Long carbon nanotubes intercrossed Cu/Zn/Al/Zr catalyst for CO/CO2 hydrogenation to methanol/dimethyl ether

被引:82
作者
Zhang, Qiang [1 ]
Zuo, Yi-Zan [1 ]
Han, Ming-Han [1 ]
Wang, Jin-Fu [1 ]
Jin, Yong [1 ]
Wei, Fei [1 ]
机构
[1] Tsinghua Univ, Dept Chem Engn, Beijing Key Lab Green Chem React Engn & Technol, Beijing 100084, Peoples R China
关键词
Carbon nanotube; Cu/Zn/Al/Zr catalyst; CO/CO2; hydrogenation; Methanol synthesis; Dimethyl ether synthesis; Stability; CU-ZN-AL; TEMPERATURE METHANOL SYNTHESIS; THERMAL-CONDUCTIVITY; DIMETHYL ETHER; OXIDATIVE DEHYDROGENATION; CO2; HYDROGENATION; HYBRID CATALYSTS; LARGE-SCALE; ARRAYS; GROWTH;
D O I
10.1016/j.cattod.2009.05.018
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
Vertically aligned carbon nanotube (CNT) arrays were dispersed in Na2CO3 solution and co-precipitated with metal nitrite to form long CNTs (over 500 mu m) intercrossed Cu/Zn/Al/Zr catalyst (CD703). The catalyst was used for methanol synthesis from CO/CO2 hydrogenation. The space time yield (STY) of methanol on CD703 increased to 0.94 and 0.28 g/(gcat h), with an increment of 7% and 8% compared with that on the Cu/Zn/Al/Zr catalyst without CNTs for CO and CO2 hydrogenation, respectively. Furthermore, when combined with gamma-Al2O3 catalyst and HZSM-5, dimethyl ether (DME) was obtained with a STY of 0.90 and 0.077 g/(gcat h) at 270 degrees C from one step CO and CO2 hydrogenation, respectively. Due to the phase separation, ion doping and valence compensation, hydrogen reversibly adsorption and storage on CNTs promoting hydrogen spillover, CD703 catalyst show good activity for methanol synthesis. Owing to the high thermal conductivity of CNTs, the stability of CD703 was improved. This indicated that long CNTs were a good promoter on the Cu/Zn/Al/Zr catalyst for methanol/DME production from CO/CO2 hydrogenation. (C) 2009 Elsevier B.V. All rights reserved.
引用
收藏
页码:55 / 60
页数:6
相关论文
共 41 条
[1]   Production of hydrogen from methanol over Cu/ZnO catalysts promoted by ZrO2 and Al2O3 [J].
Agrell, J ;
Birgersson, H ;
Boutonnet, M ;
Melián-Cabrera, I ;
Navarro, RM ;
Fierro, JLG .
JOURNAL OF CATALYSIS, 2003, 219 (02) :389-403
[2]   Deactivation and regeneration of hybrid catalysts in the single-step synthesis of dimethyl ether from syngas and CO2 [J].
Aguayo, AT ;
Ereña, J ;
Sierra, I ;
Olazar, M ;
Bilbao, J .
CATALYSIS TODAY, 2005, 106 (1-4) :265-270
[3]  
An X, 2005, CHINESE J CATAL, V26, P729
[4]   Dimethyl ether synthesis from CO2 hydrogenation on a CuO-ZnO-Al2O3-ZrO2/HZSM-5 bifunctional catalyst [J].
An, Xin ;
Zuo, Yi-Zan ;
Zhang, Qiang ;
Wang, De-zheng ;
Wang, Jin-Fu .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2008, 47 (17) :6547-6554
[5]   A Cu/Zn/Al/Zr fibrous catalyst that is an improved CO2 hydrogenation to methanol catalyst [J].
An, Xin ;
Li, Jinlu ;
Zuo, Yizan ;
Zhang, Qiang ;
Wang, Dezheng ;
Wang, Jinfu .
CATALYSIS LETTERS, 2007, 118 (3-4) :264-269
[6]   Unusually high thermal conductivity of carbon nanotubes [J].
Berber, S ;
Kwon, YK ;
Tománek, D .
PHYSICAL REVIEW LETTERS, 2000, 84 (20) :4613-4616
[7]   CATALYSTS FOR LOW-TEMPERATURE METHANOL SYNTHESIS - PREPARATION OF CU-ZN-AL MIXED OXIDES VIA HYDROTALCITE-LIKE PRECURSORS [J].
BUSETTO, C ;
DELPIERO, G ;
MANARA, G ;
TRIFIRO, F ;
VACCARI, A .
JOURNAL OF CATALYSIS, 1984, 85 (01) :260-266
[8]   Effects of anisotropy, aspect ratio, and nonstraightness of carbon nanotubes on thermal conductivity of carbon nanotube composites [J].
Deng, Fei ;
Zheng, Quan-Shui ;
Wang, Li-Feng ;
Nan, Ce-Wen .
APPLIED PHYSICS LETTERS, 2007, 90 (02)
[9]   Highly active CNT-promoted Cu-ZnO-Al2O3 catalyst for methanol synthesis from H2/CO/CO2 [J].
Dong, X ;
Zhang, HB ;
Lin, GD ;
Yuan, YZ ;
Tsai, KR .
CATALYSIS LETTERS, 2003, 85 (3-4) :237-246
[10]   Spectroscopic evidence of Cu-Al interactions in Cu-Zn-Al mixed oxide catalysts used in CO hydrogenation [J].
Figueiredo, RT ;
Martinez-Arias, A ;
Granados, ML ;
Fierro, JLG .
JOURNAL OF CATALYSIS, 1998, 178 (01) :146-152