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

IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL
Jialiang Qi, Xu Hou, Xinyao Sun, Jing Huang, Li Yin, Tingting Cui
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引用次数: 0

Abstract

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

制备Zr-Al和Zr-Mn载体调控塑料废弃物中碳纳米管生长的铁基催化剂
将塑料废弃物转化为高价值的碳材料(如碳纳米管)是可持续发展的有效策略。本文以柠檬酸为沉淀剂,采用共沉淀法制备了原子比分别为7:3和5:5的Zr-Al和Zr-Mn载体,并通过浸渍法制备了Fe/Zr7Al3、Fe/Zr5Al5、Fe/Zr7Mn3和Fe/Zr5Mn5铁基催化剂。然后,在两级固定反应器上,将fe基催化剂用于PE(聚乙烯)的热催化合成CNTs。采用SEM、XRD、N2物理吸附、H2-TPR、TG-DSC、Raman等方法对载体及新废催化剂进行了详细表征。CNTs的产率依次为Fe/Zr5Al5 (451.0 mg/g) > Fe/Zr7Al3 (367.8 mg/g) > Fe/Zr7Mn3 (284.3 mg/g) > Fe/Zr5Mn5 (51.6 mg/g)。与Fe/Zr5Al5和Fe/Zr5Mn5相比,Fe/Zr7Al3和Fe/Zr7Mn3制备的CNTs具有良好的生长结构:Fe/Zr7Al3表面的CNTs呈细长波状,外表面光滑,平均直径为30.5 nm;Fe/Zr7Mn3上的碳纳米管比Fe/Zr7Al3上的碳纳米管更长、更直,外表面更光滑,平均直径更大,为55.5 nm。此外,Fe/Zr7Al3和Fe/Zr7Mn3的独特性能可以有效调节正己烷合成碳纳米管的形貌、质量和数量。这可能是由于Zr-Al和Zr-Mn载体的不同晶体结构和还原性决定了铁基催化剂的金属-载体相互作用,从而调节了烃转化的反应途径,从而生长出不同形态、质量和数量的CNTs。图形抽象
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Catalysis Letters
Catalysis Letters 化学-物理化学
CiteScore
5.70
自引率
3.60%
发文量
327
审稿时长
1 months
期刊介绍: Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.
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