Research on stop-effect on the catalytic dehydration of ethanol over HZSM-5

ZHANG Ye-long; LI Yuan-yuan; JIA Chen; HAN Yu-wang; HU Yi

Volume 41 Issue 12

Dec. 2013

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Article Navigation > Journal of Fuel Chemistry and Technology > 2013 > 41(12): 1495-1501

ZHANG Ye-long, LI Yuan-yuan, JIA Chen, HAN Yu-wang, HU Yi. Research on stop-effect on the catalytic dehydration of ethanol over HZSM-5[J]. Journal of Fuel Chemistry and Technology, 2013, 41(12): 1495-1501.

Citation:

ZHANG Ye-long, LI Yuan-yuan, JIA Chen, HAN Yu-wang, HU Yi. Research on stop-effect on the catalytic dehydration of ethanol over HZSM-5[J]. Journal of Fuel Chemistry and Technology, 2013, 41(12): 1495-1501.

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Research on stop-effect on the catalytic dehydration of ethanol over HZSM-5

1.
College of Science, Nanjing University of Technology, Nanjing 210009, China;
2.
College of Chemistry and Chemical Engineering, Nanjing University of Technology, Nanjing 210009, China;
3.
State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing University of Technology, Nanjing 210009, China

Received Date: 2013-04-22
Rev Recd Date: 2013-06-05
Publish Date: 2013-12-30

Abstract

Abstract

The stop-effect phenomenon on the catalytic dehydration of ethanol over HZSM-5 zeolite was observed. That is, when stopping ethanol-water feed for a period of time and restoring the feed, a dramatic increase on ethylene selectivity could be found. At different reaction conditions, it was found that the stop-effect was enhanced by increasing the stop time and reaction temperature or decreasing the feed speed. When the ethanol concentration was kept at 55%, the stop-effect could be strengthened and the high ethylene selectivity was maintained at long time. 500 h catalyst stability test showed that the stop-effect can improve the life span of the catalyst effectively. By studying the aqueous ethanol dehydration mechanism and experimental results, the preliminary conclusion is that causes of the stop-effect on the catalytic dehydration of ethanol over HZSM-5 is the accumulation of ethoxy intermediate and regeneration of empty catalytic active sites in stop operation.
- ethanol dehydration,
- ethylene,
- HZSM-5 catalyst,
- stop-effect

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References(23)

References

胡燚, 李慧, 黄和, 胡耀池. 生物乙烯开发进展与产业化[J]. 现代化工, 2009, 29(1): 6-9. (HU Yi, LI Hui, HUANG He, HU Yao-chi. Development progress and industrialization of bio-ethylene[J]. Modern Chemical Industry, 2009, 29(1): 6-9.)

王红秋, 郑轶丹. 世界乙烯工业发展现状与展望[J]. 国际石油经济, 2010, 10: 51-56. (WANG Hong-qiu, ZHENG Yi-dan. Present and future status of the global ethylene industry[J]. International Petroleum Economics, 2010, 10: 51-56.)

潘锋, 吴玉龙, 张建安, 童军茂. 生物发酵乙醇催化脱水制乙烯发展状况[J]. 现代化工, 2006, 26(S2): 27-29. (PAN Feng, WU Yu-long, ZHANG Jian-an, TONG Jun-mao. Development status of ethylene production by catalytic dehydration of fermented alcohol[J]. Modern Chemical Industry, 2006, 26(S2): 27-29.)

刘铭, 初旭明, 李慧, 胡燚. Fe₂O₃/γ-Al₂O₃催化乙醇脱水制乙烯[J]. 石油化工, 2010, 39(8): 861-865. (LIU Ming, CHU Xu-ming, LI Hui, HU Yi. Catalytic dehydration of ethanol to ethylene over Fe₂O₃/γ-Al₂O₃[J]. Petrochemical Technology, 2010, 39(8): 861-865.)

沈德建, 刘宗章, 张敏华. ZSM-5上乙醇催化脱水制乙烯的研究进展[J]. 分子催化, 2011, 25(4): 348-35. (SHEN De-jian, LIU Zong-zhang, ZHANG Min-hua. Study of catalytic dehydration of ethanol into ethylene over ZSM-5[J]. Journal of Molecular Catalysis(China), 2011, 25(4): 348-35.)

ZHANG X, WANG R J, YANG X X, ZHANG F B. Comparison of four catalysts in the catalytic dehydration of ethanol to ethylene[J]. Micropor Mesopor Mater, 2008, 116(1/3): 210-215.

HAN Y W, LU C Y, XU D S, ZHANG Y L, HU Y, HUANG H. Molybdenum oxide modified HZSM-5 catalyst: Surface acidity and catalytic performance for the dehydration of aqueous ethanol[J]. Appl Catal A: Gen, 2011, 396(1/2): 8-13.

陆翠云, 张叶龙, 卢圣国, 韩毓旺. Mo/HZSM-5催化乙醇制备乙烯的性能研究[J]. 石油化工, 2011, 40(12): 1281-1286. (LU Cui-yun, ZHANG Ye-long, LU Sheng-guo, HAN Yu-wang, Ethanol dehydration to ethylene over Mo/HZSM-5 catalyst[J]. Petrochemical Technology, 2011, 40(12): 1281-1286.)

BI J D, GUO X W, LIU M, WANG X S. High effective dehydration of bio-ethanol into ethylene over nanoscale HZSM-5 zeolite catalysts[J]. Catal Today, 2010, 149(1/2): 143-147.

KOUBEK J, PASEK J, RUZICKA V. Exploitation of a nonstationary kinetic phenomenon for the elucidation of surface progresses in a catalytic reaction[C]. New horizons in catalysis, Amsterdam-Tokyo: Elsevier-Kodansha, 1980: 853-862.

KOUBEK J, PASEK J, RUZICKA V. Stationary and nonstationary deactivation of alumina and zeolites in elimination reactions[C]. Catal Deactivation, Amsterdam: Elsevier, 1980: 251-260.

PEKAI M, KOUBEK J. Modelling study of transient behaviour of elimination reactions of alcohols and amines on oxide catalysts[J]. J Mol Catal A: Chem, 1997, 123(2/3): 131-139.

MORAVEK V, KRAUS M. Transient behavior of the system ethanol-diethyl ether-water-alumina[J]. J Catal, 1984, 87(2): 452-460.

MORAVEK V. Steady-state and transient kinetics of displacement adsorption and educt inhibition in dehydration of alcohols on alumina[J]. J Catal, 1992, 133: 170-178.

RENKEN A. Reactor performance enhancement under periodic operation for the ethanol dehydration over r-alumina, a reaction with a stop-effect[J]. Chem Eng Sci, 1999, 54: 4469-4474.

GOLAY S, DOEPPER R, RENKEN A. In-situ characterization of the surface intermediates for the ethanol dehydration reaction over r-alumina under dynamic conditions[J]. Appl Catal A: Gen, 1998, 172: 97-106.

GOLAY S, WOLFRATH O, DOEPPER R, RENKEN A. Model discrimination for reactions with stop-effect[J]. Stud Surf Sci Catal, 1997, 109: 295-304.

THULLIE J, RENKEN A. Forced concentration oscillations for catalytic reactions with stop-effect[J]. Chem Eng Sci, 1991, 46(4): 1083-1088.

董娇娇, 朱瑾, 申群兵, 刘子玉, 朱学栋, 朱子彬. MoO₃/HZSM-5催化剂上重芳烃加氢脱烷基反应[J]. 石油化工, 2008, 37(3): 232-237. (DONG Jiao-jiao, ZHU Jin, SHEN Qun-bing, LIU Zi-yu, ZHU Xue-dong, ZHU Zi-bin. Hydrodealkylation of heavy aromatics on MoO₃/HZSM-5 catalyst[J]. Petrochemical Technology, 2008, 37(3): 232-237.)

李斌, 李景林, 梁宇宁. Mo/HZSM-5分子筛的表征和液相催化酯化活性[J]. 广西大学学报, 1999, 24(1): 57-60. (LI Bin, LI Jing-lin, LIANG Yu-ning. Characteristics and activity of catalytic esterification in liquid phase of Mo/HZSM-5 zeolites[J]. Journal of Guangxi University, 1999, 24(1): 57-60.)

CORY P, RAVINDRA D. Production of ethylene from hydrous ethanol on H-ZSM-5 under mild conditions[J]. Ind Eng Chem Res, 1997, 36(11): 4466-4475.

CHIANG H, BHAN A. Catalytic consequences of hydroxyl group location on the rate and mechanism of parallel dehydration reactions of ethanol over acidic zeolites[J]. J Catal, 2010, 271(2): 251-261.

SCHULZ J, BANDERMANN F. Conversion of ethanol over zeolite H-ZSM-5[J]. Chem Eng Technol, 1994, 17(3): 179-186.

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