth from Plastic Wastes

  • 期刊论文

  • 发表日期：

    2025年5月2日

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  • Jialiang Qi,
  • Xu Hou,
  • Xinyao Sun,
  • Jing Huang,
  • Li Yin,
  • Tingting Cui

摘要

Upgrading plastic wastes into high-value carbon materials such as carbon nanotubes (CNTs) is an efficient strategy for the sustainable development. Herein, Zr-Al and Zr-Mn supports with an atom ratio of 7:3 and 5:5 were prepared via the co-precipitation method using citric acid as the precipitant, and used to fabricate Fe-based catalysts (Fe/Zr7Al3, Fe/Zr5Al5, Fe/Zr7Mn3 and Fe/Zr5Mn5) via the impregnation method. Then, the Fe-based catalysts were used in CNTs synthesis from PE (polyethylene) via the thermo-catalytic process on a two-stage fixed reactor. The supports as well as the fresh and spent catalysts were characterized in detail by SEM, XRD, N2 physisorption, H2-TPR, TG-DSC, Raman, etc. It was found that CNTs yield was in an order of Fe/Zr5Al5 (451.0 mg/g) > Fe/Zr7Al3 (367.8 mg/g) > Fe/Zr7Mn3 (284.3 mg/g) > Fe/Zr5Mn5 (51.6 mg/g). Compared with Fe/Zr5Al5 and Fe/Zr5Mn5, the CNTs obtained by Fe/Zr7Al3 and Fe/Zr7Mn3 exhibited the well-grown structure: The CNTs on Fe/Zr7Al3 was in an elongated and waved shape with smooth external surface and an average diameter of 30.5 nm; the CNTs on Fe/Zr7Mn3 was longer and straighter than that of Fe/Zr7Al3, and had a smoother external surface and a larger average diameter of 55.5 nm. In addition, the unique capability of Fe/Zr7Al3 and Fe/Zr7Mn3 was effective in regulating the morphology, quality and quantity of CNTs synthesis from n-hexane. This can be attributed to different crystal structure and reducibility of Zr-Al and Zr-Mn supports that tailored the metal-support interaction of Fe-based catalysts, which regulated the reaction pathways for hydrocarbon transformation, and thus CNTs growth with different morphology, quality and quantity.

Graphical abstract