晶种法合成整体式多级孔ZSM-5分子筛
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摘要
以四丙基氢氧化铵为模板,采用原位水热法,添加Silicalite-1晶种和十六烷基三甲基溴化铵,一步合成直径约为2 cm、高约为0. 8 cm、中间部位向内凹、边缘部位凸起且表面较光滑的分子筛圆片集聚体。XRD、SEM和N_2吸附-脱附表征结果表明,该分子筛圆片集聚体是由小晶粒堆积成的具有微孔和介孔的多级孔ZSM-5分子筛。
Hierarchical ZSM-5 monolith with diameter of 2 cm and hight of 0. 8 cm was successfully synthesized by in-situ hydrothermal method using tetrapropylammonium hydroxide solution as template,adding silicalite-1 gel as seeds and hexadecyl trimethyl ammonium bromide. The synthesized ZSM-5 monolith was aggregates of molecular sieve disks with inward center,bulging edge and smooth surface. XRD,SEM and N_2 adsorption-desorption characterization results indicated that molecular sieve disks were miro-and meso-porous ZSM-5.
Hierarchical ZSM-5 monolith with diameter of 2 cm and hight of 0. 8 cm was successfully synthesized by in-situ hydrothermal method using tetrapropylammonium hydroxide solution as template,adding silicalite-1 gel as seeds and hexadecyl trimethyl ammonium bromide. The synthesized ZSM-5 monolith was aggregates of molecular sieve disks with inward center,bulging edge and smooth surface. XRD,SEM and N_2 adsorption-desorption characterization results indicated that molecular sieve disks were miro-and meso-porous ZSM-5.
引文
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[22]邵秀丽.晶种法合成TS-1分子筛催化剂[J].工业催化,2016,24(11):37-40.Shao Xiuli. Synthesis of TS-1 zeolite by the seed-induced method[J]. Industrial Catalysis,2016,24(11):37-40.
[2]Feng Hui,Chen Yanhong,Li Chunyi,et al. In-situ systhesis of ZSM-5 on silica gel and studies on its catalytic activity[J]. Journal of Fuel Chemistry and Technology,2008,36(2):144-150.
[3]Chang Fuxiang,Wei Yingxu,Liu Xianbin,et al. A mechanistic investigation of the coupled reaction of n-hexane and methanol over HZSM-5[J]. Applied Catalysis A:General,2007,328(2):163-173.
[4]Abul-Hamayel M A,Aitani A M,Saeed M R. Enhancement of propylene production in a downer FCC operation using a ZSM-5 additive[J]. Chemical Engineering&Technology,2005,28(8):923-929.
[5]Lee Y J,Lee J S,Park Y S,et al. Synthesis of large monolithic zeolite foams with variable macropore architectures[J]. Advanced Materials,2001,13(16):1259-1263.
[6]赵阳,郑亚峰,辛峰.整体式催化剂性能及应用的研究进展[J].化学反应工程与工艺,2004,20(4):357-362.Zhao Yang,Zheng Yafeng,Xin Feng. Properties and applications of monolithic catalysts[J]. Chemical Reaction Engineering&Technology,2004,20(4):357-362.
[7]Williams J L. Monolith structures,materials,properties,and uses[J]. Catalysis Today,2001,69(1):3-9.
[8]Lachman I M,Patil M D. Cryallising zeolite onto surface of monolithic ceramic substrate to obtain catalyst of industrial use:US,4800187[P]. 1989-01-24.
[9]Li Wencui,Lu Anhui,Schmidt W,et al. Hierarchically structured monolithic silicalite-1 consisting of crystallized nanoparticles and its performance in the beckmann rearrangement of cyclohexanone oxime[J]. Journal of the American Chemical Society,2005,127(36):12595-12600.
[10]Wang Yingyong,Jin Guoqiang,Guo Xiangyun. Growth of ZSM-5 coating on biomorphic porous silicon carbide derived from durra[J]. Microporous and Mesoporous Materials,2009,118(1):302-306.
[11]Liu Y,Thomas J P. Assembly of hydrothermally stable aluminosilicate foams and large-pore hexagonal mesostructures from zeolite seeds under strongly acidic conditions[J]. Chemistry of Materials,2002,14(1):3-5.
[12]Xiao Fengshou,Wang Lifeng,Yin Chengyang,et al. Catalytic properties of hierarchical Mmesoporous zeolites templated with a mixture of small organic ammonium salts and mesoscale cationic polymers[J]. Angewandte Chemie International Edition,2006,118(19):3162-3165.
[13]Liu Fujian,Willhammar T,Xiao Fengshou,et al. ZSM-5zeolite single crystals with b-axis-aligned mesoporous channels as an efficient catalyst for conversion of bulky organic molecules[J]. Journal of the American Chemical Society,2012,134(10):4557-4560.
[14]Choi M,Srivastava R,Ryoo R,et al. Organosilane surfactantdirected synthesis of mesoporous aluminophosphates constructed with crystalline microporous frameworks[J].Chemical Communications,2006,(42):4380-4382.
[15]Liu Min,Jia Wenzhi,Liu Xinhua,et al. Transalkylation properties of hierarchical MFI and MOR zeolites:direct synthesis over modulating the zeolite grow kinetics with controlled morphology[J]. Catalysis Letters,2018,148(5):1396-1406.
[16]Meng Lingqian,Zhu Xiaochun,Wannapakdee W,et al. A dual-templating synthesis strategy to hierarchical ZSM-5zeolites as efficient catalysts for the methanol-to-hydrocarbons reaction[J]. Journal of Catalysis,2018,361(2):135-142.
[17]Choi M,Na K,Kim J,et al. Stable single-unit-cell nanosheets of zeolite MFI as active and long-lived catalysts[J]. Nature,2009,461(7261):246-249.
[18]Na K,Choi M,Park W,et al. Pillared MFI zeolite nanosheets of a single-unit-cell thickness[J]. Journal of the American Chemical Society,2010,132(12):4169-4177.
[19]Chao Peiyu,Hsu C H,Loganathan,et al. One-pot synthesis of sheet-like MFI as high-performance catalyst for toluene disproportionation[J]. Journal of the American Chemical Society,2018,101(8):1-10.
[20]Liu Min,Li Junhui,Jia Wenzhi,et al. Seed-induced synthesis of hierarchical ZSM-5 nanosheets in the presence of hexadecyl trimethyl ammonium bromide[J]. Royal Society of Chemistry,2014,5(12):9237-9240.
[21]Schmidt F. Improved catalytic performance of hierarchical ZSM-5 synthesized by desilication with surfactants[J].Microporous Mesoporous Mater,2013,165:148-157.
[22]邵秀丽.晶种法合成TS-1分子筛催化剂[J].工业催化,2016,24(11):37-40.Shao Xiuli. Synthesis of TS-1 zeolite by the seed-induced method[J]. Industrial Catalysis,2016,24(11):37-40.