Abstract
The failure in some direct synthesis of hierarchical zeolite with a hard- or soft-templating method would be caused by the brittle binding forces between the templates and zeolite precursors or frameworks. In present work, high-quality hierarchically porous ZSM-5 with crystalline pore walls is synthesized by using hydroxylated carbon nanotubes (CNTs) as templates. Mesopores structure with a size of about 10–35 nm similar to the diameters of the CNTs template is successfully fabricated in the as-synthesized ZSM-5 zeolite. The structural and textural properties of the as-synthesized samples are revealed by characterization of X-ray powder diffraction, scanning electron microscopy, transmission electron microscopy, in situ infrared spectroscopy of pyridine, temperature-programmed desorption of ammonia (NH3-TPD), N2 adsorption–desorption, and nuclear magnetic resonance spectroscopy in details. Catalytic cracking of tri-isopropylbenzene is chosen as a probe reaction so as to explore the catalytic performances of the hierarchical zeolite because of its notably increased external surfaces resulted from the created hierarchical pore system. A hierarchically cracking manner of bulky reactants is found over the as-synthesized the meso-zeolite ZSM-5.
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References
Cundy CS, Cox PA (2005) The hydrothermal synthesis of zeolites: precursors, intermediates and reaction mechanism. ChemInform 82:1–78
Meng X, Liang W, Xiao FS (2017) Sustainable routes for synthesis of zeolite catalysts. In: Van de Voorde M, Sels B (eds) Nanotechnology in catalysis. Wiley, Berlin, pp 251–274
Meng X, Xiao FS (2014) Green routes for synthesis of zeolites. Chem Rev 114:1521–1543
Vogt ETC, Weckhuysen BM (2015) Fluid catalytic cracking: recent developments on the grand old lady of zeolite catalysis. Chem Soc Rev 44:7342–7370
Wang Z, Li C, Cho HJ, Shih-Chieh K, Mark AS, Wei F (2015) Direct, single-step synthesis of hierarchical zeolites without secondary templating. J Mater Chem A 3:1298–1305
He X, Ge T, Hua Z, Zhou J, Lv J, Zhou J, Liu Z, Shi J (2016) Mesoporogen-free synthesis of hierarchically structured zeolites with variable Si/Al ratios via a steam-assisted crystallization process. ACS Appl Mater Interfaces 8:7118–7124
Zhu J, Zhu YH, Zhu LK, Rigutto M, van der Made A, Yang CG, Pan SX, Wang L, Zhu LF, Jin YY, Sun Q, Wu QM, Meng XJ, Zhang DL, Han Y, Li JX, Chu YY, Zheng AM, Qiu SL, Zheng XM, Xiao FS (2014) Highly mesoporous single-crystalline zeolite beta synthesized using a nonsurfactant cationic polymer as a dual-function template. J Am Chem Soc 136:2503–2510
Wei Y, Parmentier TE, de Jong KP, Zečević J (2015) Tailoring and visualizing the pore architecture of hierarchical zeolites. Chem Soc Rev 44:7234–7261
Xu D, Ma Y, Jing Z, Han L, Singh B, Feng J, Shen X, Cao F, Oleynikov P, Sun H, Terasaki O, Che SA (2014) π–π interaction of aromatic groups in amphiphilic molecules directing for singlecrystalline mesostructured zeolite nanosheets. Nat Commun 5:4262–4271
Meng L, Mezari B, Goesten MG, Hensen EJM (2017) One-step synthesis of hierarchical ZSM-5 using cetyltrimethylammonium as mesoporogen and structure-directing agent. Chem Mater 29:4091–4096
Möller K, Bein T (2013) Mesoporosity—a new dimension for zeolites. Chem Soc Rev 42:3689–3707
Sachse A, García-Martínez J (2017) Surfactant-templating of zeolites: from design to application. Chem Mater 29:3827–3853
Verboekend D, Pérez-Ramírez J (2011) Design of hierarchical zeolite catalysts by desilication. Catal Sci Technol 1:879–890
Groen JC, Bach T, Ziese U, Paulaime-van Donk AM, de Jong KP, Moulijn JA, Pérez-Ramírez J (2005) Creation of hollow zeolite architectures by controlled desilication of Al-zoned ZSM-5 crystals. J Am Chem Soc 127:10792–10793
Li J, Liu M, Guo X, Xu S, Wei Y, Liu Z, Song C (2017) Interconnected hierarchical ZSM-5 with tunable acidity prepared by a dealumination–realumination process: a superior MTP catalyst. ACS Appl Mater Interfaces 9:26096–26106
Garcíamartínez J, Johnson M, Valla J, Li K, Ying J (2012) Mesostructured zeolite Y-high hydrothermal stability and superior FCC catalytic performance. Catal Sci Technol 2:987–994
Groen JC, Zhu WD, Brouwer S, Huynink SJ, Kapteijn F, Moulijn JA (2007) Direct demonstration of enhanced diffusion in mesoporous ZSM-5 zeolite obtained via controlled desilication. J Am Chem Soc 129:355–360
Möller K, Yilmaz B, Müller U, Bein T (2011) Hierarchical zeolite beta via nanoparticle assembly with a cationic polymer. Chem Mater 23:4301–4310
Zhou J, Hua Z, Liu Z, Wu W, Zhu Y, Shi JL (2011) Direct synthetic strategy of mesoporous ZSM-5 zeolites by using conventional block copolymer templates and the improved catalytic properties. ACS Catal 1:287–291
White RJ, Fischer A, Goebel C, Thomas A (2014) A sustainable template for mesoporous zeolite synthesis. J Am Chem Soc 136:2715–2718
Zhu H, Liu Z, Wang Y, Kong DJ, Yuan XH, Xie ZK (2008) Nanosized CaCO3 as hard template for creation of intracrystal pores within silicalite-1 crystal. Chem Mater 20:1134–1139
Jacobsen CJH, Madsen C, Houzvicka J, Schmidt I, Carlsson A (2000) Mesoporous zeolite single crystals. J Am Chem Soc 122:7116–7117
Schmidt I, Boisen A, Gustavsson E, Ståh K, Pehrson S, Dahl S, Carlsson A, Jacobsen CJH (2001) Carbon nanotube templated growth of mesoporous zeolite single crystals. Chem Mater 13:4416–4418
Zhang C, Chen H, Zhang X, Wang Q (2017) TPABr-grafted MWCNT as bifunctional template to synthesize hierarchical ZSM-5 zeolite. Mater Lett 197:111–114
Chen H, Zhang X, Zhang J, Wang Q (2017) Controllable synthesis of hierarchical ZSM-5 for hydroconversion of vegetable oil to aviation fuel-like hydrocarbons. RSC Adv 7:46109–46117
Tang K, Hong X, Qi JG (2011) Carbon nanotube templated growth of the nano-crystalline NaY zeolite. Adv Mater Res 194–196:594–597
Meng X, Nawaz F, Xiao FS (2009) Templating route for synthesizing mesoporous zeolites with improved catalytic properties. Nano Today 4:292–301
Choi M, Na K, Kim J, Sakamoto Y, Terasaki O, Ryoo R (2009) Stable single-unit-cell nanosheets of zeolite MFI as active and long-lived catalysts. Nature 461:246–249
Qiu Y, Wang L, Zhang X (2015) Different roles of CNTs in hierarchical HZSM-5 synthesis with hydrothermal and steam-assisted crystallization. RSC Adv 5:78238–78246
Groen JC, Peffer LAA, Pérez-Ramírez J (2003) Pore size determination in modified micro- and mesoporous materials. pitfalls and limitations in gas adsorption data analysis. Micropor Mesopor Mater 60:1–17
Neves TM, Fernandes JO, Lião LM, da Silva ED, da Rosa CA, Mortola VB (2019) Glycerol dehydration over micro- and mesoporous ZSM-5 synthesized from a one-step method. Micropor Mesopor Mater 275:244–252
Zhang HB, Hu ZJ, Huang L, Zhang HX, Song KS, Wang L, Shi ZP, Ma JX, Zhuang Y, Shen W, Zhang YH, Xu HL, Tang Y (2015) Dehydration of glycerol to acrolein over hierarchical ZSM-5 zeolites: effects of mesoporosity and acidity. ACS Catal 5:2548–2558
Li WC, Lu AH, Palkovits R, Schmidt W, Spliethoff B, Schüth F (2005) Hierarchically structured monolithic silicalite-1 consisting of crystallized nanoparticles and its performance in the Beckmann rearrangement of cyclohexanone oxime. J Am Chem Soc 127:12595–12600
Liu JY, Wang JG, Li N, Zhao H, Zhou HJ, Sun PC, Chen TH (2012) Polyelectrolyte-surfactant complex as a template for the synthesis of zeolites with intracrystalline mesopores. Langmuir 28:8600–8607
Pagis C, Prates ARM, Farrusseng D, Bats N, Tuel A (2016) Hollow zeolite structures: an overview of synthesis methods. Chem Mater 8:5205–5223
Sazama P, Dědeček J, Gábová V, Wichterlová B, Spoto G, Bordiga S (2008) Effect of aluminium distribution in the framework of ZSM-5 on hydrocarbon transformation. Cracking of 1-butene. J Catal 254:180–189
Araki S, Kiyohara Y, Tanaka S, Miyake Y (2012) Crystallization process of zeolite rho prepared by hydrothermal synthesis using 18-crown-6 ether as organic template. J Colloids Interf Sci 376:28–33
Nagy JB, Gabelica Z, Debras G, Bodart P, Derouane EG, Jacobs PA (1983) High-resolution magic-angle-spinning solid-state 29 Si NMR characterization of the structure and aluminium orderings of zeolites. J Mol Catal 20:327–336
Xin H, Li X, Fang Y, Yi X, Hu W, Chu Y, Zhang F, Zheng A, Zhang H, Li X (2014) Dehydration of Ethanol over Post-Treated ZSM-5 Zeolites. J Catal 312:204–215
Zhao QQ, Qin B, Zheng JJ, Du YZ, Sun WH, Ling FX, Zhang XW, Li RF (2014) Core-shell structured zeolite-zeolite composites comprising Y zeolite cores and nano-β zeolite shells: synthesis and application in hydrocracking of VGO oil. Chem Eng J 257:262–272
Du YZ, Kong QL, Gao ZH, Wang ZJ, Zheng JJ, Qin B, Pan M, Li WL, Li RF (2018) Flowerlike hierarchical Y with dramatically increased external surface: a potential catalyst contributing to improving precracking for Bulky reactant molecules. Ind Eng Chem Res 57:7395–7403
Wang QH, Zhang LC, Yao ZJ, Guo YN, Gao ZH, Zheng JJ, Li WL, Fan BB, Wang Y, Chen SW, Li RF (2020) Synthesis of loosely aggregating polycrystalline ZSM-5 with luxuriant mesopore structure and its hierarchically cracking for bulky reactants. Mater Chem Phys 243:122610–122618
Zheng JJ, Zhang HY, Liu YJ, Wang GS, Kong QL, Pan M, Tian HP, Li RF (2016) Synthesis of wool-ball-like ZSM-5 with enhanced external surfaces and improved diffusion: a potential high-efficiency FCC catalyst component for elevating pre-cracking of large molecules and catalytic longevity. Catal Lett 146:1457–1469
Vu X, Bentrup U, Hunger M, Kraehnert R, Armbruster U, Martin A (2014) Direct synthesis of nanosized-ZSM-5/SBA-15 analog composites from preformed ZSM-5 precursors for improved catalytic performance as cracking catalyst. J Mater Sci 49:5676–5689. https://doi.org/10.1007/s10853-014-8287-z
Yang XY, Tian G, Chen HL, Li Y, Rooke JC, Wei YX, Liu ZM, Deng Z, Van Tendeloo G, Su BL (2011) Well-organized zeolite nanocrystal aggregates with interconnected hierarchically micro-meso-macropore systems showing enhanced catalytic performance. Chem Eur J 17:14987–14995
Miao P, Li K, Fan J, Xu N, Zhu X, Li C (2019) Efficient ring-opening reaction of tetralin over nanosized ZSM-5 Zeolite: effect of SiO2/Al2O3 ratio and reaction condition. Energy Fuel 33:9480–9490
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This work is supported by NSFC (21371129, U19B2003, 21706177) and SinoPEC (116050).
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Zhang, L., Sun, X., Pan, M. et al. Interfacial effects between carbon nanotube templates and precursors on fabricating a wall-crystallized hierarchical pore system in zeolite crystals. J Mater Sci 55, 10412–10426 (2020). https://doi.org/10.1007/s10853-020-04708-1
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DOI: https://doi.org/10.1007/s10853-020-04708-1