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Acidity and catalyst performance of two shape-selective HZSM-5 catalysts for alkylation of toluene with methanol

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Abstract

Two shape-selective HZSM-5 catalysts with similar pore size were prepared by silicalite-1 coating or boron modification, respectively. These catalysts samples were characterized by XRD, SEM, NH3-TPD, Py-IR and N2 adsorption–desorption isotherms and tested in the alkylation reaction of toluene with methanol. The results indicated that the boron modification weakened the acidity but increased the total amount of acidity sites, while the silicalite-1 coating led to the decrease of the strong acidity and total acidity. Due to the specific shape-selectivity that the micropore architecture afforded and the increment of the weak acid percentage, both catalysts exhibited a highp-xylene selectivity over 98%. Moreover, the higher toluene conversion would be retained once the strong acid sites in the micropores were remained as many as possible under the premise of the shape-selectivity of pore size.

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References

  1. Ghani NNM, Jalil AA, Triwahyono S, Aziz MAA, Rahman AFA, Hamid MYS, Izan SM, Nawawi MGM (2019) Tailored mesoporosity and acidity of shape-selective fibrous silica beta zeolite for enhanced toluene co-reaction with methanol. Chem Eng Sci 193:217–229

    Article CAS  Google Scholar 

  2. Teng H, Wang J, Chen D, Liu P, Wang X (2011) Silicalite-1 membrane on millimeter-sized HZSM-5 zeolite extrudates: controllable synthesis and catalytic behavior in toluene disproportionation. J Membr Sci 381(1–2):197–203

    Article CAS  Google Scholar 

  3. Wang C, Zhang Q, Zhu Y, Zhang D, Chen J, Chiang F-K (2017) p- Xylene selectivity enhancement in methanol toluene alkylation by separation of catalysis function and shape-selective function. Mol Catal 433:242–249

    Article CAS  Google Scholar 

  4. Wang C, Wang Y, Chen H, Wang X, Li H, Sun C, Sun L, Fan C, Zhang X (2019) Effect of phosphorus on the performance of IM-5 for the alkylation of toluene with methanol into p-xylene. C R Chim 22(1):13–21

    Article CAS  Google Scholar 

  5. Zhou J, Wang Y, Zou W, Wang C, Li L, Liu Z, Zheng A, Kong D, Yang W, Xie Z (2017) Mass transfer advantage of hierarchical zeolites promotes methanol converting into para-methyl group in toluene methylation. Ind Eng Chem Res 56(33):9310–9321

    Article CAS  Google Scholar 

  6. Ahn JH, Kolvenbach R, Gutiérrez OY, Al-Khattaf SS, Jentys A, Lercher JA (2015) Tailoring p-xylene selectivity in toluene methylation on medium pore-size zeolites. Microporous Mesoporous Mater 210:52–59

    Article CAS  Google Scholar 

  7. van Miltenburg A, Pawlesa J, Bouzga AM, Žilková N, Čejka J, Stöcker M (2009) Alkaline modification of MCM-22 to a 3D interconnected pore system and its application in toluene disproportionation and alkylation. Top Catal 52(9):1190–1202

    Article CAS  Google Scholar 

  8. Liu C, Long Y, Wang Z (2018) Optimization of conditions for preparation of ZSM-5@silicalite-1 core–shell catalysts via hydrothermal synthesis. Chin J Chem Eng 26(10):2070–2076

    Article CAS  Google Scholar 

  9. Ghiaci M, Abbaspur A, Arshadi M, Aghabarari B (2007) Internal versus external surface active sites in ZSM-5 zeolite. Part 2: toluene alkylation with methanol and 2-propanol catalyzed by modified and unmodified H3PO4/ZSM-5. Appl Catal A 316(1):32–46

    Article CAS  Google Scholar 

  10. Ghiaci M, Abbaspur A, Kalbasi R (2006) Internal versus external surface active sites in ZSM-5 zeolite. Part 1. Fries rearrangement catalyzed by modified and unmodified H3PO4/ZSM-5. Appl Catal A 298:32–39

    Article CAS  Google Scholar 

  11. Wu H, Liu M, Tan W, Hou K, Zhang A, Wang Y, Guo X (2014) Effect of ZSM-5 zeolite morphology on the catalytic performance of the alkylation of toluene with methanol. J Energy Chem 23(4):491–497

    Article  Google Scholar 

  12. Sun L, Guo X, Liu M, Wang X (2009) Ethylation of coking benzene over nanoscale HZSM-5 zeolites: Effects of hydrothermal treatment, calcination and La2O3 modification. Appl Catal A 355(1–2):184–191

    Article CAS  Google Scholar 

  13. Aboul-Gheit AK, Aboul-Enein AA, Awadallah AE, Ghoneim SA, Emam EA (2010) Para-xylene maximization, part VIII: promotion of H-ZSM-5 Zeolite by Pt and HF doping for use as catalysts in toluene alkylation with methanol. Chin J Catal 31(9–10):1209–1216

    Article CAS  Google Scholar 

  14. Tominaga K, Maruoka S, Gotoh M, Katada N, Niwa M (2009) HZSM-5 modified by silica CVD for shape-selective production of p-xylene: influence of in situ and ex situ preparation conditions of the zeolite. Microporous Mesoporous Mater 117(3):523–529

    Article CAS  Google Scholar 

  15. Okamoto M, Osafune Y (2011) MFI-type zeolite with a core–shell structure with minimal defects synthesized by crystal overgrowth of aluminum-free MFI-type zeolite on aluminum-containing zeolite and its catalytic performance. Microporous Mesoporous Mater 143(2–3):413–418

    Article CAS  Google Scholar 

  16. Vu DV, Miyamoto M, Nishiyama N, Ichikawa S, Egashira Y, Ueyama K (2008) Catalytic activities and structures of silicalite-1/H-ZSM-5 zeolite composites. Microporous Mesoporous Mater 115(1–2):106–112

    Article CAS  Google Scholar 

  17. Vanvu D, Miyamoto M, Nishiyama N, Egashira Y, Ueyama K (2006) Selective formation of para-xylene over H-ZSM-5 coated with polycrystalline silicalite crystals. J Catal 243(2):389–394

    Article CAS  Google Scholar 

  18. Zhang J, Zhu X, Wang G, Wang P, Meng Z, Li C (2017) The origin of the activity and selectivity of silicalite-1 zeolite for toluene methylation to para-xylene. Chem Eng J 327:278–285

    Article CAS  Google Scholar 

  19. Zhou J, Liu Z, Wang Y, Kong D, Xie Z (2017) Shape selective catalysis in methylation of toluene: development, challenges and perspectives. Front Chem Sci Eng 12(1):103–112

    Article CAS  Google Scholar 

  20. Breen JP, Burch R, Kulkarni M, McLaughlin D, Collier PJ, Golunski SE (2007) Improved selectivity in the toluene alkylation reaction through understanding and optimising the process variables. Appl Catal A 316(1):53–60

    Article CAS  Google Scholar 

  21. Van Vu D, Miyamoto M, Nishiyama N, Egashira Y, Ueyama K (2008) Morphology control of silicalite/HZSM-5 composite catalysts for the formation of para-xylene. Catal Lett 127(3–4):233–238

    Google Scholar 

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

    Article CAS  Google Scholar 

  23. Dedecek J, Balgová V, Pashkova V, Klein P, Wichterlová B (2012) Synthesis of ZSM-5 zeolites with defined distribution of Al atoms in the framework and multinuclear MAS NMR analysis of the control of Al distribution. Chem Mater 24(16):3231–3239

    Article CAS  Google Scholar 

  24. Masoumifard N, Guillet-Nicolas R, Kleitz F (2018) Synthesis of engineered zeolitic materials: from classical zeolites to hierarchical core-shell materials. Adv Mater 30(16):e1704439

    Article PubMed CAS  Google Scholar 

  25. Wang Q, Han W, Hu H, Lyu J, Xu X, Zhang Q, Wang H, Li X (2017) Influence of the post-treatment of HZSM-5 zeolite on catalytic performance for alkylation of benzene with methanol. Chin J Chem Eng 25(12):1777–1783

    Article  Google Scholar 

  26. Kaeding WW, Chu C, Young LB, Weinstein B, Butter SA (1981) Selective alkylation of toluene with methanol to produce para-Xylene. J Catal 67(1):159–174

    Article CAS  Google Scholar 

  27. Ghorbanpour A, Gumidyala A, Grabow LC, Crossley SP, Rimer JD (2015) Epitaxial growth of ZSM-5@Silicalite-1: a core-shell zeolite designed with passivated surface acidity. ACS Nano 9(4):4006–4016

    Article CAS PubMed  Google Scholar 

  28. Al-Khattaf S (2007) Xylenes reactions and diffusions in ZSM-5 zeolite-based catalyst. Ind Eng Chem Res 46(1):59–69

    Article CAS  Google Scholar 

  29. Tsai T-C, Wang I, Huang C-K, Liu S-D (2007) Study on ethylbenzene and xylene conversion over modified ZSM-5. Appl Catal A 321(2):125–134

    Article CAS  Google Scholar 

  30. Chen LZ, Feng YQ (1992) Toluene alkylation over ZSM-5 zeolite catalysts with skeletal and nonskeletal boron. Zeolites 12(4):347–350

    Article CAS  Google Scholar 

  31. Romannikov VN, Ione KG (1993) Alkylation of aromatics on B-containing ZSM-5 zeolites. React Kinet Catal Lett 51(1):151–159

    Article CAS  Google Scholar 

  32. Sotelo JL, Uguina MA, Valverde JL, Serrano DP (1994) Deactivation of toluene alkylation with methanol over magnesium-modified ZSM-5 shape selectivity changes induced by coke formation. Appl Catal A 114(2):273–285

    Article CAS  Google Scholar 

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Acknowledgements

This study was supported by the Key Science and Technology Foundation of Gansu Province (Grant No. 2016GS09293) and Natural Science Foundation of Gansu Province (Grant No. 18JR3RA143).

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Authors and Affiliations

  1. School of Petrochemical Engineering, Lanzhou University of Technology, Lanzhou, 730050, China

    Guixian Li, Chao Wu, Dong Ji, Peng Dong, Yongfu Zhang & Yong Yang

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Correspondence toYong Yang.

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Li, G., Wu, C., Ji, D.et al. Acidity and catalyst performance of two shape-selective HZSM-5 catalysts for alkylation of toluene with methanol.Reac Kinet Mech Cat129, 963–974 (2020). https://doi.org/10.1007/s11144-020-01732-9

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