Jialiang Qi, Xu Hou, Xinyao Sun, Jing Huang, Li Yin, Tingting Cui
{"title":"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","authors":"Jialiang Qi, Xu Hou, Xinyao Sun, Jing Huang, Li Yin, Tingting Cui","doi":"10.1007/s10562-025-05036-2","DOIUrl":null,"url":null,"abstract":"<div><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 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.</p><h3>Graphical abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 6","pages":""},"PeriodicalIF":2.3000,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Fabricating Zr-Al and Zr-Mn Supports for Fe-based Catalysts To Regulate CNTs Growth from Plastic Wastes\",\"authors\":\"Jialiang Qi, Xu Hou, Xinyao Sun, Jing Huang, Li Yin, Tingting Cui\",\"doi\":\"10.1007/s10562-025-05036-2\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><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 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.</p><h3>Graphical abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":508,\"journal\":{\"name\":\"Catalysis Letters\",\"volume\":\"155 6\",\"pages\":\"\"},\"PeriodicalIF\":2.3000,\"publicationDate\":\"2025-05-02\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Letters\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s10562-025-05036-2\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Letters","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s10562-025-05036-2","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Fabricating Zr-Al and Zr-Mn Supports for Fe-based Catalysts To Regulate CNTs Growth from Plastic Wastes
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.
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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