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沉淀及老化温度对浆态床合成甲醇CuO/ZnO/Al2O3催化剂活性及稳定性的影响

李忠 张小兵 郭启海 刘岩 郑华艳

李忠, 张小兵, 郭启海, 刘岩, 郑华艳. 沉淀及老化温度对浆态床合成甲醇CuO/ZnO/Al2O3催化剂活性及稳定性的影响[J]. 燃料化学学报(中英文), 2012, 40(05): 569-575.
引用本文: 李忠, 张小兵, 郭启海, 刘岩, 郑华艳. 沉淀及老化温度对浆态床合成甲醇CuO/ZnO/Al2O3催化剂活性及稳定性的影响[J]. 燃料化学学报(中英文), 2012, 40(05): 569-575.
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.

沉淀及老化温度对浆态床合成甲醇CuO/ZnO/Al2O3催化剂活性及稳定性的影响

基金项目: 国家重点基础研究发展规划(973计划,2012CB723105)。
详细信息
    通讯作者:

    李忠, 博士生导师, 主要从事煤化工, 工业催化和有机合成等方向研究, Tel: 0351-6018526; E-mail: lizhong@tyut.edu.cn。

  • 中图分类号: O614.121

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)。
  • 摘要: 利用浆态床反应器,考察了沉淀及老化温度对CuO/ZnO/Al2O3催化剂催化合成甲醇的活性及稳定性的影响,并用XRD、BET、FT-IR以及XPS等技术对前驱体及催化剂进行了表征。结果表明,前驱体物相主要以孔雀石(Cu2(CO3)(OH)2)和类孔雀石((Cu,Zn)2(CO3)(OH)2)为主,其中,70 ℃沉淀和80 ℃老化条件下制备的前驱体具有适当的结晶度,焙烧后的催化剂中CuO分布均匀,Cu元素的电子结合能位移最大,CuO与ZnO之间作用较强,催化剂的性能最佳,时空收率和失活率分别达到了153.3 g/(kgcat·h)和1.44%/d。
  • 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.
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出版历程
  • 收稿日期:  2011-07-19
  • 修回日期:  2011-10-26
  • 刊出日期:  2012-05-31

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