Enhanced tandem hydrogenation of nitroaromatics to alicyclic amines via Pt-Ru synergistic catalysis

被引:0
|
作者
Wu, Jiale [1 ,2 ,3 ]
Zhang, Jiajun [1 ]
Wang, Liguo [1 ,2 ,3 ]
Han, Ziqiang [1 ]
Hui, Xiang [1 ]
Cao, Yan [1 ]
Shi, Jianhui [1 ]
Xu, Shuang [1 ]
He, Peng [1 ]
Li, Huiquan [1 ,2 ,3 ,4 ]
机构
[1] Chinese Acad Sci, Inst Proc Engn, Natl Engn Res Ctr Green Recycling Strateg Met Reso, CAS 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
基金
中国国家自然科学基金;
关键词
Nitroaromatics; Tandem hydrogenation; Alicyclic amines; Hydrogen spillover; Bimetal catalysts; SITU INFRARED-SPECTROSCOPY; CHEMOSELECTIVE HYDROGENATION; MESOPOROUS CARBON; CYCLOHEXYLAMINE; NITROBENZENE; ASSIGNMENTS; ANILINE; INSIGHT;
D O I
10.1016/j.cej.2024.151083
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Green production of alicyclic amines is highly desirable but of great challenges. Herein, an efficient one-pot synthesis of alicyclic amines from nitroaromatics was realized with a Pt-Ru bimetallic catalyst. 0.5 %Pt-2.5 % Ru supported on an air-exfoliated C3N4 nanosheet achieved 100.0 % conversion of nitrobenzene (NB) with 98.9 % selectivity of cyclohexylamine (CHA) under mild conditions of 80 degrees C and 1 MPa, attaining a yield rate for alicyclic amine of 357.9 mmol/gmetal & sdot;h. Our study has shown hydrogenation of nitro group and aromatic ring took place in sequence over Pt and Ru in a tandem manner due to the highly selective adsorption. During the hydrogenation, the homolytic dissociation of H2 occurred on the bimetal sites and the inter-site hydrogen spillover between the bimetal played a crucial role. C3N4 nanosheet as the support not only gave rise to the uniform dispersion of metal nanoparticles, but was crucial in curbing the unnecessary adsorption of intermediate aromatic amines. Our study has also demonstrated the good stability and wide applicability of the Pt-Ru/C3N4-air catalyst for the hydrogenation of various nitroaromatic derivatives.
引用
收藏
页数:13
相关论文
共 50 条
  • [41] Rationally constructing hollow N-doped carbon supported Ru catalysts for enhanced hydrogenation catalysis
    Liu, Tiantian
    Li, Jing
    Yan, Xiaorui
    Li, Kairui
    Wang, Wenhua
    Wei, Haisheng
    [J]. NEW JOURNAL OF CHEMISTRY, 2024, 48 (13) : 5649 - 5657
  • [42] Synergistic effect in heterogeneously catalyzed reduction of U(VI) and Np(V) and decomposition of hydrazine and oxalic acid with bimetallic Pt-Ru catalysts
    M. S. Tyumentsev
    A. V. Anan’ev
    A. A. Shiryaev
    T. P. Puryaeva
    Ya. V. Zubavichus
    B. G. Ershov
    [J]. Doklady Physical Chemistry, 2013, 450 : 142 - 145
  • [43] Engineering the geometric and electronic structure of Ru via Ru-TiO2 interaction for enhanced selective hydrogenation
    Zhou, Qiang
    Zhao, Zijiang
    Yao, Zihao
    Wei, Zhongzhe
    Huang, Songtao
    Shao, Fangjun
    Li, Aiyuan
    Wang, Jianguo
    [J]. CATALYSIS SCIENCE & TECHNOLOGY, 2022, 12 (03) : 1005 - 1016
  • [44] Synthesis and structural characterization of a highly ordered mesoporous Pt-Ru alloy via "evaporation-mediated direct templating"
    Yamauchi, Yusuke
    Ohsuna, Tetsu
    Kuroda, Kazuyuki
    [J]. CHEMISTRY OF MATERIALS, 2007, 19 (06) : 1335 - 1342
  • [45] Metal-acid site synergistic catalysis in Ru-ZrO2 toward selective hydrogenation of benzene to cyclohexene
    Rao, Deming
    Xue, Xiaoge
    Cui, Guoqing
    He, Shan
    Xu, Ming
    Bing, Weihan
    Shi, Shuxian
    Wei, Min
    [J]. CATALYSIS SCIENCE & TECHNOLOGY, 2018, 8 (01) : 236 - 243
  • [46] Advanced photothermal synergistic catalysis of Ru-doped Ni/ZrO2 in hydrogenation of CO2
    Wang, Weiguo
    Ding, Xin
    Liu, Yuhao
    Li, Tengfei
    Cheng, Jiahui
    Li, Dan
    Guo, Yang
    [J]. JOURNAL OF MATERIALS SCIENCE, 2024, 59 (38) : 18062 - 18078
  • [47] Pt-Ru bimetallic nanoparticles anchored on carbon nanotubes/polyaniline composites with coral-like structure for enhanced methanol oxidation
    Zhang, Xiaoling
    Yan, Ruiwen
    Zhou, Wenchang
    Zhou, Sijie
    [J]. JOURNAL OF ALLOYS AND COMPOUNDS, 2022, 920
  • [48] Ultrahigh Bifunctional Photocatalytic CO2 Reduction and H2 Evolution by Synergistic Interaction of Heteroatomic Pt-Ru Dimerization Sites
    You, Xiao-Meng
    Xu, Beibei
    Zhou, Hang
    Qiao, Hongwei
    Lv, Xingxi
    Huang, Zejiang
    Pang, Jingyi
    Yang, Lingyun
    Liu, Peng Fei
    Guan, Xiaohong
    Yang, Hua Gui
    Wang, Xuelu
    Yao, Ye-Feng
    [J]. ACS NANO, 2024, 18 (13) : 9403 - 9412
  • [49] Dual Interface Synergistic Catalysis: The Selective Hydrogenation of Crotonaldehyde Over Pt/Co3O4@PDA
    Tong Zhang
    HuaHua Zhao
    Jian Yang
    Jun Zhao
    Liang Yan
    Lingjun Chou
    Huanling Song
    [J]. Catalysis Letters, 2023, 153 : 965 - 977
  • [50] Dual Interface Synergistic Catalysis: The Selective Hydrogenation of Crotonaldehyde Over Pt/Co3O4@PDA
    Zhang, Tong
    Zhao, HuaHua
    Yang, Jian
    Zhao, Jun
    Yan, Liang
    Chou, Lingjun
    Song, Huanling
    [J]. CATALYSIS LETTERS, 2023, 153 (04) : 965 - 977