Catalytic Performance and Coking Behavior of a Submicron HZSM‐5 Zeolite in Ethanol Dehydration

The catalytic performance and coking behavior of a submicron ZSM-5 zeolite in dehydration of ethanol to ethylene were investigated by means of low temperature nitrogen adsorption, thermal gravimetric analysis, and nuclear magnetic resonance. The submicron catalyst showed higher activity than the micron one due to more mesopores and more strong acid sites. As the reaction temperature increased, ethanol conversion increased over the submicron catalyst, while ethylene selectivity went through a maximum. The selectivities of propylene and butylene increased with increasing reaction temperature, and they decreased with time on stream at constant temperature. The coke deposits can be divided into coke precursor and hard coke, which were attributed to polyalkylbenzene and polycyclic aromatic hydrocarbons, respectively; and increasing reaction temperature can accelerate the transformation of coke precursor into hard coke. A precoking pretreatment method was verified very effective for improving the catalyst stability.

[1]  Yingcai Long,et al.  Coking behavior of a submicron MFI catalyst during ethanol dehydration to ethylene in a pilot-scale fixed-bed reactor , 2011 .

[2]  Xiaohong Cheng,et al.  Hydrogen Bonded Supramolecular Liquid Crystalline Complex of 2,4,6‐Triarylamino‐1,3,5‐triazines with Semiperfluorinated Benzoic Acids , 2010 .

[3]  R. Baker,et al.  Ethanol Dehydration Using Hydrophobic and Hydrophilic Polymer Membranes , 2010 .

[4]  A. Bhan,et al.  Catalytic consequences of hydroxyl group location on the rate and mechanism of parallel dehydration reactions of ethanol over acidic zeolites , 2010 .

[5]  J. Bilbao,et al.  Kinetic Model for the Transformation of Bioethanol into Olefins over a HZSM-5 Zeolite Treated with Alkali , 2010 .

[6]  A. Borgna,et al.  Synthesis, Characterization, and Catalytic Activity of Phosphorus Modified H-ZSM-5 Catalysts in Selective Ethanol Dehydration , 2010 .

[7]  Heng Li,et al.  Lanthanum–phosphorous modified HZSM-5 catalysts in dehydration of ethanol to ethylene: A comparative analysis , 2010 .

[8]  K. Murata,et al.  Conversion of Ethanol to Propylene by H-ZSM-5 with Si/Al2 Ratio of 280 , 2010 .

[9]  J. Pérez–Ramírez,et al.  Mesoporous ZSM-5 zeolites prepared by a two-step route comprising sodium aluminate and acid treatments , 2010 .

[10]  Yingcai Long,et al.  Catalytic Performances of Binder‐free ZSM‐5 Catalysts for Dehydration of Crude Methanol to Dimethyl Ether , 2010 .

[11]  Shengwei Zhu,et al.  An improved dealumination method for adjusting acidity of HZSM-5 , 2010 .

[12]  N. Viswanadham,et al.  Catalytic properties of nano-sized ZSM-5 aggregates , 2009 .

[13]  Fengbao Zhang,et al.  Comparison of four catalysts in the catalytic dehydration of ethanol to ethylene , 2008 .

[14]  Hui-wen Lin,et al.  Precoking selectivation for improving benzene product purity in heavy aromatics transalkylation , 2008 .

[15]  S. Al-Khattaf Enhancing p-xylene selectivity during m-xylene transformation using mildly pre-coked ZSM-5 catalyst , 2007 .

[16]  Ratna R. Sharma-Shivappa,et al.  Potential of Agricultural Residues and Hay for Bioethanol Production , 2007, Applied biochemistry and biotechnology.

[17]  H. Matsuhashi,et al.  Increase in the number of acid sites of a H-ZSM5 zeolite during the dehydration of ethanol , 2007 .

[18]  M. Galbe,et al.  Bio-ethanol--the fuel of tomorrow from the residues of today. , 2006, Trends in biotechnology.

[19]  T. Baba,et al.  Highly selective conversion of ethene to propene over SAPO-34 as a solid acid catalyst , 2006 .

[20]  K. Murata,et al.  Dehydration of Ethanol into Ethylene over Solid Acid Catalysts , 2005 .

[21]  Wei Wang,et al.  Formation and decomposition of surface ethoxy species on acidic zeolite Y. , 2005, Chemphyschem : a European journal of chemical physics and physical chemistry.

[22]  K. Domen,et al.  An ethoxy intermediate in ethanol dehydration on Brønsted acid sites in zeolite. , 2005, The journal of physical chemistry. B.

[23]  C. H. Bartholomew Mechanisms of catalyst deactivation , 2001 .

[24]  P. Magnoux,et al.  Coke formation and coke profiles during the transformation of various reactants at 450°C over a USHY zeolite , 2001 .

[25]  R. Datta,et al.  Production of ethylene from hydrous ethanol on H-ZSM-5 under mild conditions , 1997 .

[26]  J. Fraissard,et al.  Use of NMR techniques for studying deactivation of zeolites by coking , 1995 .

[27]  Jianhua Yao,et al.  Conversion of ethanol in aqueous solution over ZSM-5 zeolites: Influence of Reaction Parameters and Catalyst Acidic Properties as Studied by Ammonia TPD Technique , 1990 .