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Highly dispersed Ru anchored on nanosheet N-doped carbon for efficient and chemoselective hydrogenation of nitroaromatics to aromatic amines under mild conditions

文献类型：期刊论文

作者Yang, Huanhuan1,2,3; Wang, Liguo1,2,3,5; Xu, Shuang1; Hui, Xiang1,2,3; Cao, Yan1; He, Peng1; Li, Yang1; Li, Huiquan1,2,3,4
刊名CHEMICAL ENGINEERING JOURNAL
出版日期2022-03-01
卷号431页码:14
关键词Nanosheet N -doped carbon Nitroaromatics Aromatic amines Ru-N-x species Mild hydrogenation Stable
ISSN号1385-8947
DOI10.1016/j.cej.2021.133863
英文摘要An efficient catalyst for chemoselective hydrogenation of nitroaromatics to produce aromatic amines under mild conditions is highly desirable. In this work, a series of N-doped carbon (NC-x) with high nitrogen contents were firstly synthesized by pyrolysis of 1-butyl-3-vinylimidazolium bromide-co-acrylonitrile with a template of g-C3N4. Furthermore, Ru/NC-x catalysts were successfully prepared by ultrasonic-assisted impregnation method. The catalysts were characterized by various methods in detail, e.g.X-ray diffraction, N-2 physical adsorption-desorption, Transmission electron microscopy, Raman spectra, Scanning electron microscopy and H-2 temperature programmed reduction. Characterization results revealed that N-doping on carbon contributed to the high dispersion of Ru nanoparticles and resulted in the forming of the electron-deficient of Ru species. Nanosheet Ru/NC-2 with high N-doping content of 28 wt% exhibited superior performance under room temperature, i.e., nitrobenzene conversion > 99.0% and aniline selectivity 98.4%. Kinetic study indicated that the hydrogenation of nitrobenzene over Ru/NC-2 was the first-order kinetics with an intrinsic activation energy of 43.7 kJ/mol. Density functional theory calculation results suggested that Ru-N-x species, especially, Ru-pyrrolic-N facilitated nitrobenzene adsorption and H-2 dissociation, resulting in enhanced catalytic performance. In addition, the excellent stability of Ru/NC-2 made it essentially reserved for 410 h in the fixed-bed reactor. Moreover, Ru/NC-2 exhibited superior performance for the hydrogenation of various nitroaromatics to corresponding aromatic amines. This work could provide meaningful guidance on designing effective and stable catalyst for chemo-selective hydrogenation of nitroaromatics to aromatic amines under mild conditions.
WOS关键词LIQUID-PHASE HYDROGENATION ; SELECTIVE HYDROGENATION ; CATALYTIC-ACTIVITY ; METAL-CATALYSTS ; NANOPARTICLES ; REDUCTION ; OXIDATION ; GRAPHENE ; NITROBENZENE ; ACTIVATION
资助项目National Natural Science Foundation of China[21576272] ; Chinese Academy of Sciences[XDA 21030600] ; Science and Technology Service Network Initiative, Chinese Academy of Sciences[KFJ-STS-QYZD-138]
WOS研究方向Engineering
语种英语
WOS记录号WOS:000772843500002
出版者ELSEVIER SCIENCE SA
资助机构National Natural Science Foundation of China ; Chinese Academy of Sciences ; Science and Technology Service Network Initiative, Chinese Academy of Sciences
源URL[http://ir.ipe.ac.cn/handle/122111/52555]  
专题中国科学院过程工程研究所
通讯作者Wang, Liguo; Li, Huiquan
作者单位1.Chinese Acad Sci, Natl Engn Res Ctr Green Recycling Strateg Met Res, Inst Proc Engn, Key Lab Green Proc & Engn, Beijing 100190, Peoples R China
2.Univ Chinese Acad Sci, Sino Danish Coll, Beijing 100049, Peoples R China
3.Univ Chinese Acad Sci, Sino Danish Ctr Educ & Res, Beijing 100049, Peoples R China
4.Univ Chinese Acad Sci, Sch Chem Engn, Beijing 100049, Peoples R China
5.Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
推荐引用方式
GB/T 7714		 Yang, Huanhuan,Wang, Liguo,Xu, Shuang,et al. Highly dispersed Ru anchored on nanosheet N-doped carbon for efficient and chemoselective hydrogenation of nitroaromatics to aromatic amines under mild conditions[J]. CHEMICAL ENGINEERING JOURNAL,2022,431:14.
APA Yang, Huanhuan.,Wang, Liguo.,Xu, Shuang.,Hui, Xiang.,Cao, Yan.,...&Li, Huiquan.(2022).Highly dispersed Ru anchored on nanosheet N-doped carbon for efficient and chemoselective hydrogenation of nitroaromatics to aromatic amines under mild conditions.CHEMICAL ENGINEERING JOURNAL,431,14.
MLA Yang, Huanhuan,et al."Highly dispersed Ru anchored on nanosheet N-doped carbon for efficient and chemoselective hydrogenation of nitroaromatics to aromatic amines under mild conditions".CHEMICAL ENGINEERING JOURNAL 431(2022):14.

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来源：过程工程研究所

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