Preparation of mesoporous CuO/γ-Al<sub>2</sub>O<sub>3</sub> for one-step synthesis of dimethyl ether from syngas

CHEN Yue-xian; WANG Yan; MA Jing-hong; LI Rui-feng

Volume 43 Issue 01

Jan. 2015

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CHEN Yue-xian, WANG Yan, MA Jing-hong, LI Rui-feng. Preparation of mesoporous CuO/γ-Al2O3 for one-step synthesis of dimethyl ether from syngas[J]. Journal of Fuel Chemistry and Technology, 2015, 43(01): 65-73.

Citation:

CHEN Yue-xian, WANG Yan, MA Jing-hong, LI Rui-feng. Preparation of mesoporous CuO/γ-Al₂O₃ for one-step synthesis of dimethyl ether from syngas[J]. Journal of Fuel Chemistry and Technology, 2015, 43(01): 65-73.

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Preparation of mesoporous CuO/γ-Al₂O₃ for one-step synthesis of dimethyl ether from syngas

Institute of Special Chemicals, Taiyuan University of Technology, Taiyuan 030024, China

Received Date: 2014-07-24
Rev Recd Date: 2014-09-19
Publish Date: 2015-01-30

Abstract

Abstract

Solvent evaporation self-assembly method was adopted to synthesize CuO/γ-Al₂O₃ composite catalysts with mesoporous structure using F₁₂₇ as template, aluminum isopropoxide and copper nitrate as precursor. X-ray diffraction (XRD), scanning electron microscope (SEM), energy dispersive spectrometer (EDS), H₂ temperature program reduction (H₂-TPR), nitrogen adsorption-desorption and transmission electron microscope (TEM) were used to characterize the properties of the catalysts. The results show that ordered and uniform mesoporous structure as well as large specific surface area were discovered in catalysts with different copper contents. In the syngas to dimethyl ether (DME) reaction, the highest conversion of CO reached 68.8% and the selectivity of DME achieved 59.0% under space velocity of 1 500 h^-1, 320 ℃ and 5 MPa. The conversion of CO decreased from 68.8% to 59.5% after 50 h on stream, and the selectivity of DME kept constant. The partial loss of activity was due to the aggregation of copper on this catalyst.
- solvent evaporation self-assembly method,
- syngas,
- DME

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References(22)

References

KIM M Y, YOON S H, RYU B W, LEE C S. Combustion and emission characteristics of DME as an alternative fuel for compression ignition engines with a high pressure injection system[J]. Fuel, 2008, 87(12): 2779-2786.

KAJOMSAK F, TETSUYA F, RYUJI K, KOICHI E. Deactivation and regeneration behaviors of copper spinel-alumina composite catalysts in steam reforming of dimethyl ether[J]. J Catal, 2008, 256(1): 37-44.

ADACHI Y, KOMOTO M, WATANABE I, OHNO Y, FUJIMOTO K. Effective utilization of remote coal through dimethyl ether synthesis[J]. Fuel, 2000, 79(3): 229-234.

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]. J Fuel Chem Technol, 2008, 36(1): 74-78.)

MAO D S, YANG W M, XIA J C, ZHANG B, SONG Q Y, CHEN Q L. Highly effective hybrid catalyst for the direct synthesis of dimethyl ether from syngas with magnesium oxide-modified HZSM-5 as a dehydration component[J]. J Catal, 2005, 230(1): 140-149.

毛东森, 夏建超. 分子筛硅铝比及晶粒粒径对CuO-ZnO-Al₂O₃/HZSM-5催化剂直接合成二甲醚反应性能的影响[J]. 燃料化学学报, 2012, 40(2): 235-40.(MAO Dong-sen, XIA Jian-chao. Effects of silicon to aluminum ratio and crystal size of zeolite on catalytic properties of CuO-ZnO-Al₂O₃/HZSM-5 for the direct synthesis of dimethyl ether from syngas[J]. J Fuel Chem Technol, 2012, 40(2): 235-40.)

WANG D S, HAN Y Z, TAN Y S, TSUBAKI N. Effect of H₂O on Cu-based catalyst in one-step slurry phase dimethyl ether synthesis[J]. Fuel Process Technol, 2009, 90(3): 446-451.

李超, 李琢, 李建青, 杨成, 吴晋沪. 一步法合成二甲醚整体式催化剂的制备及反应性能研究[J]. 燃料化学学报, 2011, 39(4): 287-292.(LI Chao, LI Zhuo, LI Jian-qing, YANG Cheng, WU Jin-hu. Preparation and catalytic properties of a monolithic catalyst for one step synthesis of dimethyl ether[J]. J Fuel Chem Technol, 2011, 39(4): 287-292.)

RAMOS F S, DE FARIAS A M D, BORGES L E P, MONTEIRO J L, FRAGA M A, SOUSA-AGUIAR E F, APPEL L G. Role of dehydration catalyst acid properties on one-step DME synthesis over physical mixtures[J]. Catal Today, 2005, 101(1): 39-44.

QI G X, ZHENG X M, FEI J H, HOU Z Y. A novel catalyst for DME synthesis from CO hydrogenation: 1. Activity, structure and surface properties[J]. J Mol Catal A: Chem, 2001, 176(1/2): 195-203.

SIERRA I, ERENA J, AGUAYO A T, ARANDES J M, BILBAO J. Regeneration of CuO-ZnO-Al₂O₃/γ-Al₂O₃ catalyst in the direct synthesis of dimethyl ether[J]. Appl Catal B: Environ, 2010, 94(1/2): 108-116.

TAKEGUCHI T, YANAGISAWA K I, 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: Gen, 2000, 192(2): 201-209.

SUN K, LU W, QIU F, XU X. Direct synthesis of DME over bifunctional catalyst: surface properties and catalytic performance[J]. Appl Catal A: Gen, 2003, 252(2): 243-249.

GE Q, HUANG Y, QIU F, LI S. Bifunctional catalysts for conversion of synthesis gas to dimethyl ether[J]. Appl Catal A: Gen, 1998, 167: 23-30.

SAI PRASAD P S, BAE J W, KANG S H, LEE Y J, JUN K W. Single-step synthesis of DME from syngas on Cu-ZnO-Al₂O₃/zeolite bifunctional catalysts: The superiority of ferrierite over the other zeolites[J]. Fuel Process Technol, 2008, 89(12): 1281-1286.

WU X, ABRAHA M G, ANTHONY R G. Methanol conversion on SAPO-34: Reaction condition for fixed-bed reactor[J]. Appl Catal A: Gen, 2004, 260(1): 63-69.

FEI J H, TANG X J, HUO Z Y. Effect of copper content on Cu-Mn-Zn/zeolite-Y catalysts for the synthesis of dimethyl ether from syngas[J]. Catal Commun, 2006, 7(11): 827-831.

杨明霞, 费金华, 郑小明. 共沉淀浸渍法制备由合成气直接合成二甲醚的Cu-Mn催化剂[J]. 燃料化学学报, 2004, 32(2): 83-87.(YANG Ming-xia, FEI Jin-hua, ZHENG Xiao-ming. A novel preparetion of Cu-Mn catalysts for dimethyl ether synthesis from syngas[J]. J Fuel Chem Technol, 2004, 32(2): 83-87.)

JIANG H Q, BONGARD H, SCHMIDT W, SCHUTH F. One-pot synthesis of mesoporous Cu-γ-Al₂O₃ as bifunctional catalyst for direct dimethyl ether synthesis[J]. Microporous Mesoporous Mater, 2012, 164: 3-8.

刘源, 钟炳, 王琴, 彭少逸. 氧化铜/氧化锆甲醇合成催化剂的性能研究[J]. 催化学报, 1995, 16(6): 442-446.(LIU Yuan, ZHONG Bing, WANG Qin, PENG Shao-yi. Study of CuO/ZrO₂ catalysts for methanol synthesis from CO/H₂[J]. Chin J Catal, 1995, 16(6): 442-446.)

KUNG H H. Deactivation of methanol synthesis catalysts-A review[J]. Catal Today, 1992, 11(4): 443-453.

TOPSE H. Developments in operando studies and in situ characterization of heterogeneous catalysts[J]. J Catal, 2003, 216(1/2): 155-164.

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