Constructing hierarchical ZSM-5 coated with small ZSM-5 crystals via oriented-attachment and in situ assembly for methanol-to-aromatics reaction

Abstract

Developing hierarchical and nanoscale ZSM-5 catalysts for diffusion-limited reactions has received ever-increasing attention. Here, ZSM-5 architecture integrated with hierarchical pores and nanoscale crystals was successfully prepared via in situ self-assembly of nanoparticles-coated silicalite-1. First, the oriented attachment of amorphous nanoparticles on external surface of silicalite-1 was achieved by controlling the alkalinity of Si-Al coating solution. The partial exposure of the external surface of silicalite-1 ensured the uniform removal of silicon in the bulk phase for the creation of hierarchical pores during the subsequent desilication-recrystallization. The uniform removal of silicon species in the bulk phase was mainly due to the synergistic effect of surface protection and alkaline etching, which could be balanced by regulating the relative amount of tetrapropylammonium cation and OH^– in desilication-recrystallization solution. Importantly, the removed silicon from silicalite-1 recrystallized and in situ assembled into final ZSM-5 nanocrystals induced by surface Si-Al nanoparticles. The hierarchical pores and nanoscale crystals on this integrated architecture not only promoted the removal of coke precursors from micropores but also provided large external specific surface (91 m²·g^–1) for coke deposition. Consequently, a much longer catalytic lifetime was achieved for methanol-to-aromatics reaction compared to conventional hollow structure ZSM-5 (84 h vs 46 h), with relatively high stability.

Key words： hierarchical ZSM-5; nanocrystal; integrated architecture; diffusion; coke

Competing interests

The authors declare that they have no competing interests.

Acknowledgements

We thank the financial support from the National Natural Science Foundation of China (Nos. 22278292, 21978191).

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://dx.doi.org/10.1007/s11705-024-2432-2 and is accessible for authorized users.

References

1 Rahimi N , Karimzadeh R . Catalytic cracking of hydrocarbons over modified ZSM-5 zeolites to produce light olefins: a review. Applied Catalysis A, General, 2011, 398(1–2): 1–17

2 Wang R , Gong Y , Wang P , He W , Song Y , Xin M , Jiang Q , Sha Y , Cao T , Song H , Lin W . In situ crystal engineering on 3D-printed woodpile scaffolds: a monolith catalyst with highly accessible active sites for enhanced catalytic cracking. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 2023, 11(26): 13945–13955

3 Alipour S M . Recent advances in naphtha catalytic cracking by nano ZSM-5: a review. Chinese Journal of Catalysis, 2016, 37(5): 671–680

4 Suganuma S , Nakamura K , Okuda A , Katada N . Enhancement of catalytic activity for toluene disproportionation by loading Lewis acidic nickel species on ZSM-5 zeolite. Molecular Catalysis, 2017, 435: 110–117

5 Liu N , Zhu X , Hua S , Guo D , Yue H , Xue B , Li Y . A facile strategy for preparation of phosphorus modified HZSM-5 shape-selective catalysts and its performances in disproportionation of toluene. Catalysis Communications, 2016, 77: 60–64

6 Miao L , Hong Z , Wang X , Jia W , Zhao G , Huang Y , Zhu Z . Catalytic synergistic effect of bis-ZSM-5 zeolite with different crystal sizes for xylene isomerization. Microporous and Mesoporous Materials, 2022, 332: 111718

7 Hao J , Feng P , Xin F , Wang Z , Zhou Z , Bao D , Zhu Z . A comprehensive kinetics for p-xylene increment by isomerizing C₈ aromatics over Pt/HZSM-5. Chemical Engineering Science, 2023, 268: 118425

8 Zhang J , Zhou A , Gawande K , Li G , Shang S , Dai C , Fan W , Han Y , Song C , Ren L , Zhang A , Guo X . b-Axis-Oriented ZSM-5 nanosheets for efficient alkylation of benzene with methanol: synergy of acid sites and diffusion. ACS Catalysis, 2023, 13(6): 3794–3805

9 Wang Y , He X , Yang F , Su Z , Zhu X . Control of framework aluminum distribution in MFI channels on the catalytic performance in alkylation of benzene with methanol. Industrial & Engineering Chemistry Research, 2020, 59(30): 13420–13427

10 Yan Z , Chen D , Huang L , Liu J , Fu H , Xiao Y , Li S . A theoretical insight into diffusion mechanism of benzene-methanol alkylation reaction in ZSM-5 zeolite. Microporous and Mesoporous Materials, 2022, 337: 111926

11 Li J , Liu M , Guo X , Xu S , Wei Y , Liu Z , Song C . Interconnected hierarchical ZSM-5 with tunable acidity prepared by a dealumination–realumination process: a superior MTP catalyst. ACS Applied Materials & Interfaces, 2017, 9(31): 26096–26106

12 Liu Z , Wu D , Ren S , Chen X , Qiu M , Liu G , Zeng G , Sun Y . Facile one-pot solvent-free synthesis of hierarchical ZSM-5 for methanol to gasoline conversion. RSC Advances, 2016, 6(19): 15816–15820

13 Liu P , Wang J , Ling L , Shen X , Li X , Zhang R , Wang B . Suitable location of Lewis acid over ZnOH⁺/HZSM-5 catalysts effectively enhance dehydrogenation activity and catalyze the aromatization process of C6 olefins in MTA. Fuel, 2024, 357: 130000

14 Bensafi B , Chouat N , Djafri F . The universal zeolite ZSM-5: structure and synthesis strategies: a review. Coordination Chemistry Reviews, 2023, 496: 215397

15 Peng P , Gao X , Yan Z , Mintova S . Diffusion and catalyst efficiency in hierarchical zeolite catalysts. National Science Review, 2020, 7(11): 1726–1742

16 Zhang H , Samsudin I B , Jaenicke S , Chuah G K . Zeolites in catalysis: sustainable synthesis and its impact on properties and applications. Catalysis Science & Technology, 2022, 12(19): 6024–6039

17 Kerstens D , Smeyers B , Van Waeyenberg J , Zhang Q , Yu J , Sels B F . State of the art and perspectives of hierarchical zeolites: practical overview of synthesis methods and use in catalysis. Advanced Materials, 2020, 32(44): 2004690

18 Li S , Yang H , Wang S , Wang J , Fan W , Dong M . Improvement of adsorption and catalytic properties of zeolites by precisely controlling their particle morphology. Chemical Communications (Cambridge), 2022, 58(13): 2041–2054

19 Grand J , Talapaneni S N , Vicente A , Fernandez C , Dib E , Aleksandrov H A , Vayssilov G N , Retoux R , Boullay P , Gilson J P , Valtchev V , Mintova S . One-pot synthesis of silanol-free nanosized MFI zeolite. Nature Materials, 2017, 16(10): 1010–1015

20 Kianfar E . Nanozeolites: synthesized, properties, applications. Journal of Sol-Gel Science and Technology, 2019, 91(2): 415–429

21 Zhang W , Bao X , Guo X , Wang X . A high-resolution solid-state NMR study on nano-structured HZSM-5 zeolite. Catalysis Letters, 1999, 60(1): 89–94

22 Wan Z , Li G K , Wang C , Yang H , Zhang D . Relating coke formation and characteristics to deactivation of ZSM-5 zeolite in methanol to gasoline conversion. Applied Catalysis A, General, 2018, 549: 141–151

23 Kim S , Park G , Woo M H , Kwak G , Kim S K . Control of hierarchical structure and framework-Al distribution of ZSM-5 via adjusting crystallization temperature and their effects on methanol conversion. ACS Catalysis, 2019, 9(4): 2880–2892

24 Javdani A , Ahmadpour J , Yaripour F . Nano-sized ZSM-5 zeolite synthesized via seeding technique for methanol conversions: a review. Microporous and Mesoporous Materials, 2019, 284: 443–458

25 Li C , Moliner M , Corma A . Building zeolites from precrystallized units: nanoscale architecture. Angewandte Chemie International Edition, 2018, 57(47): 15330–15353

26 Jain R , Mallette A J , Rimer J D . Controlling nucleation pathways in zeolite crystallization: seeding conceptual methodologies for advanced materials design. Journal of the American Chemical Society, 2021, 143(51): 21446–21460

27 Mochizuki H , Yokoi T , Imai H , Namba S , Kondo J N , Tatsumi T . Effect of desilication of H-ZSM-5 by alkali treatment on catalytic performance in hexane cracking. Applied Catalysis A, General, 2012, 449: 188–197

28 Chen L , Sun M , Wang Z , Yang W , Xie Z , Su B L . Hierarchically structured zeolites: from design to application. Chemical Reviews, 2020, 120(20): 11194–11294

29 Jiao Y , Forster L , Xu S , Chen H , Han J , Liu X , Zhou Y , Liu J , Zhang J , Yu J , D’Agostino C , Fan X . Creation of Al-enriched mesoporous ZSM-5 nanoboxes with high catalytic activity: converting tetrahedral extra-framework Al into framework sites by post treatment. Angewandte Chemie International Edition, 2020, 59(44): 19478–19486

30 Dai C , Zhang A , Li L , Hou K , Ding F , Li J , Mu D , Song C , Liu M , Guo X . Synthesis of hollow nanocubes and macroporous monoliths of silicalite-1 by alkaline treatment. Chemistry of Materials, 2013, 25(21): 4197–4205

31 Dai C , Zhang A , Li J , Hou K , Liu M , Song C , Guo X . Synthesis of yolk-shell HPW@Hollow silicalite-1 for esterification reaction. Chemical Communications, 2014, 50(37): 4846–4848

32 Dai C , Zhang A , Liu M , Gu L , Guo X , Song C . Hollow alveolus-like nanovesicle assembly with metal-encapsulated hollow zeolite nanocrystals. ACS Nano, 2016, 10(8): 7401–7408

33 Dai C , Zhang A , Liu M , Guo X , Song C . Hollow ZSM-5 with silicon-rich surface, double shells, and functionalized interior with metallic nanoparticles and carbon nanotubes. Advanced Functional Materials, 2015, 25(48): 7479–7487

34 Ren N , Yang Z , Lv X , Shi J , Zhang Y H , Tang Y . A seed surface crystallization approach for rapid synthesis of submicron ZSM-5 zeolite with controllable crystal size and morphology. Microporous and Mesoporous Materials, 2010, 131(1–3): 103–114

35 Zhai Y , Zhang X , Wang F , Lv G , Jiang T , Wu Y , Li M , Li M , Zhang Q , Liu Y . Racing crystallization mechanism for economical design of single-crystal hollow ZSM-5 with the broken limit of Si/Al ratio and improved mass transfer. ACS Applied Materials & Interfaces, 2021, 13(13): 15246–15260

36 Ou X , Xu S , Warnett J M , Holmes S M , Zaheer A , Garforth A A , Williams M A , Jiao Y , Fan X . Creating hierarchies promptly: microwave-accelerated synthesis of ZSM-5 zeolites on macrocellular silicon carbide (SiC) foams. Chemical Engineering Journal, 2017, 312: 1–9

37 Wang N , Li J , Sun W , Hou Y , Zhang L , Hu X , Yang Y , Chen X , Chen C , Chen B , Qian W . Rational design of zinc/zeolite catalyst: selective formation of p-xylene from methanol to aromatics reaction. Angewandte Chemie International Edition, 2022, 61(10): e202201057

38 Li S , Li J , Dong M , Fan S , Zhao T , Wang J , Fan W . Strategies to control zeolite particle morphology. Chemical Society Reviews, 2019, 48(3): 885–907