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ISSN 1000-6818CN 11-1892/O6CODEN WHXUEU
Acta Phys Chim Sin >> 2015,Vol.31>> Issue(7)>> 1374-1382     doi: 10.3866/PKU.WHXB201504302         中文摘要
CATALYSIS AND SURFACE SCIENCE
Catalytic Conversion of Methanol to Propylene over HZSM-5 Modified by NaOH and (NH4)2SiF6
HU Si1, ZHANG Qing2, YIN Qi2, ZHANG Ya-Fei2, GONG Yan-Jun2, ZHANG Ying1, WU Zhi-Jie2, DOU Tao2
1 Department of Materials Science and Engineering, College of Science, China University of Petroleum-Beijing, Beijing 102249, P. R. China;
2 The Key Laboratory of Catalysis, China National Petroleum Corporation, China University of Petroleum-Beijing, Beijing 102249, P. R. China
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A sequential modification by sodium hydroxide (NaOH) and ammonium hexafluorosilicate ((NH4)2SiF6) solution was used for preparing MTP (methanol to propylene reaction) catalyst for the first time. The parent and modified samples were characterized by diverse techniques including powder X-ray diffraction (XRD), X-ray fluorescence (XRF) spectroscopy, N2 adsorption-desorption, transmission electron microscopy (TEM), and NH3 temperature-programmed desorption (NH3-TPD). The effect of modification on the physicochemical properties, such as framework, chemical composition, texture, and acidity, were investigated in detail. The results showed that the mesopore volume of the zeolite catalyst increased significantly following sequential NaOH and (NH4)2SiF6 modification. The acidity was also modulated effectively. The composite modification method successfully overcame the disadvantages associated with individual simple alkali and (NH4)2SiF6 treatments. For instance, using a simple alkali treatment would destroy the framework of the zeolite easily, whereas using a simple (NH4)2SiF6 treatment would only modify the external surface of the zeolite owing to the limited diffusion of the ammonium hexafluorosilicate molecule. When used in MTP reaction, the induction period of the composite modified sample was greatly shortened, and the initial selectivity for propylene increased to 43% under the following operating conditions: T=470 ℃, p=0.1 MPa (pMeOH=50 kPa), and weight hourly space velocity (WHSV)=2 h-1. Moreover, the composite modified zeolite catalyst exhibited significantly improved stability, and the catalytic lifespan was triple that of the parent sample.



Keywords: Alkali treatment   Ammonium hexafluorosilicate   Composite modification   Mesopore   Acidity   Methanol to propylene  
Received: 2015-01-07 Accepted: 2015-04-30 Publication Date (Web): 2015-04-30
Corresponding Authors: DOU Tao Email: doutao@cup.edu.cn

Fund: The project was supported by the National Key Basic Research Program of China (973) (2012CB215002) and National Natural Science Foundation of China (21206192).

Cite this article: HU Si, ZHANG Qing, YIN Qi, ZHANG Ya-Fei, GONG Yan-Jun, ZHANG Ying, WU Zhi-Jie, DOU Tao. Catalytic Conversion of Methanol to Propylene over HZSM-5 Modified by NaOH and (NH4)2SiF6[J]. Acta Phys. -Chim. Sin., 2015,31 (7): 1374-1382.    doi: 10.3866/PKU.WHXB201504302

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56. HU Xiao-Yan, LI Chun-Yi, YANG Chao-He.Catalytic Cracking Behavior of n-Heptane over HZSM-5 Catalyst[J]. Acta Phys. -Chim. Sin., 2010,26(12): 3291-3298
57. CHEN Tian, WANG Tao, WANG Dao-Jun, ZHAO Jian-Qing, DING Xiao-Chun, WU Shi-Chao, XUE Hai-Rong, HE Jian-Ping.Selective Adsorption Behavior of Cu(II) and Cr(VI) Heavy Metal Ions by Functionalized Ordered Mesoporous Carbon[J]. Acta Phys. -Chim. Sin., 2010,26(12): 3249-3256
58. LIU Bai-Jun, MENG Qing-Lei, WANG Hui, MENG Qing-Min.Synthesis and Characterization of Al MCM-41 Mesoporous Molecular Sieves[J]. Acta Phys. -Chim. Sin., 2010,26(12): 3257-3262
59. YANG Xiao-Long, XIA Chun-Gu, TANG Li-Ping, XIONG Xu-Mao, MU Xin-Yuan, HU Bin.Effect of Alumina Support and Barium Oxide on the Structure and Catalytic Activity of Ruthenium Catalysts for Ammonia Synthesis[J]. Acta Phys. -Chim. Sin., 2010,26(12): 3263-3272
60. ZONG Hua, WANG Lei, FANG Hong-Bo, MAO Lei-Ting, WANG Yu-Hui, ZHANG Lu, ZHAO Sui, YU Jia-Yong.Effect of Hydrophobically Modified Polyacrylamide on Interfacial Dilational Rheological Properties of Crude Oil Components[J]. Acta Phys. -Chim. Sin., 2010,26(11): 2982-2988
61. CHEN Zhao-Yang, ZHAO Feng-Ming, MA Chun-An, QIAO Yun.Ultrasonic-Assisted Preparation of Bimodal Mesoporous HollowGlobal Tungsten Carbide and Its Electrocatalytic Performance[J]. Acta Phys. -Chim. Sin., 2010,26(09): 2569-2574
62. ZHANG Wei-Min, YANG Zhen-Dong, LIU Jia, SUN Zhong-Xi.Determination of Acid-Base Equilibrium Constants on Aqueous Mesoporous Silica Surfaces[J]. Acta Phys. -Chim. Sin., 2010,26(08): 2109-2114
63. CHE Hong-Wei, HAN Shu-Hua, HOU Wan-Guo, LIU Ai-Feng.Novel Synthesis of Mesoporous Nanocrystalline Zirconia[J]. Acta Phys. -Chim. Sin., 2010,26(08): 2177-2181
64. LIU Shu-Ping, YUE Ming-Bo, WANG Yi-Meng.One-Step Synthesis of Mesoporous Beta Zeolite Using Phosphate[J]. Acta Phys. -Chim. Sin., 2010,26(08): 2224-2228
65. WU Bao-Hu, ZHANG Shu-Cui, TANG Tao, XU Yao, LIU Yi, WU Zhong-Hua.Small-Angle X-Ray Scattering Studies of Carboxyl Functionalized[J]. Acta Phys. -Chim. Sin., 2010,26(08): 2217-2223
66. LIU Si-Yu, MENG Xiang-Ju, XIAO Feng-Shou.Hydrothermal Synthesis of Ordered Mesoporous Materials with High Stability at High Temperatures[J]. Acta Phys. -Chim. Sin., 2010,26(07): 1852-1859
67. SHEN Bin, WANG Yong-An, WANG Zhi-Fei, ZHANG Ling.Catalytic Activity of an Oxime Carbapalladacycle Complex Grafted onto Superparamagnetically Mesoporous Nanoparticles for the Heck Reaction[J]. Acta Phys. -Chim. Sin., 2010,26(07): 1860-1866
68. ZHANG Jing, KONG Ling-Bin, CAI Jian-Jun, YANG Zhen-Sheng, LUO Yong-Chun, KANG Long.Novel Polypyrrole/Mesoporous Carbon Nanocomposite Electrode for an Electrochemical Hybrid Capacitor[J]. Acta Phys. -Chim. Sin., 2010,26(06): 1515-1520
69. LIU Yi-Wu, YU Huan, ZHANG Xiao-Ming, SUO Ji-Shuan.Direct Gas-Phase Epoxidation of Propylene over Au/Ti-MCM-41(H) Catalysts[J]. Acta Phys. -Chim. Sin., 2010,26(06): 1585-1592
70. YUAN Jin-Fang, LI Jian-Sheng, GU Juan, WANG Fang, SUN Xiu-Yun, HAN Wei-Qing, WANG Lian-Jun.Synthesis and Adsorption Properties of Amino-Functionalized H2N-Zr-Ce-SBA-15 Mesoporous Materials with Short Mesochannels[J]. Acta Phys. -Chim. Sin., 2010,26(06): 1711-1716
71. HE Jie, FAN Yi-Ning.Dispersion and Acidity of Niobia on Nb2O5/γ-Al2O3[J]. Acta Phys. -Chim. Sin., 2010,26(03): 679-684
72. GENG Wang-Chang, LAI Xiao-Yong, LI Xiao-Tian.Ordered Mesoporous MgZnO with Crystalline Walls[J]. Acta Phys. -Chim. Sin., 2010,26(02): 527-530
73. SUN Dun, HE Jian-Ping, ZHOU Jian-Hua, WANG Tao, DI Zhi-Yong, WANG Dao-Jun, DING Xiao-Chun.MClx(M=Pd, Fe, Cr) Assisted Synthesis of Ordered Mesoporous Carbon and Their Electrocatalytic Performance after Loading with Pt Nanoparticles[J]. Acta Phys. -Chim. Sin., 2010,26(02): 385-391
74. WANG Jin-E, YANG Chun.Direct Syntheses and Characterizations of PW11/SBA-15 Mesoporous Hybrid Materials[J]. Acta Phys. -Chim. Sin., 2010,26(02): 515-520
75. LI Kui-Ying, LIU Tong, ZHOU Bing-Jing, WEI Sai-Ling, YANG Wei-Yong.Transient Photovoltaic and Surface Photoacoustic Characteristics of Mesoporous Crystalline La-doped TiO2 Nanoparticles[J]. Acta Phys. -Chim. Sin., 2010,26(02): 403-408
76. HU Long-Xing, DANG Song-Tao, YANG Xia-Ping.Incorporation of CuO into Mesoporous Carbon CMK-3 and Its Adsorption and Catalytic Oxidation of Phenol[J]. Acta Phys. -Chim. Sin., 2010,26(02): 373-377
77. HE Shu-Heng, PU Min, LI Jun-Nan, HE Jing, EVANS David G..Assembly, Structure and Properties of Acid Orange 7-Pillared Zn/Al Hydrotalcite[J]. Acta Phys. -Chim. Sin., 2010,26(01): 259-264
78. YANG Bai-Qin, CHEN Kai, XING Hang, XIAO Jin-Xin.Perfluorobutyl-Based Fluorinated Surfactant with High Surface Activity[J]. Acta Phys. -Chim. Sin., 2009,25(12): 2409-2412
79. WANG Tao, ZHOU Jian-Hua, WANG Dao-Jun, SUN Dun, DI Zhi-Yong, HE Jian-Ping.Syntheses and Infrared Emissivities of Ordered Mesoporous C-Al2O3 Nanocomposites[J]. Acta Phys. -Chim. Sin., 2009,25(10): 2155-2160
80. SUN Zhe, LIU Kai-Yu, ZHANG Hai-Feng, LI Ao-Sheng, XU Xiao-Cun.Study on Meso-C/MnO2 Asymmetric Supercapacitors[J]. Acta Phys. -Chim. Sin., 2009,25(10): 1991-1997
81. LIU Jie-Xiang, WEI Xian, ZHANG Xiao-Guang, HAN En-Shan.Acidities of Cu-[M’]MORand Ag-[M’]MOR (M’=B, Al, Ga, Fe)[J]. Acta Phys. -Chim. Sin., 2009,25(10): 2123-2129
82. YU Yong, LIU Shi-Jun, LI Jie, CHEN Qi-Yuan.Preparation and Characterization ofMesoporous Tungsten Oxides[J]. Acta Phys. -Chim. Sin., 2009,25(09): 1890-1894
83. SHEN Jing-Jing, LIU Chang, ZHU Yu-Dan, LI Wei, FENG Xin, LU Xiao-Hua.Photocatalytic Properties of Mesoporous TiO2 Prepared by Hydrothermal Method[J]. Acta Phys. -Chim. Sin., 2009,25(05): 1013-1018
84. LU Xia; TANG Jing; FAN Yu-Bing; HU Jun; LIU Hong-Lai.Synthesis of Mesoporous Polystyrene Using Reversed Microemulsion Template Method[J]. Acta Phys. -Chim. Sin., 2009,25(01): 178-182
85. JIN Zheng-Wei; LIU Chang-Ling; LIANG Hao.Effects of pH on the Structure of Non-Ionically Templated MSU-X Mesoporous Silica via a Two-Step Synthesis[J]. Acta Phys. -Chim. Sin., 2009,25(01): 150-154
86. WANG Tao, HE Jian-Ping, ZHANG Chuan-Xiang, ZHOU Jian-Hua, GUO Yun-Xia, CHEN Xiu, DI Zhi-Yong, SUN Dun, WANG Dao-Jun.Preparation and Electrochemical Properties of Ordered Mesoporous C/NiO Composites[J]. Acta Phys. -Chim. Sin., 2008,24(12): 2314-2320
87. JIN Zheng-Wei; WANG Xiao-Dong.Mechanism of Acidity-Induced Mesostructure Transformation for Highly Ordered Mesoporous Silica Materials and Their Functionalizations[J]. Acta Phys. -Chim. Sin., 2008,24(08): 1519-1523
88. ZHOU Jian-Hua; HE Jian-Ping; JI Ya-Jun; ZHAO Gui-Wang; ZHANG Chuan-Xiang; CHEN Xiu; WANG Tao.Influence of Hierarchical Porosity in Carbon Material on Electrocatalytic Property of Supported Pt Nanoparticles[J]. Acta Phys. -Chim. Sin., 2008,24(05): 839-843
89. PEI Su-Peng; ZHANG Bin; JIAO Kun; BAO Ren-Lie; YUE Bin; HE He-Yong.Nanostructured CoMoO4 Supported on Mesoporous SBA-15 for Catalytic Oxidative Dehydrogenation of Propane to Propene[J]. Acta Phys. -Chim. Sin., 2008,24(04): 561-564
90. WANG Jian-Hua; LI Bin; WU Hai-Yan; GUO Yu-Zhong.Synthesis of Mesoporous SnO2 and Its Application in Lithium-Ion Battery[J]. Acta Phys. -Chim. Sin., 2008,24(04): 681-685
91. LIU Xiao-Lei; HE Jian-Ping; DANG Wang-Juan; JI Ya-Jun; ZHAO Gui-Wang; ZHANG Chuan-Xiang.Structural Characteristics and Humidity Sensing of Mesoporous SnO2[J]. Acta Phys. -Chim. Sin., 2008,24(03): 475-480
92. MA Xue-Hui; ZHAO Yan-Bao; XIAO Gao-Feng; WU Zhi-Shen.Synthesis of Mercaptopropyl Functionalized Nanosized Mesoporous Silica[J]. Acta Phys. -Chim. Sin., 2008,24(03): 492-496
93. SU Zhao-Hui; CHEN Qi-Yuan; LI Jie; LIU Shi-Jun.Preparation and Characterization of Mesoporous Silicon Dioxide Doped with Tungsten[J]. Acta Phys. -Chim. Sin., 2007,23(11): 1760-1764
94. MA Na; JI Sheng-Fu; WU Ping-Yi; HU Lin-Hua; NIE Ping-Ying.Preparation, Characterization and Catalytic Performance for Hydrodesulfurization of WxC/SBA-16 Catalysts[J]. Acta Phys. -Chim. Sin., 2007,23(08): 1189-1194
95. LI Jing-Yi; MA Jun-Hua; BAI Tu-Ya; SUYOU Le-Ma.Effect of Fluoride Ion on the Photocatalytic Degradation of Sulforhodamine B on TiO2/Bentonite[J]. Acta Phys. -Chim. Sin., 2007,23(08): 1213-1218
96. DANG Wang-Juan; HE Jian-Ping; ZHOU Jian-Hua; JI Ya-Jun; LIU Xiao-Lei; MEI Tian-Qing; LI Hu-Lin.Dispersion and Electrocatalytic Performance of Platinum Nanoparticles Supported on Ordered Mesoporous Carbon[J]. Acta Phys. -Chim. Sin., 2007,23(07): 1085-1089
97. HE Yi-Ming; YI Xiao-Dong; HUANG Chuan-Jing; YING Fang; ZHANG Xiao-Bing; WENG Wei-Zheng; WAN Hui-Lin.Role of Te on Selective Oxidation of Propane to Acrolein over MoBiTeO/SiO2 Catalysts[J]. Acta Phys. -Chim. Sin., 2007,23(06): 851-855
98. ZHAO Hai-Jun; HOU Hai-Tao; CAO Jie-Ming ZHENG Ming-Bo; LIU Jing-Song; ZHANG Fang.Solvothermal Synthesis of Mesoporous SnO2 with Spongy Structure[J]. Acta Phys. -Chim. Sin., 2007,23(06): 959-963
99. KE Xing-Fei; CAO Jie-Ming; ZHENG Ming-Bo; CHEN Yong-Ping; LIU Jin-Song.Synthesis of Hierarchically Meso-Macroporous Structured Carbon Sieve by Dual-template Method[J]. Acta Phys. -Chim. Sin., 2007,23(05): 757-760
100. LIU Yong; MENG Ming; YAO Jin-Song; ZHA Yu-Qing.Preparation and Characterization of the Multi-component Mesoporous Mixed Oxide La-Mn-Ce-O Catalysts[J]. Acta Phys. -Chim. Sin., 2007,23(05): 641-646
101. HAO Zhi-Xian;LIU Hui;GUO Bin;LI Hong;ZHANG Jia-Wei;GAN Li-Hua;XU Zi-Jie;CHEN Long-Wu.Sol-Gel Synthesis of Alumina Using Inorganic Salt Precursor[J]. Acta Phys. -Chim. Sin., 2007,23(03): 289-294
102. LI Cui-Ping;ZHAO Rui-Hong;GUO Fen;CHEN Jian-Feng.Preparation and Characterization of Ni Catalysts Supported on Organized Mesoporous Alumina[J]. Acta Phys. -Chim. Sin., 2007,23(02): 157-161
103. ZHANG Yue-Wei;SHEN Mei-Qing;WU Xiao-Dong;WENG Duan;ZHANG Zhi-Hua;TIAN Ran;CHI Ke-Bin.Modification of the Structure and Properties of SAPO-11 Using Rare Earths[J]. Acta Phys. -Chim. Sin., 2006,22(12): 1495-1500
104. ZHAO Chun-Xia;CHEN Wen;LIU Qi;TIAN Gao.Influence of HCl on the Mesostructure and Morphology of the Ordered Mesoporous Silica[J]. Acta Phys. -Chim. Sin., 2006,22(10): 1201-1205
105. HU Jun;WANG Jian-Jun;ZHOU Li-Hui;XIE Song-Hai;LIU Hong-Lai.The Mechanism of Mesoporous Phase Transition of Titanic-Silica Mesoporous Materials[J]. Acta Phys. -Chim. Sin., 2006,22(06): 679-683
106. ZHANG Xue-Hong;TANG Xing-Hua;CHENG Xin-Sun.Synthesis and Application of Ce-doped Mesoporous TiO2[J]. Acta Phys. -Chim. Sin., 2006,22(05): 532-537
107. LI Xue-Hui;ZHANG Lei;WANG Le-Fu;TANG Ying-Biao.Characterization of N-carboxyl Appended Pyridine Task-Specific Ionic Liquids[J]. Acta Phys. -Chim. Sin., 2006,22(04): 430-435
108. GENG Wei-guo; LI Xue-hui; WANG Le-fu; DUAN Hong-li; PAN Wei-ping.Acidic Characterization of Polycarboxyl Imidazolium Ionic Liquids[J]. Acta Phys. -Chim. Sin., 2006,22(02): 230-233
109. HU Jun; ZHOU Li-hui; LI Hong-ning; LI Wan-xin; LIU Hong-lai; HU Ying.The Influences of the Spacer of Gemini Surfactants on the Structure of Silicic Mesoporous Materials[J]. Acta Phys. -Chim. Sin., 2005,21(11): 1217-1222
110. LIU Li-cheng; LI Hui-quan; CAI Wei-quan; ZHANG Yi.Synthesis, Characterization and Catalytic Activity of Mesoporous Cr-MSU-1[J]. Acta Phys. -Chim. Sin., 2005,21(11): 1311-1314
111. JIN Sheng-ming; QIU Guan-zhou; YANG Hua-ming; DENG Zhen-xia.Preparation of HMS and AlSBA Mesoporous Materials from Sepiolite[J]. Acta Phys. -Chim. Sin., 2005,21(07): 796-799
112. WANG Xiao-Hua; TAO Guo-Hong; WU Xiao-Mu; KOU Yuan.Investigation of the Acidity of Ionic Liquids by IR Spectroscopy[J]. Acta Phys. -Chim. Sin., 2005,21(05): 528-533
113. ZHENG Jun-Lin; ZHAI Shang-Ru; YANG Dong-Jiang; ZHANG Ye; WU Dong; SUN Yu-Han.Comparison on the Catalytic Cracking and Alkylation Activities between MSU-SMFI and MCM-41 Aluminosilicates[J]. Acta Phys. -Chim. Sin., 2005,21(03): 324-327
114. Dai Zhi-Hui;Ju Huang-Xian.Direct Electron Transfer of Protein Immobilized on Mesoporous Molecular Sieves Matrix[J]. Acta Phys. -Chim. Sin., 2004,20(10): 1262-1266
115. Piao Ling-Yu;Han Yang;Kou Yuan.The Reuse of Acidic Ionic Liquids as Catalysts in Diphenyl Oxide Alkylation with Dodecene[J]. Acta Phys. -Chim. Sin., 2004,20(09): 1083-1088
116. Zhu Jian-Hua;Xu Yang;Wang Ying;Zhou Shi-Lu;Zhou Chun-Fang.Adsorption and Catalytic Degradation of Nitrosamines by Zeolites and Molecular Sieves[J]. Acta Phys. -Chim. Sin., 2004,20(08S): 946-952
117. Chen Hong-Lin;Shen Bao-Jian;Pan Hui-Fang.Physicochemical and Catalytic Properties of ZSM-5/Y Composite Zeolites Dealuminated by the Steaming[J]. Acta Phys. -Chim. Sin., 2004,20(08): 854-859
118. Shi Xi-E;Zhai Shang-Ru;Dai Li-Yi;Shan Yong-Kui;He Ming-Yuan;Wei Wei;Wu Dong;Sun Yu-Han.Synthesis of Mesoporous Aluminosilicate Nanoparticles and Its Performance in Catalytic Cracking[J]. Acta Phys. -Chim. Sin., 2004,20(03): 265-270
119. Nie Chun-Fa;Suo Ji-Shuan.Synthesis,Characterization and Catalytic Applications of Asymmetric Hydrogenation Catalyst Immobilized on Hybrid MCM-41[J]. Acta Phys. -Chim. Sin., 2004,20(02): 149-153
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123. Wang Jin-Zhong;Zhao Yan;Zhang Cai-Bei.Synthesis of Ordered Mesoporous TiO2 on a Composite Surfactant Template[J]. Acta Phys. -Chim. Sin., 2003,19(03): 251-255
124. Song Chun-Min;Yan Zi-Feng;Max Lu.Synthesis and Characterization of Supersurface MCM-41 Zeolites[J]. Acta Phys. -Chim. Sin., 2002,18(03): 279-283
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