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Sequential hydrogenation of nitroaromatics to alicyclic amines via highly-dispersed Ru-Pd nanoparticles anchored on air-exfoliated C3N4 nanosheets | |
Wu, Jiale1,2,3; Wang, Liguo1,2,3,5; Xu, Shuang1; Cao, Yan1; Han, Ziqiang1; Li, Huiquan1,2,3,4 | |
2023-01-06 | |
Source Publication | RSC ADVANCES
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Volume | 13Issue:3Pages:2024-2035 |
Abstract | Developing efficient and green catalytic systems is highly desired in the syntheses of alicyclic amines via hydrogenation of nitroaromatics. Herein, we developed Ru-Pd dual active site catalysts in which Ru and Pd species were anchored and highly dispersed on air-exfoliated carbon nitride (Ru-Pd/C3N4-air). As-prepared catalysts were employed in the hydrogenation of nitrobenzene (NB) to cyclohexylamine (CHA). Compared with single Ru or Pd based catalysts, Ru-Pd dual active site catalysts obtained a higher CHA production rate of 26.7 mol CHA mol(-1) Ru center dot Pd h(-1) at 80 degrees C and 3 MPa H-2. The activation energy for the hydrogenation of the nitro group and benzene ring was calculated as 26.26 kJ mol(-1) and 66.30 kJ mol(-1), respectively. Intrinsic kinetic studies demonstrated that Pd was the dominant metal for hydrogenation of nitro group, while Ru was dominant for benzene ring. Thereinto, the corresponding non-dominant metals enhanced activation and dissociation of H-2, thereby improving catalytic activity significantly. This excellent performance of Ru-Pd catalysts could be attributed to highly dispersed Ru-N-x and Pd-N-x at a nanoscale distance, which was conducive to metal-assisted hydrogenation. Stability investigation showed that the performance of Ru-Pd catalysts could be essentially maintained at a high level. Additionally, the substrate scope could be successfully extended to hydrogenation of other nitroaromatics with different substituents. |
DOI | 10.1039/d2ra07612h |
Language | 英语 |
WOS Keyword | SITU INFRARED-SPECTROSCOPY ; SELECTIVE HYDROGENATION ; CATALYST ; CYCLOHEXYLAMINE ; NITROBENZENE ; REDUCTION |
Funding Project | Strategic Priority Research Program of the Chinese Academy of Sciences ; [XDA 29030201] |
WOS Research Area | Chemistry |
WOS Subject | Chemistry, Multidisciplinary |
Funding Organization | Strategic Priority Research Program of the Chinese Academy of Sciences |
WOS ID | WOS:000910078100001 |
Publisher | ROYAL SOC CHEMISTRY |
Citation statistics | |
Document Type | 期刊论文 |
Identifier | http://ir.ipe.ac.cn/handle/122111/56511 |
Collection | 中国科学院过程工程研究所 |
Corresponding Author | Wang, Liguo |
Affiliation | 1.Chinese Acad Sci, Inst Proc Engn, Natl Engn Res Ctr Green Recycling Strateg Met Reso, 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 |
Recommended Citation GB/T 7714 | Wu, Jiale,Wang, Liguo,Xu, Shuang,et al. Sequential hydrogenation of nitroaromatics to alicyclic amines via highly-dispersed Ru-Pd nanoparticles anchored on air-exfoliated C3N4 nanosheets[J]. RSC ADVANCES,2023,13(3):2024-2035. |
APA | Wu, Jiale,Wang, Liguo,Xu, Shuang,Cao, Yan,Han, Ziqiang,&Li, Huiquan.(2023).Sequential hydrogenation of nitroaromatics to alicyclic amines via highly-dispersed Ru-Pd nanoparticles anchored on air-exfoliated C3N4 nanosheets.RSC ADVANCES,13(3),2024-2035. |
MLA | Wu, Jiale,et al."Sequential hydrogenation of nitroaromatics to alicyclic amines via highly-dispersed Ru-Pd nanoparticles anchored on air-exfoliated C3N4 nanosheets".RSC ADVANCES 13.3(2023):2024-2035. |
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