Volume 40 Issue 02
Feb.  2012
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MAO Dong-sen, XIA Jian-chao. Effects of silicon to aluminum ratio and crystal size of zeolite on catalytic properties of Cu-ZnO-Al2O3/HZSM-5 for the direct synthesis of dimethyl ether from syngas[J]. Journal of Fuel Chemistry and Technology, 2012, 40(02): 235-240.
Citation: MAO Dong-sen, XIA Jian-chao. Effects of silicon to aluminum ratio and crystal size of zeolite on catalytic properties of Cu-ZnO-Al2O3/HZSM-5 for the direct synthesis of dimethyl ether from syngas[J]. Journal of Fuel Chemistry and Technology, 2012, 40(02): 235-240.

Effects of silicon to aluminum ratio and crystal size of zeolite on catalytic properties of Cu-ZnO-Al2O3/HZSM-5 for the direct synthesis of dimethyl ether from syngas

  • Received Date: 2011-03-25
  • Rev Recd Date: 2011-07-01
  • Publish Date: 2012-02-29
  • A series of HZSM-5 zeolite samples with different n(SiO2)/n(Al2O3) ratios and crystal sizes were hydrothermally synthesized and physically mixed with a methanol synthesis component (CuO-ZnO-Al2O3) to form hybrid catalysts. The direct synthesis of dimethyl ether (DME) from syngas was carried out over the prepared hybrid catalysts in a pressurized fixed-bed under continuous flow conditions. The results indicated that the selectivity for CO2 decreased with the increase of n(SiO2)/n(Al2O3) ratios in HZSM-5 zeolite due to the decrease in the amount and strength of the acid sites, so the selectivity for DME was enhanced greatly. On the other hand, although the activity was not enhanced on the smaller sized HZSM-5 compared to the larger sized one, the selectivity for CO2 and hydrocarbons was decreased evidently.
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  • 秦冉冉, 常杰, 叶跃元, 范娟. 一步法制二甲醚双功能催化剂研究进展[J]. 可再生能源, 2009, 27(6): 96-101. (QIN Ran-ran, CHANG Jie, YE Yue-yuan, FAN Juan. Bifunctional catalysts for direct synthesis of dimethyl ether from syngas[J]. Renewable Energy Resources, 2009, 27(6): 96-101.)
    别良伟, 王华. 合成气一步法制二甲醚催化剂研究进展[J]. 工业催化, 2009, 17(2): 34-39. (BIE Liang-wei, WANG Hua. Advances in developments of the catalysts for one-step synthesis of dimethyl ether from syngas[J]. Industrial Catalysis, 2009, 17(2): 34-39.)
    SOFIANOS A C, SCURRELL M S. Conversion of synthesis gas to dimethyl ether over bifunctional catalytic systems[J]. Ind Eng Chem Res, 1991, 30(11): 2372-2378.
    陈建刚, 牛玉琴. HZSM-5分子筛与铜基的复合催化剂上合成气制二甲醚[J]. 天然气化工, 1997, 22(6): 6-10. (CHEN Jian-gang, NIU Yu-qin. A hybrid catalyst for DME synthesis from syngas with HZSM-5 as dehydration catalyst[J]. Natural Gas Chemical Industry, 1997, 22(6): 6-10.)
    TAKEGUCHI T, YANAGISAWA K, INUI T, INOUE M. Effect of the property of solid acid upon syngas-to-dimethyl ether conversion on the hybrid catalysts composed of Cu-Zn-Ga and solid acids[J]. Appl Catal A, 2000, 192(2): 201-209.
    JOO O S, JUNG K D, HAN S H. Modification of HZSM-5 and γ-alumina with formaldehyde and its application to the synthesis of dimethyl ether from syn-gas[J]. Bull Korean Chem Soc, 2002, 23(8): 1103-1105.
    鲁皓, 常杰, 付严, 王铁军. HZSM-5型分子筛硅铝比对一步法合成二甲醚的影响[J]. 燃料化学学报, 2005, 33(3): 324-328. (LU Hao, CHANG Jie, FU Yan, WANG Tie-jun. Study of the effects of Si/Al ratio of HZSM-5 on the direct synthesis of DME[J]. Journal of Fuel Chemistry and Technology, 2005, 33(3): 324-328.)
    许庆利, 李庭琛, 张素平, 任铮伟, 颜涌捷. 分子筛改性对一步法合成二甲醚的影响[J]. 燃料化学学报, 2008, 36(1): 74-78. (XU Qing-li, LI Ting-chen, ZHANG Su-ping, REN Zheng-wei, YAN Yong-jie. Effect of the modified zeolite on one-step dimethyl ether synthesis[J]. Journal of Fuel Chemistry and Technology, 2008, 36(1): 74-78.)
    XIA J, MAO D, ZHANG B, CHEN Q, TANG Y. One-step synthesis of dimethyl ether from syngas with Fe-modified zeolite ZSM-5 as dehydration catalyst[J]. Catal Lett, 2004, 98(4): 235-240.
    KIM J H, PARK M J, KIM S J, JOO O S, JUNG K D. DME synthesis from synthesis gas on the admixed catalysts of Cu/ZnO/Al2O3 and ZSM-5[J]. Appl Catal A, 2004, 264(1): 37-41.
    ERENA J, GARONA R, ARANDES J M, AGUAYO A T, BILBAO J. Effect of operating conditions on the synthesis of dimethyl ether over a CuO-ZnO-Al2O3/NaHZSM-5 bifunctional catalyst[J]. Catal Today, 2005, 107-108(1/4): 467-473.
    WANG L, QI Y, WEI Y, FANG D, MENG S, LIU Z. Research on the acidity of the double-function catalyst for DME synthesis from syngas[J]. Catal Lett, 2006, 106(1/2): 61-66.
    MAO D, XIA J, ZHANG B, LU G. Highly efficient synthesis of dimethyl ether from syngas over the admixed catalyst of CuO-ZnO-Al2O3 and antimony oxide modified HZSM-5 zeolite[J]. Energy Convers Manage, 2010, 51(6): 1134-1139.
    何凤仙, 唐秀娟, 费金华, 郑小明. 金属组分负载量对Cu-Mn-Zn/Y直接合成二甲醚催化剂的影响[J]. 燃料化学学报, 2006, 34(2): 191-194. (HE Feng-xian, TANG Xiu-juan, FEI Jin-hua, ZHENG Xiao-ming. Effect of the content of metallic component on Cu-Mn-Zn/Y catalysts for direct synthesis of DME[J]. Journal of Fuel Chemistry and Technology, 2006, 34(2): 191-194.)
    于翔, 王军华, 张立伟, 侯昭胤, 费金华, 郑小明. 甲醇及合成气制二甲醚中不同粒径的HY分子筛及复合Cu-Mn-Zn/HY催化剂[J]. 催化学报, 2010, 31(5): 591-596. (YU Xiang, WHANG Jun-hua, ZHANG Li-wei, HOU Zhao-yin, FEI Jin-hua, ZHENG Xiao-ming. Dimethyl ether synthesis from methanol and syngas over different sized HY zeolite and Cu-Mn-Zn/HY bifunctional catalyst[J]. Chinese Journal of Catalysis, 2010, 31(5): 591-596.)
    YOO K S, KIM J H, PARK M J, KIM S J, JOO O S, JUNG K D. Influence of solid acid catalyst on DME production directly from synthesis gas over the admixed catalyst of Cu/ZnO/Al2O3 and various SAPO catalysts[J]. Appl Catal A, 2007, 330(1): 57-62.
    MAO D, XIA J, CHEN Q, LU G. Highly effective conversion of syngas to dimethyl ether over the hybrid catalysts containing high silica HMCM-22 zeolites[J]. Catal Commun, 2009, 10(5): 620-624.
    BAE J W, KANG S-H, LEE Y-J, JUN K-W. Synthesis of DME from syngas on the bifunctional Cu-ZnO-Al2O3/Zr-modified ferrierite: Effect of Zr content[J]. Appl Catal B, 2009, 90(3/4): 426-435.
    许庆利, 李庭琛, 张素平, 任铮伟, 颜涌捷. 固体酸脱水剂表面酸性对一步法合成二甲醚的影响[J]. 过程工程学报, 2007, 7(5): 905-909. (XU Qing-li, LI Ting-chen, ZHANG Su-ping, REN Zheng-wei, YAN Yong-jie. Effect of solid acid as dchydrant on one-step DME synthesis[J]. The Chinese Tournal of process Engineering , 2007, 7(5): 905-909.)
    刘志坚, 廖建军, 谭经品, 李大东. 甲醇脱水生成二甲醚的沸石催化剂[J]. 石油化工, 1999, 28(4): 236-240. (LIU Zhi-jian, LIAO Jian-jun, TAN Jing-pin, LI Da-dong. Study on the zeolite catalysts for dimethyl ether synthesis from methanol[J]. Petrochemical Technology, 1999, 28(4): 236-240.)
    KANG S-H, BAE J W, JUN K-W, POTDAR H S. Dimethyle ether synthesis from syngas over the composite catalysts of Cu-ZnO-Al2O3/Zr-modified zeolites[J]. Catal Commun, 2008, 9(10): 2035-2039.
    毛东森, 郭强胜, 卢冠忠. 分子筛晶粒大小及磷改性对ZSM-5催化甲醇转化制丙烯的影响[J]. 石油学报(石油加工), 2009, 25(4): 503-508. (MAO Dong-sen, GUO Qian-sheng, LU Guan-zhong. Effects of crystal size and phosphorus modification on catalytic conversion of methanol to propylene over ZSM-5 zeolite[J]. Acta Petrolei Sinica (Petroleum Processing Section), 2009, 25(4): 503-508.)
    滕加伟, 赵国良, 谢在库, 陈庆龄. ZSM-5分子筛晶粒尺寸对C4烯烃催化裂解制丙烯的影响[J]. 催化学报, 2004, 25(8): 602-606. (TENG Jia-wei, ZHAO Guo-liang, XIE Zai-ku, CHEN Qing-ling. Effect of ZSM-5 zeolite crystal size on propylene production from catalytic cracking of C4 olefins[J]. Chinese Journal of Catalysis, 2004, 25(8): 602-606.)
    SHIRALKAR V P, JOSHI P N, EAPEN M J, RAO B S. Synthesis of ZSM-5 with variable crystallite size and its influence on physicochemical properties[J]. Zeolites, 1991, 11(1/3): 511-516.
    SINGH M, KAMBLE R, VISWANADHAM N. Effect of crystal size on physico-chemical properties of ZSM-5[J]. Catal Lett, 2008, 120(3/4): 288-293.
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