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Hydrogenation of Nitrobenzene Catalyzed by Pt Supported on Carbon Coated Nickel Magnetic Supports
Wu Yi1; Si Yang1; Huang Yanmin2; Diao Jiangyong1; Meng Fanjing2; Liu Zeng2; Liu Hongyang1
通讯作者Liu Hongyang(liuhy@imr.ac.cn)
2024-08-11
发表期刊ACTA METALLURGICA SINICA
ISSN0412-1961
卷号60期号:8页码:1141-1149
摘要Aniline is an important chemical raw material widely used in various industries, including medicine, dye manufacturing, and rubber production. Catalytic liquid-phase dhydrogenation of nitrobenzene is a main industrial production method for aniline. However, the separation and recovery of the catalyst from the liquid hydrogenation system remain challenging. Graphene-encapsulated transition-metal nanoparticles (TM@G, where TM = Fe, Co, and Ni) exhibit magnetic separability and electron transfer effects, making them widely applicable in heterogeneous catalysis. In this study, a magnetically separable catalyst support, comprising graphene-encapsulated Ni nanoparticles (Ni@NG), was developed. This support was then loaded with a Pt metal catalyst for efficient catalytic hydrogenation of nitrobenzene to aniline. To fabricate the catalyst support, ethylenediaminetetraacetic acid and Ni(OH)(2) were uniformly mixed in deionized water until the solution turned blue at 90 degrees C. The resulting blue solid precursor was then dried and annealed at 600 degrees C in argon to yield the magnetic support (Ni@NG). The support was then characterized using Raman spectroscopy, TEM, XRD, and XPS. TEM results revealed that the Ni@NG support exhibited a typical core-shell structure (with nanoscale Ni particles as the core and 2-5 layers of graphene as the shell). The Raman spectrum of the Ni@NG support exhibited the characteristic D and G bands of graphene at 1341 and 1604 cm(-1), respectively. Moreover, the XRD spectrum of this support exhibited distinct peaks corresponding to Ni and graphene, while its XPS analysis confirmed the presence of an approximate nitrogen atom concentration of 3.64% in the nitrogen-doped graphene shell. Furthermore, the deposition-precipitation method was employed to synthesize a Pt-loaded Ni@NG catalyst (Pt/ Ni@NG), which was later used in the catalytic hydrogenation of nitrobenzene in a liquid-phase reaction. Results revealed that increasing the Pt weight loading (mass fraction) from 0.1% to 0.5% altered the Pt dispersion state from single atoms to clusters and then to particles. In particular, at a Pt weight loading of 0.3%, the Pt/Ni@NG catalyst dominated by Pt clusters exhibited the highest activity for the hydrogenation of nitrobenzene. At this Pt weight loading, the catalyst achieved a turnover frequency of 27239.2 h(-1) at 1 MPa reaction pressure under 30 degrees C, completely converting nitrobenzene to aniline within 60 min. Furthermore, the Pt/Ni@NG catalyst maintained its activity over five testing cycles, attributed to its excellent liquid-phase magnetic separability.
关键词core-shell structure nitrobenzene hydrogenation magnetic separability nitrogen-doped carbon material
DOI10.11900/0412.1961.2024.00079
收录类别SCI
语种英语
WOS研究方向Metallurgy & Metallurgical Engineering
WOS类目Metallurgy & Metallurgical Engineering
WOS记录号WOS:001281277300013
出版者SCIENCE PRESS
引用统计
文献类型期刊论文
条目标识符http://ir.imr.ac.cn/handle/321006/189693
专题中国科学院金属研究所
通讯作者Liu Hongyang
作者单位1.Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, Shenyang 110016, Peoples R China
2.Cangzhou Dahua Co Ltd, Technol Innovat Ctr Modified Isocyanate Hebei Pro, Cangzhou 061000, Peoples R China
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GB/T 7714
Wu Yi,Si Yang,Huang Yanmin,et al. Hydrogenation of Nitrobenzene Catalyzed by Pt Supported on Carbon Coated Nickel Magnetic Supports[J]. ACTA METALLURGICA SINICA,2024,60(8):1141-1149.
APA Wu Yi.,Si Yang.,Huang Yanmin.,Diao Jiangyong.,Meng Fanjing.,...&Liu Hongyang.(2024).Hydrogenation of Nitrobenzene Catalyzed by Pt Supported on Carbon Coated Nickel Magnetic Supports.ACTA METALLURGICA SINICA,60(8),1141-1149.
MLA Wu Yi,et al."Hydrogenation of Nitrobenzene Catalyzed by Pt Supported on Carbon Coated Nickel Magnetic Supports".ACTA METALLURGICA SINICA 60.8(2024):1141-1149.
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