Volume 40 Issue 05
May  2012
Turn off MathJax
Article Contents
LI Zhong, ZHANG Xiao-bing, GUO Qi-hai, LIU Yan, ZHENG Hua-yan. Influence of precipitation and aging temperature on the performance of CuO/ZnO/Al2O3 catalyst for methanol synthesis in slurry reactor[J]. Journal of Fuel Chemistry and Technology, 2012, 40(05): 569-575.
Citation: LI Zhong, ZHANG Xiao-bing, GUO Qi-hai, LIU Yan, ZHENG Hua-yan. Influence of precipitation and aging temperature on the performance of CuO/ZnO/Al2O3 catalyst for methanol synthesis in slurry reactor[J]. Journal of Fuel Chemistry and Technology, 2012, 40(05): 569-575.

Influence of precipitation and aging temperature on the performance of CuO/ZnO/Al2O3 catalyst for methanol synthesis in slurry reactor

Funds:  国家重点基础研究发展规划(973计划,2012CB723105)。
  • Received Date: 2011-07-19
  • Rev Recd Date: 2011-10-26
  • Publish Date: 2012-05-31
  • The influence of the temperature of precipitation and aging on the performance of the CuO/ZnO/Al2O3 catalyst used for methanol synthesis was studied in a slurry reactor. The catalysts and precursors were characterized through XRD, BET, FT-IR and XPS. The results show that the phases of the precursors are mainly consisted of malachite (Cu2(CO3)(OH)2) and zinc malachite ((Cu,Zn)2(CO3)(OH)2), the crystallinity degree of the precursor that precipitated at 70 ℃ and aged at 80 ℃ is proper, and the performance of the catalyst from the precursor is optimal, with its CuO phase dispersing homogeneously, the electron binding energy of Cu element shifting the largest and the electron binding energy of Zn element shifting the minimum. Its space time yield and deactivation rate reach 153.3 g/(kgcat·h) and 1.44%/d respectively.
  • loading
  • ANDRZEJ C. Liquid-phase methanol synthesis[J]. Catal Rev, 1994, 36(4): 557-615.
    LEE S. Methanol synthesis technology[M]. Boca Raton, Florida, USA: CRC Press Inc, 1990.
    ZhAI X, SHAMOTO J, XIE H, TAN Y, HAN Y, NORITATSU T. Study on the deactivation phenomena of Cu-based catalyst for methanol synthesis in slurry phase[J]. Fuel, 2008, 87(45): 430-434.
    翟旭芳, 社本纯, 解红娟, 谭猗生, 韩怡卓, 椿范立. 浆态相甲醇合成催化剂的失活机理[J]. 催化学报, 2007, 28(1): 51-56. (ZHAI Xu-fang, SHAMOTO Jun, XIE Hong-juan, TAN Yi-sheng, HAN Yi-zhuo, NORITATSU TSUBAKI. Deactivation mechanism of Cu-based catalyst for methanol synthesis in slurry phase[J]. Chinese Journal of Catalysis, 2007, 28(1): 51-56.)
    ZHANG X B, LI Z, GUO Q H. Influence of the calcination on the activity and stability of the Cu/ZnO/Al2O3 catalyst in liquid phase methanol synthesis[J]. Fuel, 2009, 89(7): 1348-1352.
    ZHANG X B, LI Z, GUO Q H, FAN H, ZHENG H Y, LI Z, XIE K C. Influence of the calcinations temperature on the performance of the Cu/ZnO/Al2O3 catalyst for synthesis of methanol in slurry reactor// Proceedings of the 17th International Symposium on Alcohol Fuels. Taiyuan, China: 2008: 438-444.
    ERTL G, KNZINGER H, SCHUTH F. Handbook of Heterogeneous Catalysis[M]. Malden, MA, USA: John Wiley & Sons, Inc, 2008: 2920-2949.
    宋维端, 肖任坚, 房鼎业. 甲醇工学[M]. 北京: 化学工业出版社, 1990: 92-102. (SONG Wei-duan, XIAO Ren-jian, FANG Ding-ye. Methanol Production Technology[M]. Beijing: Chemical Industry Press, 1990: 92-102)
    房德仁, 刘中民, 黎晓琼, 张慧敏, 许磊, 徐秀峰. 沉淀pH对CuO/ZnO/Al2O3系催化剂前驱体性质的影响[J]. 石油化工, 2004, 33(7): 622-626. (FANG De-ren, LIU Zhong-min, LI Xiao-qiong, ZHANG Hui-ming, XU Lei, XU Xiu-feng. Influence of pH on properties of CuO/ZnO/Al2O3 catalyst precursors[J]. Petrochemical Technology, 2004, 33(7): 622-626.)
    房德仁, 刘中民, 张慧敏, 许磊, 徐秀峰, 索掌怀. 沉淀温度对CuO/ZnO/Al2O3系催化剂前驱体性质的影响[J]. 天然气化工, 2004, 29(4): 28-32. (FANG De-ren, LIU Zhong-min, ZHANG Hui-ming, XU Lei, XU Xiu-feng, SUO Zhang-huai. Influence of temperature on the properties of precursors of CuO/ZnO/Al2O3 catalysts[J]. Natural Gas Chemical Industry, 2004, 29(4): 28-32.)
    房德仁, 刘中民, 黎晓琼, 张慧敏, 许磊. 加料方式对CuO/ZnO/Al2O3系催化剂前驱体性质的影响[J]. 燃料化学学报, 2004, 32(6): 734-739. (FANG De-ren, LIU Zhong-min, LI Xiao-qiong, ZHANG Hui-ming, XU Lei. Influence of precipitation method on the properties of precursors of CuO/ZnO/Al2O3 catalysts[J]. Journal of Fuel Chemistry and Technology, 2004, 32(6): 734-739.)
    BALTES C, VUKOJEVI S, SCHUTH C F. Correlations between synthesis, precursor, and catalyst structure and activity of a large set of CuO/ZnO/Al2O3 catalysts for methanol synthesis[J]. J Catal, 2008, 258(2): 334-344.
    QUINN R, MEBRAHTU T, DAHL T A, LUCREZI F A, TOSELAND B A. The role of arsine in the deactivation of methanol synthesis catalysts[J]. Appl Catal A, 2004, 264(1): 103-109.
    刘志坚, 廖建军, 谭经品, 李大东. 甲醇合成催化剂Cu-ZnO的共沉淀机理研究[J]. 石油化工, 1998, 27(7): 479-482. (LIU Zhi-jian, LIAO Jian-jun, TAN Jin-pin, LI Da-dong. Studies on the coprecipitation mechanism of CuO/ZnO catalysts for methanol synthesis from carbon dioxide[J]. Petrochemical Technology, 1998, 27(7): 479-482.)
    LI JL, INUI T. Characterization of precursors of methanol synthesis catalysts, copper/zinc/aluminum oxides, precipitated at different pHs and temperatures[J]. Appl Catal A, 1996, 137(1): 105-117.
    MILLAR G J, HOLM I H, UWINS P J. Characterization of precursors to methanol synthesis catalysts Cu/ZnO system[J]. J Chem Soc, Faraday Trans, 1998, 94(4): 593-600.
    STOILOVA D, KOLEVA V, VASSILEVA V. Infrared study of some synthetic phases of malachite (Cu2(OH)2CO3)–hydrozincite (Zn5(OH)6(CO3)2) series[J]. Spectrochim Acta, Part A, 2002, 58(9): 2051-2059.
    李忠, 郑华艳, 谢克昌. 浆态床合成甲醇CuO/ZnO/Al2O3催化剂的表面性质[J]. 催化学报, 2008, 29(5): 431-435. (LI Zhong, ZHENG Hua-yan, XIE Ke-chang. Surface properties of CuO/ZnO/Al2O3 catalyst for methanol synthesis in slurry reactor[J]. Chinese Journal of Catalysis, 2008, 29(5): 431-435.)
    FIERRO G, LO JACONO M, INVERSI M, PORTA P, CIOCI F, LAVECCHIA R. Study of the reducibility of copper in CuO-ZnO catalysts by temperature-programmed reduction[J]. Appl Catal A, 1996, 137(2): 327-348.
    刘源, 钟炳, 樊彦贞, 彭少逸. 载体制备方法对合成甲醇催化剂的影响[J]. 燃料化学学报, 1996, 24(3): 202-205. (LIU Yuan, ZHONG Bing, FAN Yan-zhen, PENG Shao-yi. Comparative study of CuO/ZrO2 catalysts with the support prepared by different methods[J]. Journal of Fuel Chemistry and Technology, 1996, 24(3): 202-205.)
    OKAMOTO Y, FUKINO K, IMANAKA T. Surface characterization of CuO-ZnO methanol synthesis catalyst by X-ray photoelectric spectroscopy[J]. J Phys Chem, 1983, 87(1): 3740-3747.
    GARBASSI F, PETRINI G. XPS study on the low-temperature CO shift reaction catalyst: I The unreduced copper-zinc system[J]. J Catal, 1984, 90(1): 106-112.
    CLAUSEN B S, SCHITZ J, GRBK L, OVESEN C V, JCOBSEN K W. Wetting non-wetting phenomena during catalysis: Evidence from in situ on-line EXAFS studies of Cu-based catalysts[J]. Top Catal, 1994, 1(34): 367-376.
    TOPSE H, OVESEN C V, CLAUSEN B S. Importance of dynamics in real catalyst systems[J]. Stud Surf Sci Catal, 1997, 109(1):121-139.
  • 加载中

Catalog

    通讯作者: 陈斌, bchen63@163.com
    • 1. 

      沈阳化工大学材料科学与工程学院 沈阳 110142

    1. 本站搜索
    2. 百度学术搜索
    3. 万方数据库搜索
    4. CNKI搜索

    Article Metrics

    Article views (1762) PDF downloads(713) Cited by()
    Proportional views
    Related

    /

    DownLoad:  Full-Size Img  PowerPoint
    Return
    Return