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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 PublicationRSC ADVANCES
Volume13Issue:3Pages:2024-2035
AbstractDeveloping 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.
DOI10.1039/d2ra07612h
Language英语
WOS KeywordSITU INFRARED-SPECTROSCOPY ; SELECTIVE HYDROGENATION ; CATALYST ; CYCLOHEXYLAMINE ; NITROBENZENE ; REDUCTION
Funding ProjectStrategic Priority Research Program of the Chinese Academy of Sciences ; [XDA 29030201]
WOS Research AreaChemistry
WOS SubjectChemistry, Multidisciplinary
Funding OrganizationStrategic Priority Research Program of the Chinese Academy of Sciences
WOS IDWOS:000910078100001
PublisherROYAL SOC CHEMISTRY
Citation statistics
Document Type期刊论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/56511
Collection中国科学院过程工程研究所
Corresponding AuthorWang, Liguo
Affiliation1.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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