Citation: Kexin Yan, Zhaoqi Ye, Lingtao Kong, He Li, Xue Yang, Yahong Zhang, Hongbin Zhang, Yi Tang. Seed-Induced Synthesis of Disc-Cluster Zeolite L Mesocrystals with Ultrashort c-Axis: Morphology Control, Decoupled Mechanism, and Enhanced Adsorption[J]. Acta Physico-Chimica Sinica, ;2024, 40(9): 230801. doi: 10.3866/PKU.WHXB202308019 shu

Seed-Induced Synthesis of Disc-Cluster Zeolite L Mesocrystals with Ultrashort c-Axis: Morphology Control, Decoupled Mechanism, and Enhanced Adsorption

Kexin Yan ¹ ,
Zhaoqi Ye ¹ ,
Lingtao Kong ¹ ,
He Li ¹ ,
Xue Yang ¹ ,
Yahong Zhang ¹ ,
Hongbin Zhang ^1,2,, ,
Yi Tang ^1,,

1.
Department of Chemistry, Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Laboratory of Advanced Materials, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai 200433, China;
2.
Institute for Preservation of Chinese Ancient Books, Fudan University Library, Fudan University, Shanghai 200433, China

Corresponding author: Hongbin Zhang, Yi Tang,
Received Date: 12 August 2023
Revised Date: 2 October 2023
Accepted Date: 9 October 2023

Fund Project: The project was supported by the National Key R&D Program of China (2018YFA0209402) and the National Natural Science Foundation of China (22088101, 22175040).

Zeolites with short microporous channels offer advantages in the diffusion of guest molecules, leading to significant improvements in their adsorption and catalytic performance, as well as a reduction in coke formation during catalytic reactions. However, preparing zeolite L (LTL) with an ultrashort length (20–50 nm) along the c-axis has proven challenging due to its preferential growth behavior along the one-dimensional microporous channel direction. Additionally, the conventional synthesis method of zeolite L struggles to achieve both low aspect ratio and short length along the c-axis due to the coupling of nucleation and growth stages during crystallization. In this study, we present an innovative approach by utilizing seeds of nanorod-cluster zeolite L, pre-prepared under high alkalinity conditions, to synthesize a novel morphology of zeolite L mesocrystals. The resulting zeolite L product exhibits a unique cluster structure composed of a series of disc nanocrystals with an ultrashort c-axis length (approximately 29 nm), and the entire crystallization process is completed within just 4 h in a low alkaline system without the need for additional additives. This intentionally designed seed-induced synthesis method effectively decouples the nucleation and growth stages of zeolite L, enabling precise control of each stage to achieve the desired morphology. By analyzing the time-resolved evolution of mesoscopic nuclei and microscopic building units in the synthetic system, we find that the ring-cage structures dissolved from seeds exist as four-membered rings and eight-membered rings. These structures accelerate gel ordering and shorten the induction period. Meanwhile, the reserved part of the seeds provides densely-distributed nuclei for growth, resulting in the formation of the novel disc-cluster structures. Furthermore, by controlling growth conditions, we confirm the assembly of worm-like precursor particles during the growth period, allowing for precise regulation of the length along the c-axis of each disc within the range of 18 to 55 nm. Moreover, we extensively demonstrate the significantly enhanced adsorption and diffusion properties of zeolite L with an ultrashort c-axis for a range of model molecules, spanning sizes from 0.43 to 4.5 nm, in both gaseous and liquid phase systems. Our typical sample exhibits advantages in the diffusion rate of small molecules and the adsorption capacity of large molecules in the gaseous phase. It holds great potential for practical applications in the adsorption and separation of aromatic hydrocarbons, as well as the adsorption of dyes and proteins.
- Zeolite L,
- Crystallization mechanism,
- Nonclassical crystallization,
- Morphology regulation,
- Adsorption performance,
- Seed-assisted synthesis
1. [1]
  (1) Yao, J.; Wu, Q.; Fan, J.; Komiyama, S.; Yong, X.; Zhang, W.; Zhao, T.; Guo, Z.; Yang, G.; Tsubaki, N. ACS Nano 2021, 15 (8), 13568. doi: 10.1021/acsnano.1c04419
2. [2]
  (2) Qureshi, B. A.; Lan, X.; Arslan, M. T.; Wang, T. Ind. Eng. Chem. Res. 2019, 58 (28), 12611. doi: 10.1021/acs.iecr.9b01882
3. [3]
  (3) Verboekend, D.; Milina, M.; Mitchell, S.; Pérez-Ramírez, J. Cryst. Growth Des. 2013, 13 (11), 5025. doi: 10.1021/cg4010483
4. [4]
  (4) Verboekend, D.; Pérez-Ramírez, J. Catal. Sci. Technol. 2011, 1 (6), 879. doi: 10.1039/c1cy00150g
5. [5]
  (5) Petkovich, N. D.; Stein, A. Chem. Soc. Rev. 2013, 42 (9), 3721. doi: 10.1039/c2cs35308c
6. [6]
  (6) Sun, Y.; Cao, S.; Wang, J.; Tang, H.; Yang, Z.; Ma, T.; Gong, Y.; Mo, G.; Li, Z. ACS Sustain. Chem. Eng. 2022, 10 (29), 9431. doi: 10.1021/acssuschemeng.2c01813
7. [7]
  (7) Wang, C.; Fang, W.; Liu, Z.; Wang, L.; Liao, Z.; Yang, Y.; Li, H.; Liu, L.; Zhou, H.; Qin, X.; et al. Nat. Nanotechnol. 2022, 17 (7), 714. doi: 10.1038/s41565-022-01154-9
8. [8]
  (8) Su, X.; Liu, B.; Feng, C.; Wu, W. Microporous Mesoporous Mat. 2022, 344, 112215. doi: 10.1016/j.micromeso.2022.112215
9. [9]
  (9) Hao, J.; Xu, S.; Cheng, D.; Chen, F.; Zhan, X. Catal. Sci. Technol. 2022, 12 (12), 3912. doi: 10.1039/d2cy00154c
10. [10]
  (10) Yue, Q.; Liu, C.; Zhao, H.; Liu, H.; Ruterana, P.; Zhao, J.; Qin, Z.; Mintova, S. Nano Res. 2023. doi: 10.1007/s12274-023-5749-0
11. [11]
  (11) Xu, J.; Zhang, Z.; Yu, D.; Du, W.; Song, N.; Duan, X.; Zhou, X. Nano Res. 2023, 16 (5), 6278. doi: 10.1007/s12274-023-5440-5
12. [12]
  (12) Jardim, E. D. O.; Serrano, E.; Martínez, J. C.; Linares, N.; García-Martínez, J. Cryst. Growth Des. 2020, 20 (2), 515. doi: 10.1021/acs.cgd.9b01180
13. [13]
  (13) Linares, N.; Jardim, E. O.; Sachse, A.; Serrano, E.; Garcia-Martinez, J. Angew. Chem. Int. Ed. 2018, 57 (28), 8724. doi: 10.1002/anie.201803759
14. [14]
  (14) Schwieger, W.; Machoke, A. G.; Weissenberger, T.; Inayat, A.; Selvam, T.; Klumpp, M.; Inayat, A. Chem. Soc. Rev. 2016, 45 (12), 3353. doi: 10.1039/c5cs00599j
15. [15]
  (15) Hu, Y.; Liu, C.; Zhang, Y.; Ren, N.; Tang, Y. Microporous Mesoporous Mat. 2009, 119 (1–3), 306. doi: 10.1016/j.micromeso.2008.11.005
16. [16]
  (16) Larlus, O.; Valtchev, V. P. Chem. Mat. 2004, 16 (17), 3381. doi: 10.1021/cm0498741
17. [17]
  (17) Brent, R.; Stevens, S. M.; Terasaki, O.; Anderson, M. W. Cryst. Growth Des. 2010, 10 (12), 5182. doi: 10.1021/cg100964j
18. [18]
  (18) Brent, R.; Anderson, M. W. Angew. Chem. Int. Ed. 2008, 47 (29), 5327. doi: 10.1002/anie.200800977
19. [19]
  (19) Lee, Y.-J.; Lee, J. S.; Yoon, K. B. Microporous Mesoporous Mat. 2005, 80 (1–3), 237. doi: 10.1016/j.micromeso.2004.12.003
20. [20]
  (20) Ban, T.; Saito, H.; Naito, M.; Ohya, Y.; Takahashi, Y. J. Porous Mat. 2006, 14 (2), 119. doi: 10.1007/s10934-006-9016-z
21. [21]
  (21) Li, R.; Smolyakova, A.; Maayan, G.; Rimer, J. D. Chem. Mat. 2017, 29 (21), 9536. doi: 10.1021/acs.chemmater.7b03798
22. [22]
  (22) Das, R.; Ghosh, S.; Naskar, M. K. Mater. Lett. 2015, 143, 94. doi: 10.1016/j.matlet.2014.12.076
23. [23]
  (23) Lupulescu, A. I.; Kumar, M.; Rimer, J. D. J. Am. Chem. Soc. 2013, 135 (17), 6608. doi: 10.1021/ja4015277
24. [24]
  (24) Ye, Z.; Kong, L.; Zhao, Y.; Zhang, C.; Yang, X.; Yan, K.; Zhang, Y.; Zhang, H.; Tang, Y. Chem. Synth. 2022, 2 (4), 20. doi: 10.20517/cs.2022.25
25. [25]
  (25) Cho, H. S.; Hill, A. R.; Cho, M.; Miyasaka, K.; Jeong, K.; Anderson, M. W.; Kang, J. K.; Terasaki, O. Cryst. Growth Des. 2017, 17 (9), 4516. doi: 10.1021/acs.cgd.7b00832
26. [26]
  (26) Ruiz, A. Z.; Brühwiler, D.; Ban, T.; Calzaferri, G. Mon. Chem. 2004, 136 (1), 77. doi: 10.1007/s00706-004-0253-z
27. [27]
  (27) Li, R.; Linares, N.; Sutjianto, J. G.; Chawla, A.; Garcia-Martinez, J.; Rimer, J. D. Angew. Chem. Int. Ed. 2018, 57 (35), 11283. doi: 10.1002/anie.201805877
28. [28]
  (28) Zhang, F.; Chen, W.; Wu, Q.; Yang, Z.; Wang, L.; Meng, X.; Zhang, B.; Zheng, A.; Deng, F.; Liu, C.; et al. J. Phys. Chem. C 2020, 124 (25), 13819. doi: 10.1021/acs.jpcc.0c04315
29. [29]
  (29) Jain, R.; Chawla, A.; Linares, N.; Garcia Martinez, J.; Rimer, J. D. Adv. Mater. 2021, 33 (22), e2100897. doi: 10.1002/adma.202100897
30. [30]
  (30) Ye, Z.; Zhao, Y.; Zhang, H.; Zhang, Y.; Tang, Y. Chem. -Eur. J. 2020, 26 (28), 6147. doi: 10.1002/chem.201904807
31. [31]
  (31) Ye, Z.; Zhang, H.; Zhang, Y.; Tang, Y. Front. Chem. Sci. Eng. 2019, 14 (2), 143. doi: 10.1007/s11705-019-1852-x
32. [32]
  (32) Kim, D.; Ghosh, S.; Akter, N.; Kraetz, A.; Duan, X. Sci. Adv. 2022, 8, eabm8162. doi: 10.1126/sciadv.abm8162
33. [33]
  (33) Ye, Z.; Zhao, Y.; Zhang, H.; Shi, Z.; Li, H.; Yang, X.; Wang, L.; Kong, L.; Zhang, C.; Sheng, Z.; et al. J. Colloid Interface Sci. 2022, 608, 1366. doi: 10.1016/j.jcis.2021.10.125
34. [34]
  (34) Lin, F.; Ye, Z.; Kong, L.; Liu, P.; Zhang, Y.; Zhang, H.; Tang, Y. Nanomaterials 2022, 12 (9), 1601. doi: 10.3390/nano12091601
35. [35]
  (35) Yang, J.; Liu, J.; Liu, P.; Li, L.; Tang, X.; Shang, H.; Li, J.; Chen, B. Angew. Chem. Int. Ed. 2022, 61 (8), e202116850. doi: 10.1002/anie.202116850
36. [36]
  (36) Zhang, H.; Zhang, H.; Zhao, Y.; Shi, Z.; Zhang, Y.; Tang, Y. Chem. Mat. 2017, 29 (21), 9247. doi: 10.1021/acs.chemmater.7b03121
37. [37]
  (37) Zhang, H.; Zhao, Y.; Zhang, H.; Wang, P.; Shi, Z.; Mao, J.; Zhang, Y.; Tang, Y. Chem.-Eur. J. 2016, 22 (21), 7141. doi: 10.1002/chem.201600028
38. [38]
  (38) Jain, R.; Mallette, A. J.; Rimer, J. D. J. Am. Chem. Soc. 2021, 143 (51), 21446. doi: 10.1021/jacs.1c11014
39. [39]
  (39) Kumar, M.; Li, R.; Rimer, J. D. Chem. Mat. 2016, 28 (6), 1714. doi: 10.1021/acs.chemmater.5b04569
40. [40]
  (40) Groen, J. C.; Zhu, W.; Brouwer, S.; Huynink, S. J.; Kapteijn, F.; Moulijn, J. A.; Pérez-Ramírez, J. J. Am. Chem. Soc. 2007, 129 (2), 355. doi: 10.1021/ja065737o
41. [41]
  (41) Devi, R.; Borah, R.; Deka, R. C. Appl. Catal. A-Gen. 2012, 433–434, 122. doi: 10.1016/j.apcata.2012.05.010
42. [42]
  (42) Tangale, N. P.; Sonar, S. K.; Niphadkar, P. S.; Joshi, P. N. J. Ind. Eng. Chem. 2016, 40, 128. doi: 10.1016/j.jiec.2016.06.016
43. [43]
  (43) Li, C.; Xiong, G.; Liu, J. K.; Ying, P. L.; Xin, Q.; Feng, Z. C. J. Phys. Chem. B 2001, 105 (15), 2993. doi: 10.1021/jp0042359
44. [44]
  (44) Fan, F.; Sun, K.; Feng, Z.; Xia, H.; Han, B.; Lian, Y.; Ying, P.; Li, C. Chem.-Eur. J. 2009, 15 (13), 3268. doi: 10.1002/chem.200801916
45. [45]
  (45) Chua, Y. T.; Stair, P. C.; Wachs, I. E. J. Phys. Chem. B. 2001, 105 (36), 8600. doi: 10.1021/jp011366g
46. [46]
  (46) Yu, Y.; Xiong, G.; Li, C.; Xiao, F. Microporous Mesoporous Mat. 2001, 46 (1), 23. doi: 10.1016/s1387-1811(01)00271-2
47. [47]
  (47) Chen, C. T.; Iyoki, K.; Hu, P.; Yamada, H.; Ohara, K.; Sukenaga, S.; Ando, M.; Shibata, H.; Okubo, T.; Wakihara, T. J. Am. Chem. Soc. 2021, 143 (29), 10986. doi: 10.1021/jacs.1c03351
48. [48]
  (48) Dusselier, M.; Davis, M. E. Chem. Rev. 2018, 118 (11), 5265. doi: 10.1021/acs.chemrev.7b00738
49. [49]
  (49) Myers, A. L.; Prausnitz, J. M. AICHE J. 1965, 11 (1), 121. doi: 10.1002/aic.690110125
50. [50]
  (50) Choy, K. K. H.; Porter, J. F.; Mckay, G. J. Chem. Eng. Data 2000, 45 (4), 575. doi: 10.1021/je9902894
51. [51]
  (51) Bulut, E.; Özacar, M.; Şengil, İ. A. Microporous Mesoporous Mat. 2008, 115 (3), 234. doi: 10.1016/j.micromeso.2008.01.039
52. [52]
  (52) Hu, Y.; Zhang, Y.; Ren, N.; Tang, Y. J. Phys. Chem. C 2009, 113 (42), 18040. doi: 10.1021/jp903989p
53. [53]
  (53) Zhang, R.; Somasundaran, P. Adv. Colloid Interface Sci. 2006, 123, 213. doi: 10.1016/j.cis.2006.07.004
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Seed-Induced Synthesis of Disc-Cluster Zeolite L Mesocrystals with Ultrashort c-Axis: Morphology Control, Decoupled Mechanism, and Enhanced Adsorption

南开大学师唯/华北电力大学（保定）刘景维：二维配位聚合物中有序的亲锂冠醚位点用于无枝晶锂沉积

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通讯作者: 陈斌, bchen63@163.com