Direct Synthesis of ITR Zeolites with Different Compositions for the Conversion of Methanol to Propylene

Abstract

ITR zeolites display great potential in the methanol to propylene (MTP) reaction, and one of the important factors influencing performance is their composition. Notably, the relationship between the composition of ITR zeolites and MTP performance has been rarely explored. In this work, ITR zeolites with different compositions were successfully synthesized by changing chemical elements in the starting synthesis gel. Characterization results of X-ray diffraction (XRD), scanning electron microscopy (SEM), nitrogen sorption isotherms, solid magic angle spinning nuclear magnetic resonance (MAS NMR), temperature programmed desorption of ammonia (NH₃-TPD), and pyridine adsorption infrared spectroscopy (Py-IR) showed that the obtained products had similar crystallinity, morphology, and textural parameters, but exhibited different acidic properties. The introduction of boron species increased the weak and Brønsted acid sites of ITR zeolites. Catalytic tests in the MTP reaction showed that the aluminoborosilicate ITR zeolites exhibited enhanced propylene selectivity and catalyst lifetime.

Keywords

ITR zeolite / Direct synthesis / Methanol to propylene / Composition

References

[1] Mei C, Wen P, Liu Z, Liu H, Wang Y, Yang W, Xie Z, Hua W, Gao Z. J. Catal., 2008, 258: 243

[2] Yu B, Lou C, Zhang W, Xu S, Han J, Yu Z, Wei Y, Liu Z. Chem. Res. Chinese Universities, 2020, 36: 1203

[3] Tian P, Wei Y, Ye M, Liu Z. ACS Catal., 2015, 5: 1922

[4] Lin L, Fan M, Sheveleva A, Han X, Tang Z, Carter J, Da Silva I, Parlett C, Tuna F, McInnes E, Sastre G, Rudic S, Cavaye H, Parker S, Cheng Y, Daemen L, Ramirez-Cuesta A, Attfield M, Liu Y, Tang C, Han B, Yang S. Nat. Commun., 2021, 12: 822

[5] Yang Y, Sun Q. Chem. J. Chinese Universities, 2023, 44: 20230119

[6] Ren L, Wang B, Lu K, Peng R, Guan Y, Jiang J-G, Xu H, Wu P. Chin. J. Catal., 2021, 42: 1147

[7] Wu Y, Zhang J, Shi Z, Chen C, Yue X, Sun Q. Chem.-Asian J., 2024, 19: e202400436

[8] Karim T, Toyoda H, Sawada M, Zhao L, Wang Y, Xiao P, Wang L, Huang J, Yokoi T. Chem. Bio. Eng., 2024, 1: 805

[9] Han D, Yang D, Bi C, Zhang G, Yang F, Hao Q, Zhang J, Chen H, Ma X. Inorg. Chem. Front., 2023, 10: 6193

[10] Hua J, Dong X, Wang J, Chen C, Shi Z, Liu Z, Han Y. ACS Catal., 2020, 10: 3009

[11] Zhang K, He G, Wang N, Dong Z, Ma Y, Xu J, Mei D, Sun Q, Yu J. J. Am. Chem. Soc., 2025, 147: 26277

[12] Li S, Si X, Peng R, Pan H, Xu H, Jiang J, Ma Y, Wu P. Micro. Meso. Mater., 2022, 335: 111843

[13] Zhu X, Gao Y, Liu M, Yang Z, Li S, Chen H, Liu B, Ma W, Hensen E, Shen B. Micro. Meso. Mater., 2022, 345: 112260

[14] Zhang J, Zhou A, Hao F, Yang K, Yu Y, Qin Y, Zhang X, Ren L, Zhang A, Zhang G, Song C, Guo X. Chem. Mater., 2025, 37: 3757

[15] Chen H, Lu X, Chen Y, Li B, Gao J, Liu L, Hou J, Li X. J. Porous Mater., 2025, 32: 1485

[16] Li J, Liu M, Guo X, Dai C, Song C. J. Energy Chem., 2018, 27: 1225

[17] Zhang Q, Chen G, Wang Y, Chen M, Guo G, Shi J, Luo J, Yu J. Chem. Mater., 2018, 30: 2750

[18] Corma A, Diaz-Cabanas M, Jorda J, Rey F, Sastre G, Strohmaier K. J. Am. Chem. Soc., 2008, 130: 16482

[19] Cumplido M, Diaz-Cabanas M. Micro. Meso. Mater., 2022, 341: 112009

[20] Ma Y, Hu J, Fan K, Chen W, Han S, Wu Q, Ma Y, Zheng A, Kunkes E, Baerdemaeker T, Parvulescu A-N, Bottke N, Yokoi T, De Vos D, Meng X, Xiao F-S. J. Am. Chem. Soc., 2023, 145: 17284

[21] Lei C, Dong Z, Martínez C, Martínez-Triguero J, Chen W, Wu Q, Meng X, Parvulescu A, De Baerdemaeker T, Müller U, Zheng A, Ma Y, Zhang W, Yokoi T, Marler B, De Vos D, Kolb U, Corma A, Xiao F-S. Angew. Chem. Int. Ed., 2020, 59: 15649

[22] Luan H, Chen W, Wu Q, Zheng A, Meng X, Baerdemaeker T, Parvulescu A-N, Müller U, Xiao F-S. Catal. Today, 2022, 405: 251

[23] Ma H, Chen Y, Wang S, Wei Z, Qin Z, Dong M, Li J, Fan W, Wang J. Catal. Sci. Technol., 2018, 8: 521

[24] Park J, Kim S, Seo M, Kim S, Sugi Y, Seo G. Appl. Catal. A, 2008, 349: 76

[25] Zhang J, Xu L, Zhang Y, Huang Z, Zhang X, Zhang X, Yuan Y, Xu L. J. Catal., 2018, 368: 248

[26] Dyballa M, Klemm E, Weitkamp J, Hunger M. Chem. Ing. Tech., 2013, 85: 1719

[27] Miguel J, Chung S-H, Dikhtiarenko A, Li T, Patarroyo J, Ruiz-Martínez J. ACS Catal., 2024, 14: 5989

[28] Hu Z, Zhang H, Wang L, Zhang H, Zhang Y, Xu H, Shen W, Tang Y. Catal. Sci. Technol., 2014, 4: 2891

[29] Luan H, Wu Q, Zhang J, Wang Y, Meng X, Xiao F-S. Chem. Res. Chinese Universities, 2022, 38: 136

[30] Hong X, Chen W, Zhang G, Wu Q, Lei C, Zhu Q, Meng X, Han S, Zheng A, Ma Y, Parvulescu A-N, Müller U, Zhang W, Yokoi T, Bao X, Marler B, De Vos D, Kolb U, Xiao F-S. J. Am. Chem. Soc., 2019, 141: 18318

[31] Li C, Vidal-Moya A, Miguel P, Dedecek J, Boronat M, Corma A. ACS Catal., 2018, 8: 7688

[32] Wang S, Li S, Zhang L, Qin Z, Dong M, Li J, Wang J, Fan W. Catal. Sci. Technol., 2017, 7: 4766

[33] Tuo J, Fan S, Yang N, Cheng S, Wang D, Zhang J, Ma Q, Gao X, Zhao T. Catal. Sci. Technol., 2020, 10: 7034

[34] Cui N, Guo H, Zhou J, Li L, Guo L, Hua Z. Micro. Meso. Mater., 2020, 306: 110411

[35] Ahmed M, Muraza O, Galadima A, Yoshioka M, Yamani Z, Yokoi T. Micro. Meso. Mater., 2019, 273: 249

[36] Bjørgen M, Joensen F, Lillerud K-P, Olsbye U, Svelle S. Catal. Today, 2009, 142: 90

[37] Zhu Q., Kondo J., Setoyama T., Yamaguchi M., Domen K., Tatsumi T., Chem. Commun., 2008, 5164.

[38] Zhu Q, Kondo J N, Yokoi T, Setoyama T, Yamaguchi M, Takewaki T, Domen K, Tatsumi T. Phys. Chem. Chem. Phys., 2011, 13: 14598

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Jilin University, The Editorial Department of Chemical Research in Chinese Universities and Springer-Verlag GmbH

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