Carbon nanotubes supported Cu-Ni bimetallic catalysts and their properties for the direct synthesis of dimethyl carbonate from methanol and carbon dioxide

被引:86
作者
Bian, Jun [1 ]
Xiao, Min [1 ]
Wang, Shuan-Jin [1 ]
Lu, Yi-Xin [2 ,3 ]
Meng, Yue-Zhong [1 ]
机构
[1] Sun Yat Sen Univ, State Key Lab Optoelect Mat & Technol, Inst Optoelect & Funct Composite Mat, Guangzhou 510275, Guangdong, Peoples R China
[2] Natl Univ Singapore, Dept Chem, Singapore 117543, Singapore
[3] Natl Univ Singapore, Med Chem Program, Off Life Sci, Singapore 117543, Singapore
关键词
Dimethyl carbonate; Carbon dioxide; Bimetallic catalyst; Catalysis; MILD CONDITIONS; OXIDATION; ZIRCONIA; HYDROGENATION; PLATINUM;
D O I
10.1016/j.apsusc.2009.03.057
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Multi-walled carbon nanotubes (MWCNTs) supported Cu-Ni bimetallic catalysts for the direct synthesis of dimethyl carbonate (DMC) from CH3OH and CO2 were synthesized and investigated. The supporting materials and the synthesized catalysts were fully characterized using FTIR, scanning electron microscopy (SEM), transmission electron microscopy (TEM), temperature-programmed reduction (TPR), X-ray diffraction (XRD) and X-ray photoelectron spectrum (XPS) techniques. The catalytic activities were investigated by performing micro-reactions. The experimental results showed that the metal phase and Cu-Ni alloy phase in the catalyst were partially formed during the calcination and activation step. Active metal particles were dispersed homogeneously on the surface of the MWCNTs. Cu-Ni/MWCNTs catalysts were efficient for the direct synthesis of DMC. The highest conversion of CH3OH was higher than 4.3% and the selectivity of DMC was higher than 85.0% under the optimal catalytic conditions of 120 degrees C and around 1.2 MPa. The high catalytic activity of Cu-Ni/MWCNTs in DMC synthesis can be attributed to the synergetic effects of metal Cu, Ni and Cu-Ni alloy in the activation of CH3OH and CO2, the unique structure of MWCNTs and the interaction between the metal particles and the supports. (C) 2009 Elsevier B. V. All rights reserved.
引用
收藏
页码:7188 / 7196
页数:9
相关论文
共 36 条
  • [1] Aresta M, 1997, CHEMTECH, V27, P32
  • [2] BIAN J, 2008, CATAL COMMUN, DOI DOI 10.1016/J.CATC0M.2008.12.008
  • [3] BIAN J, 2008, CHEM ENG J, DOI DOI 10.1016/J.CEJ.2008.11.16
  • [4] Highly effective direct synthesis of DMC from CH3OH and CO2 using novel Cu-Ni/C bimetallic composite catalysts
    Bian, Jun
    Xiao, Min
    Wang, Shuan Jin
    Lu, Yi Xin
    Meng, Yue Zhong
    [J]. CHINESE CHEMICAL LETTERS, 2009, 20 (03) : 352 - 355
  • [5] X-ray diffraction characterization on the alignment degree of carbon nanotubes
    Cao, AY
    Xu, CL
    Liang, J
    Wu, DH
    Wei, BQ
    [J]. CHEMICAL PHYSICS LETTERS, 2001, 344 (1-2) : 13 - 17
  • [6] Nanotubes as nanoprobes in scanning probe microscopy
    Dai, HJ
    Hafner, JH
    Rinzler, AG
    Colbert, DT
    Smalley, RE
    [J]. NATURE, 1996, 384 (6605) : 147 - 150
  • [7] A CARBON NANOTUBE FIELD-EMISSION ELECTRON SOURCE
    DEHEER, WA
    CHATELAIN, A
    UGARTE, D
    [J]. SCIENCE, 1995, 270 (5239) : 1179 - 1180
  • [8] EBBESEN TW, 1996, ADV MAT, V155
  • [9] ERIC VS, 2002, CATAL TODAY, V71, P327
  • [10] Direct synthesis of dimethyl carbonate from carbon dioxide and methanol catalyzed by base
    Fang, SN
    Fujimoto, K
    [J]. APPLIED CATALYSIS A-GENERAL, 1996, 142 (01) : L1 - L3