Seed-Assisted Synthesis and Catalytic Performance of Nano-sized ZSM-5 Aggregates in a One-Step Crystallization Process

Ziyang Wang , Yaquan Wang , Chao Sun , Aijuan Zhao , Cui Wang , Xu Zhang , Jingjing Zhao , Taotao Zhao , Wenrong Liu , Jiaxin Lu , Shuhui Wu

Transactions of Tianjin University ›› 2020, Vol. 26 ›› Issue (4) : 292 -304.

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Transactions of Tianjin University ›› 2020, Vol. 26 ›› Issue (4) : 292 -304. DOI: 10.1007/s12209-019-00223-w
Research Article

Seed-Assisted Synthesis and Catalytic Performance of Nano-sized ZSM-5 Aggregates in a One-Step Crystallization Process

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Abstract

Hierarchical nano-sized ZSM-5 aggregates were successfully synthesized via a seed-assisted method in the presence of cetyltrimethylammonium bromide (CTAB) through a facile one-step crystallization process. Commercial ZSM-5 zeolites with a SiO2/Al2O3 ratio comparable to that of ZSM-5 products were treated with alkali and used as the seed particles. The influences of crystallization conditions were investigated, and the possible synthesis mechanism was proposed. ZSM-5 zeolites with different amounts of CTAB added were characterized using many techniques and evaluated in toluene alkylation with methanol. The results showed that a trace amount of CTAB significantly promoted the crystallization of ZSM-5 zeolite, with the morphology changing from hexagonal-shape crystals to uniform spherical aggregates. CTAB may act as the structure-directing agent and assemble the primary crystallites to generate hierarchical ZSM-5 aggregates. The ZSM-5 zeolite with the smallest primary particles of 50–80 nm exhibited large specific surface area, abundant mesopores, and the greatest microporosity. The hierarchical nano-sized ZSM-5 aggregate showed higher toluene conversion and a longer lifetime without compromising the selectivity to xylene and p-xylene in toluene alkylation with methanol.

Keywords

Hierarchical ZSM-5 / Nano-sized aggregates / Seed-assisted / CTAB / Toluene alkylation with methanol

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Ziyang Wang, Yaquan Wang, Chao Sun, Aijuan Zhao, Cui Wang, Xu Zhang, Jingjing Zhao, Taotao Zhao, Wenrong Liu, Jiaxin Lu, Shuhui Wu. Seed-Assisted Synthesis and Catalytic Performance of Nano-sized ZSM-5 Aggregates in a One-Step Crystallization Process. Transactions of Tianjin University, 2020, 26(4): 292-304 DOI:10.1007/s12209-019-00223-w

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References

[1]

Miyake K, Hirota Y, Ono K, et al. Direct and selective conversion of methanol to para-xylene over Zn ion doped ZSM-5/silicalite-1 core-shell zeolite catalyst. J Catal, 2016, 342: 63-66.

[2]

Alabi W, Atanda L, Jermy R, et al. Kinetics of toluene alkylation with methanol catalyzed by pure and hybridized HZSM-5 catalysts. Chem Eng J, 2012, 195–196: 276-288.

[3]

Wang CF, Zhang Q, Zhu YF, et al. p-Xylene selectivity enhancement in methanol toluene alkylation by separation of catalysis function and shape-selective function. Mol Catal, 2017, 433: 242-249.

[4]

Li JH, Xiang H, Liu M, et al. The deactivation mechanism of two typical shape-selective HZSM-5 catalysts for alkylation of toluene with methanol. Catal Sci Technol, 2014, 4(8): 2639-2649.

[5]

Ahn JH, Kolvenbach R, Neudeck C, et al. Tailoring mesoscopically structured H-ZSM5 zeolites for toluene methylation. J Catal, 2014, 311: 271-280.

[6]

van Vu D, Miyamoto M, Nishiyama N, et al. Morphology control of silicalite/HZSM-5 composite catalysts for the formation of para-xylene. Catal Lett, 2009, 127(3–4): 233-238.

[7]

Ahn JH, Kolvenbach R, Al-Khattaf SS, et al. Methanol usage in toluene methylation with medium and large pore zeolites. ACS Catal, 2013, 3(5): 817-825.

[8]

Odedairo T, Balasamy RJ, Al-Khattaf S. Toluene disproportionation and methylation over zeolites TNU-9, SSZ-33, ZSM-5, and mordenite using different reactor systems. Ind Eng Chem Res, 2011, 50(6): 3169-3183.

[9]

Yashima T. Alkylation on synthetic zeolites I. Alkylation of toluene with methanol. J Catal, 1970, 16(3): 273-280.

[10]

Mikkelsen Ø, Rønning PO, Kolboe S. Use of isotopic labeling for mechanistic studies of the methanol-to-hydrocarbons reaction. Methylation of toluene with methanol over H-ZSM-5, H-mordenite and H-beta. Microporous Mesoporous Mater, 2000, 40(1–3): 95-113.

[11]

Zhu ZR, Chen QL, Zhu W, et al. Catalytic performance of MCM-22 zeolite for alkylation of toluene with methanol. Catal Today, 2004, 93–95: 321-325.

[12]

Zhu ZR, Chen QL, Xie ZK, et al. The roles of acidity and structure of zeolite for catalyzing toluene alkylation with methanol to xylene. Microporous Mesoporous Mater, 2006, 88(1–3): 16-21.

[13]

Tan W, Liu M, Zhao Y, et al. Para-selective methylation of toluene with methanol over nano-sized ZSM-5 catalysts: synergistic effects of surface modifications with SiO2, P2O5 and MgO. Microporous Mesoporous Mater, 2014, 196: 18-30.

[14]

Zhu ZR, Xie ZK, Chen QL, et al. Chemical liquid deposition with polysiloxane of ZSM-5 and its effect on acidity and catalytic properties. Microporous Mesoporous Mater, 2007, 101(1–2): 169-175.

[15]

Ghorbanpour A, Gumidyala A, Grabow LC, et al. Epitaxial growth of ZSM-5@silicalite-1: a core–shell zeolite designed with passivated surface acidity. ACS Nano, 2015, 9(4): 4006-4016.

[16]

Wu HY, Liu M, Tan W, et al. Effect of ZSM-5 zeolite morphology on the catalytic performance of the alkylation of toluene with methanol. J Energy Chem, 2014, 23(4): 491-497.

[17]

Aguado J, Serrano DP, Escola JM, et al. Low temperature synthesis and properties of ZSM-5 aggregates formed by ultra-small nanocrystals. Microporous Mesoporous Mater, 2004, 75(1–2): 41-49.

[18]

Hamidzadeh M, Komeili S, Saeidi M. Seed-induced synthesis of ZSM-5 aggregates using the Silicate-1 as a seed: characterization and effect of the Silicate-1 composition. Microporous Mesoporous Mater, 2018, 268: 153-161.

[19]

Madsen C, Jacobsen CJH. Nanosized zeolite crystals: convenient control of crystal size distribution by confined space synthesis. Chem Commun, 1999, 8: 673-674.

[20]

Schmidt I, Madsen C, Jacobsen CJH. Confined space synthesis. A novel route to nanosized zeolites. Inorg Chem, 2000, 39(11): 2279-2283.

[21]

Majano G, Darwiche A, Mintova S, et al. Seed-induced crystallization of nanosized Na-ZSM-5 crystals. Ind Eng Chem Res, 2009, 48(15): 7084-7091.

[22]

Jo C, Cho K, Kim J, et al. MFI zeolite nanosponges possessing uniform mesopores generated by bulk crystal seeding in the hierarchical surfactant-directed synthesis. Chem Commun, 2014, 50(32): 4175-4177.

[23]

Li MR, Oduro IN, Zhou YP, et al. Amphiphilic organosilane and seed assisted hierarchical ZSM-5 synthesis: crystallization process and structure. Microporous Mesoporous Mater, 2016, 221: 108-116.

[24]

Choi M, Na K, Kim J, et al. Stable single-unit-cell nanosheets of zeolite MFI as active and long-lived catalysts. Nature, 2009, 461(7261): 246-249.

[25]

Lok BM, Cannan TR, Messina CA. The role of organic molecules in molecular sieve synthesis. Zeolites, 1983, 3(4): 282-291.

[26]

Meng LQ, Mezari B, Goesten MG, et al. One-step synthesis of hierarchical ZSM-5 using cetyltrimethylammonium as mesoporogen and structure-directing agent. Chem Mater, 2017, 29(9): 4091-4096.

[27]

Meng LQ, Mezari B, Goesten MG, et al. Direct synthesis of hierarchical ZSM-5 zeolite using cetyltrimethylammonium as structure directing agent for methanol-to-hydrocarbons conversion. Catal Sci Technol, 2017, 7(19): 4520-4533.

[28]

Chen HB, Wang YQ, Meng FJ, et al. Aggregates of superfine ZSM-5 crystals: the effect of NaOH on the catalytic performance of methanol to propylene reaction. Microporous Mesoporous Mater, 2017, 244: 301-309.

[29]

Chen HB, Wang YQ, Sun C, et al. Aggregates of nano-sized ZSM-5 crystals synthesized with template-free and alkali-treated seeds for improving the catalytic performance in MTP reaction. Catal Commun, 2017, 100: 107-111.

[30]

Emeis CA. Determination of integrated molar extinction coefficients for infrared absorption bands of pyridine adsorbed on solid acid catalysts. J Catal, 1993, 141(2): 347-354.

[31]

Li HJ, Zhou XD, Di YH, et al. Effect of Si-ATP/CTAB ratio on crystal morphology, pore structure and adsorption performance of hierarchical (H) ZSM-11 zeolite. Microporous Mesoporous Mater, 2018, 271: 146-155.

[32]

Wang X, Chen HB, Meng FJ, et al. CTAB resulted direct synthesis and properties of hierarchical ZSM-11/5 composite zeolite in the absence of template. Microporous Mesoporous Mater, 2017, 243: 271-280.

[33]

Sun LY, Wang YQ, Chen HB, et al. Direct synthesis of hierarchical ZnZSM-5 with addition of CTAB in a seeding method and improved catalytic performance in methanol to aromatics reaction. Catal Today, 2018, 316: 91-98.

[34]

Jin LJ, Liu SB, Xie T, et al. Synthesis of hierarchical ZSM-5 by cetyltrimethylammonium bromide assisted self-assembly of zeolite seeds and its catalytic performances. React Kinet Mech Catal, 2014, 113(2): 575-584.

[35]

Meng FH, Wang YQ, Wang LN, et al. Influence of Br and Na+ in synthesis of Silicalite-1 on catalytic performance in vapor phase Beckmann rearrangement of cyclohexanone oxime. J Mol Catal A Chem, 2011, 335(1–2): 105-111.

[36]

Chen L, Xue T, Wu HH, et al. Hierarchical ZSM-5 nanocrystal aggregates: seed-induced green synthesis and its application in alkylation of phenol with tert-butanol. RSC Adv, 2018, 8(5): 2751-2758.

[37]

Xu DD, Jing ZF, Cao FL, et al. Surfactants with aromatic-group tail and single quaternary ammonium head for directing single-crystalline mesostructured zeolite nanosheets. Chem Mater, 2014, 26(15): 4612-4619.

[38]

Chen HB, Wang YQ, Meng FJ, et al. Conversion of methanol to propylene over nano-sized ZSM-5 zeolite aggregates synthesized by a modified seed-induced method with CTAB. RSC Adv, 2016, 6(80): 76642-76651.

[39]

Xue T, Chen L, Wang YM, et al. Seed-induced synthesis of mesoporous ZSM-5 aggregates using tetrapropylammonium hydroxide as single template. Microporous Mesoporous Mater, 2012, 156: 97-105.

[40]

Xue T, Li SS, Wu HH, et al. Eco-friendly and cost-effective synthesis of ZSM-5 aggregates with hierarchical porosity. Ind Eng Chem Res, 2017, 56(46): 13535-13542.

[41]

Yang JH, Yu SX, Hu HY, et al. Synthesis of ZSM-5 hierarchical microsphere-like particle by two stage varying temperature crystallization without secondary template. Chem Eng J, 2011, 166(3): 1083-1089.

[42]

Shang YS, Wang WG, Zhai YL, et al. Seed-fused ZSM-5 nanosheet as a superior MTP catalyst: synergy of micro/mesopore and inter/external acidity. Microporous Mesoporous Mater, 2019, 276: 173-182.

[43]

Wang Y, Ma JH, Ren FF, et al. Hierarchical architectures of ZSM-5 nanocrystalline aggregates with particular catalysis for lager molecule reaction. Microporous Mesoporous Mater, 2017, 240: 22-30.

[44]

Auerbach M, Carrado KA, Dutta PK. Handbook of zeolite science and technology, 2003, New York: Marcel Dekker.

[45]

Makarova MA, Ojo AF, Karim K, et al. FTIR study of weak hydrogen bonding of Broensted hydroxyls in zeolites and aluminophosphates. J Phys Chem, 1994, 98(14): 3619-3623.

[46]

Čejka J, Žilková N, Wichterlová B, et al. Decisive role of transport rate of products for zeolite para-selectivity: effect of coke deposition and external surface silylation on activity and selectivity of HZSM-5 in alkylation of toluene. Zeolites, 1996, 17(3): 265-271.

[47]

Wang C, Wang YQ, Chen HB, et al. Effect of phosphorus on the performance of IM-5 for the alkylation of toluene with methanol into p-xylene. C R Chim, 2019, 22(1): 13-21.

[48]

Hu HL, Lyu JH, Rui JY, et al. The effect of Si/Al ratio on the catalytic performance of hierarchical porous ZSM-5 for catalyzing benzene alkylation with methanol. Catal Sci Technol, 2016, 6(8): 2647-2652.

[49]

Fan CY, Wang YQ, Li HY, et al. Seed-induced synthesis of multilamellar ZSM-5 nanosheets directed by amphiphilic organosilane. New J Chem, 2018, 42(20): 17043-17055.

[50]

Mirth G, Lercher JA. Coadsorption of toluene and methanol on HZSM-5 zeolites. J Phys Chem, 1991, 95(9): 3736-3740.

[51]

Vinek H, Derewinski M, Mirth G, et al. Alkylation of toluene with methanol over alkali exchanged ZSM-5. Appl Catal, 1991, 68(1): 277-284.

[52]

Lu P, Fei ZY, Li L, et al. Effects of controlled SiO2 deposition and phosphorus and nickel doping on surface acidity and diffusivity of medium and small sized HZSM-5 for para-selective alkylation of toluene by methanol. Appl Catal A Gen, 2013, 453: 302-309.

[53]

Li JH, Ji WX, Liu M, et al. New insight into the alkylation-efficiency of methanol with toluene over ZSM-5: microporous diffusibility significantly affects reacting-pathways. Microporous Mesoporous Mater, 2019, 282: 252-259.

[54]

Sugimoto M, Katsuno H, Takatsu K, et al. Correlation between the crystal zize and catalytic properties of ZSM-5 zeolites. Zeolites, 1987, 7(6): 503-507.

[55]

Christensen CH, Johannsen K, Schmidt I, et al. Catalytic benzene alkylation over mesoporous zeolite single crystals: improving activity and selectivity with a new family of porous materials. J Am Chem Soc, 2003, 125(44): 13370-13371.

[56]

Holm MS, Taarning E, Egeblad K, et al. Catalysis with hierarchical zeolites. Catal Today, 2011, 168(1): 3-16.

[57]

Liu M, Li JH, Jia WZ, et al. Seed-induced synthesis of hierarchical ZSM-5 nanosheets in the presence of hexadecyl trimethyl ammonium bromide. RSC Adv, 2015, 5(12): 9237-9240.

[58]

Zhou J, Wang YD, Zou W, et al. Mass transfer advantage of hierarchical zeolites promotes methanol converting into para-methyl group in toluene methylation. Ind Eng Chem Res, 2017, 56(33): 9310-9321.

[59]

Zhao Y, Tan W, Wu HY, et al. Effect of Pt on stability of nano-scale ZSM-5 catalyst for toluene alkylation with methanol into p-xylene. Catal Today, 2011, 160(1): 179-183.

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