Citation: Wen-Sen SONG, Saulat Hammad, Tao YAN, Jin-Yin LÜ, Jian-Hua YANG, Jin-Ming LU, Yan ZHANG. Preparation of MFI Zeolite Nanosheets and b-Oriented MFI Zeolite Film[J]. Chinese Journal of Inorganic Chemistry, ;2022, 38(9): 1781-1789. doi: 10.11862/CJIC.2022.159 shu

Preparation of MFI Zeolite Nanosheets and b-Oriented MFI Zeolite Film

State Key Laboratory of Fine Chemicals, Institute of Adsorption and Inorganic Membrane, School of Chemical Engineering, Dalian University of Technology, Dalian, Liaoning 116024, China

Corresponding author: Jian-Hua YANG, yjianhua@dlut.edu.cn
Received Date: 28 March 2022
Revised Date: 4 June 2022

Figures(6)

Herein, the bottom - up method was utilized for the synthesis of MFI nanosheet with a high aspect ratio and crystallinity by using homemade dC5 (bis-1, 5(tripropyl ammonium). b-Oriented MFI nanosheets seed layer was coated on glass supports by slip coating method with an average thickness of about 100 nm. The SDA (structure - directing agent) free secondary growth of the MFI nanosheet layer was conducted to effectively seal the interlayer and nanoscale gap among the nanosheet layer. The SDA-free secondary growth effectively preserves the b- orientation of the MFI film while maintaining the minimal thickness. A continuous and dense b-oriented MFI zeolite film with a thickness of about 200 nm was prepared under n_SiO₂∶n_Na₂O∶n_C₂H₅OH∶n_H₂O=1∶0.03∶1.3∶0.89 with a crystallization time and temperature of 48 h and 180 ℃, respectively. A significant decrease was observed in the thickness (approxi-mately 90%) of the synthesized film by the SDA-free secondary growth method as compared to MFI zeolite film pre-pared by the conventional secondary growth method containing tetrapropylammonium hydroxide (TPAOH) as SDA that fails to preserve the desired b-orientation of the film.
- two-dimensional material,
- MFI zeolite nanosheet,
- b-oriented MFI zeolite film
1. [1]
  Peng Y, Lu H B, Wang Z B, Yan Y S. Microstructural Optimization of MFI-Type Zeolite Membranes for Ethanol-Water Separation[J]. J. Mater. Chem. A, 2014,2(38):16093-16100. doi: 10.1039/C4TA02837F
2. [2]
  Lai Z P, Bonilla G, Diaz I, Nery J G, Sujaoti K, Amat M A, Kokkoli E, Terasaki O, Thompson R W, Tsapatsis M, Vlachos D G. Microstructural Optimization of a Zeolite Membrane for Organic Vapor Separation[J]. Science, 2003,300(5618):456-460. doi: 10.1126/science.1082169
3. [3]
  Hong Z, Wu Z J, Zhang Y T, Gu X H. Catalytic Cracking Deposition of Methyldiethoxysilane for Modification of Zeolitic Pores in MFI/ α-Al₂O₃ Zeolite Membrane with H+ Ion Exchange Pretreatment[J]. Ind. Eng. Chem. Res., 2013,52(36):13113-13119. doi: 10.1021/ie4012563
4. [4]
  Kim S, Yang S W, Reddy G K, Smirniotis P, Dong J H. Zeolite Membrane Reactor for High-Temperature Water-Gas Shift Reaction: Effects of Membrane Properties and Operating Conditions[J]. Energy Fuels, 2013,27(8):4471-4480. doi: 10.1021/ef302014n
5. [5]
  Dong Y J, Peng Y, Wang G L, Wang Z B, Yan Y S. Corrosion-Resistant Zeolite Silicalite-1 Coatings Synthesized by Seeded Growth[J]. Ind. Eng. Chem. Res., 2012,51(9):3646-3652. doi: 10.1021/ie202080a
6. [6]
  Lai Z P, Tsapatsis M, Nicolich J P. Siliceous ZSM-5 Membranes by Secondary Growth of b-Oriented Seed Layers[J]. Adv. Funct. Mater., 2004,14(7):716-729. doi: 10.1002/adfm.200400040
7. [7]
  Wang Z B, Yan Y S. Controlling Crystal Orientation in Zeolite MFI Thin Films by Direct In Situ Crystallization[J]. Chem. Mater., 2001,13(3):1101-1107. doi: 10.1021/cm000849e
8. [8]
  Gora L, Kuhn J, Baimpos T, Nikolakis V, Kapteijn F, Serwicka E M. Selective Sensor Utilizing a Thin Monolayer of b-Oriented Silicalite-1 Crystals Magneto -elastic Ribbon Assembly[J]. Analyst, 2009,134(10):2118-2122. doi: 10.1039/b905039f
9. [9]
  Wang X X, Yang G H, Zhang J F, Chen S Y, Wu Y Q, Zhang Q D, Wang J W, Han Y Z, Tan Y S. Synthesis of Isoalkanes over a Core (Fe-Zn-Zr)-Shell (Zeolite) Catalyst by CO₂ Hydrogenation[J]. Chem. Commun., 2016,52(46):7352-7355. doi: 10.1039/C6CC01965J
10. [10]
  Maas H, Calzaferri G. Trapping Energy from and Injecting Energy into Dye-Zeolite Nanoantennae[J]. Angew. Chem. Int. Ed., 2002,41(13):2284-2288. doi: 10.1002/1521-3773(20020703)41:13<2284::AID-ANIE2284>3.0.CO;2-5
11. [11]
  Liu Y, Qiang W L, Ji T T, Zhang M, Li M Y, Lu J M, Liu Y. Uniform Hierarchical MFI Nanosheets Prepared via Anisotropic Etching for Solution-Based Sub-100-nm-Thick Oriented MFI Layer Fabrication[J]. Sci. Adv., 2020,6(7)aay5993. doi: 10.1126/sciadv.aay5993
12. [12]
  Varoon K, Zhang X Y, Elyassi B, Brewer D D, Gettel M, Kumar S, Lee J A, Maheshwari S, Mittal A, Sung C Y, Cococcioni M, Francis L F, McCormick A V, Mkhoyan K A, Tsapatsis M. Dispersible Exfoliated Zeolite Nanosheets and Their Application as a Selective Membrane[J]. Science, 2011,334(6052):72-75. doi: 10.1126/science.1208891
13. [13]
  Luo R W, Ni X X, Bai P, Lyu J F, Guo X H. Fabrication of b-Oriented Silicalite-1 Membrane by Confined Space Dissolution and Recrystallization[J]. J. Porous Mater., 2022,29(2):423-431. doi: 10.1007/s10934-021-01194-x
14. [14]
  WU Y Q, ZHENG L K, CHEN Q, YU M T, WANG J G, ZHANG F M, XIAO Q, ZHU W D. Fabrication of Zeolite Membranes Using Two-Dimensional Open-Pore MFI Nanosheets as Building Blocks[J]. Chinese J. Inorg. Chem., 2019,35(1):89-94.
15. [15]
  Jeon M Y, Kim D H, Kumar P, Lee P S, Rangnekar N, Bai P, Shete M, Elyassi B, Lee H S, Narasimharao K, Basahel S N, Al-Thabaiti S, Xu W Q, Cho H J, Fetisov E O, Thyagarajan R, DeJaco R F, Fan W, Mkhoyan K A, Siepmann J I, Tsapatsis M. Ultra -Selective High-Flux Membranes from Directly Synthesized Zeolite Nanosheets[J]. Nature, 2017,543(7647):690-694. doi: 10.1038/nature21421
16. [16]
  Cao Z S, Zeng S X, Xu Z, Arvanitis A, Yang S W, Gu X H, Dong J H. Ultrathin ZSM-5 Zeolite Nanosheet Laminated Membrane for High-Flux Desalination of Concentrated Brines[J]. Sci. Adv., 2018,4(11)eaau8634. doi: 10.1126/sciadv.aau8634
17. [17]
  Peng Y, Li Y S, Ban Y J, Jin H, Jiao W M, Liu X L, Yang W S. Metal-Organic Framework Nanosheets as Building Blocks for Molecular Sieving Membranes[J]. Science, 2014,346(6215):1356-1359. doi: 10.1126/science.1254227
18. [18]
  Agrawal K V, Topuz B, Jiang Z Y, Nguenkam K, Elyassi B, Francis L F, Tsapatsis M, Navarro M. Solution-Processable Exfoliated Zeolite Nanosheets Purified by Density Gradient Centrifugation[J]. AlChE J., 2013,59(9):3458-3467. doi: 10.1002/aic.14099
19. [19]
  Rangnekar N, Shete M, Agrawal K V, Topuz B, Kumar P, Guo Q, Ismail I, Alyoubi A, Basahel S, Narasimharao K, Macosko C W, Mkhoyan K A, Al-Thabaiti S, Stottrup B, Tsapatsis M. 2D Zeolite Coatings: Langmuir-Schaefer Deposition of 3 nm Thick MFI Zeolite Nanosheets[J]. Angew. Chem. Int. Ed., 2015,54(22):6571-6575. doi: 10.1002/anie.201411791
20. [20]
  Mabande G T P, Ghosh S, Lai Z P, Schwieger W, Tsapatsis M. Preparation of b-Oriented MFI Films on Porous Stainless Steel Substrates[J]. Ind. Eng. Chem. Res., 2005,44(24):9086-9095. doi: 10.1021/ie050668s
21. [21]
  Elyassi B, Jeon M Y, Tsapatsis M, Narasimharao K, Basahel S N, Al-Thabaiti S. Ethanol/Water Mixture Pervaporation Performance of b-Oriented Silicalite -1 Membranes Made by Gel-Free Secondary Growth[J]. AlChE J., 2016,62(2):556-563. doi: 10.1002/aic.15124
22. [22]
  Agrawal K V, Topuz B, Pham T C T, Nguyen T H, Sauer N, Rangnekar N, Zhang H, Narasimharao K, Basahel , S N, Francis L F, Macosko C W, Al-Thabaiti S, Tsapatsis M, Yoon K B. Oriented MFI Membranes by Gel-Less Secondary Growth of Sub-100 nm MFI-Nanosheet Seed Layers[J]. Adv. Mater., 2015,27(21):3243-3249. doi: 10.1002/adma.201405893
23. [23]
  Min B, Yang S W, Korde A, Kwon Y H, Jones C W, Nair S. Continuous Zeolite MFI Membranes Fabricated from 2D MFI Nanosheets on Ceramic Hollow Fibers[J]. Angew. Chem. Int. Ed., 2019,58(24):8201-8205. doi: 10.1002/anie.201903554
24. [24]
  Wu Q M, Zhu L F, Chu Y Y, Liu X L, Zhang C S, Zhang J, Xu H, Xu J, Deng F, Feng Z C, Meng X J, Xiao F S. Sustainable Synthesis of Pure Silica Zeolites from a Combined Strategy of Zeolite Seeding and Alcohol Filling[J]. Angew. Chem. Int. Ed., 2019,58(35):12138-12142. doi: 10.1002/anie.201906559
25. [25]
  Han S C, Liu P, Ma Y, Wu Q M, Meng Y J, Xiao F S. Calcination-Free Fabrication of Highly b -Oriented Silicalite-1 Zeolite Films by Secondary Growth in the Absence of Organic Structure Directing Agents[J]. Ind. Eng. Chem. Res., 2021,60(19):7167-7173. doi: 10.1021/acs.iecr.1c01102
26. [26]
  Yang S W, Cao Z S, Arvanitis A, Sun X H, Xu Z, Dong J H. DDR-Type Zeolite Membrane Synthesis, Modification and Gas Permeation Studies[J]. J. Membr. Sci., 2016,505:194-204. doi: 10.1016/j.memsci.2016.01.043
27. [27]
  Bonilla G, Díaz I, Tsapatsis M, Jeong H, Lee Y J, Vlachos D G. Zeolite (MFI) Crystal Morphology Control Using Organic Structure-Directing Agents[J]. Chem. Mater., 2004,16(26):5697-5705. doi: 10.1021/cm048854w
28. [28]
  DONG W Y, REN Y, LONG Y C. In-Situ Synthesis of B -Al -MFI -Type Zeolite Membranes on a Porous Glass Disc by Substrate Self-Transformation[J]. Acta Chim. Sinica, 2000,58(11):1311-1315.
29. [29]
  Lee I, Buday J L, Jeong H. μ-Tiles and Mortar Approach: A Simple Technique for the Facile Fabrication of Continuous b-Oriented MFI Silicalite-1 Thin Films[J]. Microporous Mesoporous Mater., 2009,122(1):288-293.
30. [30]
  Peng Y, Lu X F, Wang Z B, Yan Y S. Fabrication of b-Oriented MFI Zeolite Films under Neutral Conditions without the Use of Hydrogen Fluoride[J]. Angew. Chem. Int. Ed., 2015,54(19):5709-5712. doi: 10.1002/anie.201412482
31. [31]
  Lu X F, Peng Y, Wang Z B, Yan Y S. A Facile Fabrication of Highly b-Oriented MFI Zeolite Films in the TEOS-TPAOH-H₂O System without Additives[J]. Microporous Mesoporous Mater., 2016,230:49-57. doi: 10.1016/j.micromeso.2016.04.037
32. [32]
  Zhou M, Korelskiy D, Ye P C, Grahn M, Hedlund J. A Uniformly Oriented MFI Membrane for Improved CO₂ Separation[J]. Angew. Chem. Int. Ed., 2014,53(13):3492-3495. doi: 10.1002/anie.201311324
33. [33]
  Lu X F, Peng Y, Wang Z B, Yan Y S. Rapid Fabrication of Highly b-Oriented Zeolite MFI Thin Films Using Ammonium Salts as Crystallization-Mediating Agents[J]. Chem. Commun., 2015,51(55):11076-11079. doi: 10.1039/C5CC02980E
34. [34]
  Peng Y, Xu R L. Insights into 1, 2-Dihydroxybenzene Addition on Twin Suppression during the Secondary Hydrothermal Synthesis of b-Oriented MFI Zeolite Films[J]. J. Mater. Sci., 2020,55(3):967-975. doi: 10.1007/s10853-019-03971-1
35. [35]
  Lu X F, Yang Y W, Zhang J J, Yan Y S, Wang Z B. Solvent-Free Secondary Growth of Highly b-Oriented MFI Zeolite Films from Anhydrous Synthetic Powder[J]. J. Am. Chem. Soc., 2019,141(7):2916-2919. doi: 10.1021/jacs.9b00018
36. [36]
  Kim D H, Shete M, Tsapatsis M. Large-Grain, Oriented, and Thin Zeolite MFI Films from Directly Synthesized Nanosheet Coatings[J]. Chem. Mater., 2018,30(10):3545-3551. doi: 10.1021/acs.chemmater.8b01346
37. [37]
  Luo R W, Ding H, Lyu J F, Fu T Y, Bai P, Guo X H, Tsapatsis M. Fabrication of a Sandwiched Silicalite-1 Membrane in a 2D Confined Space for Enhanced Alcohol/Water Separation[J]. Chem. Commun., 2020,56(83):12586-12588. doi: 10.1039/D0CC05019A
38. [38]
  Zhou M, Hedlund J. Facile Preparation of Hydrophobic Colloidal MFI and CHA Crystals and Oriented Ultrathin Films[J]. Angew. Chem. Int. Ed., 2018,57(34):10966-10970. doi: 10.1002/anie.201806502
1. [1]
  Jiao CHEN , Yi LI , Yi XIE , Dandan DIAO , Qiang XIAO . Vapor-phase transport of MFI nanosheets for the fabrication of ultrathin b-axis oriented zeolite membranes. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 507-514. doi: 10.11862/CJIC.20230403
2. [2]
  Mengfei He , Chao Chen , Yue Tang , Si Meng , Zunfa Wang , Liyu Wang , Jiabao Xing , Xinyu Zhang , Jiahui Huang , Jiangbo Lu , Hongmei Jing , Xiangyu Liu , Hua Xu . Epitaxial Growth of Nonlayered 2D MnTe Nanosheets with Thickness-Tunable Conduction for p-Type Field Effect Transistor and Superior Contact Electrode. Acta Physico-Chimica Sinica, 2025, 41(2): 100016-. doi: 10.3866/PKU.WHXB202310029
3. [3]
  Huayan Liu , Yifei Chen , Mengzhao Yang , Jiajun Gu . 二维材料基超级电容器的容量与倍率性能提升策略. Acta Physico-Chimica Sinica, 2025, 41(6): 100063-. doi: 10.1016/j.actphy.2025.100063
4. [4]
  Pengyu Dong , Yue Jiang , Zhengchi Yang , Licheng Liu , Gu Li , Xinyang Wen , Zhen Wang , Xinbo Shi , Guofu Zhou , Jun-Ming Liu , Jinwei Gao . NbSe₂纳米片优化钙钛矿太阳能电池的埋底界面. Acta Physico-Chimica Sinica, 2025, 41(3): 2407025-. doi: 10.3866/PKU.WHXB202407025
5. [5]
  Jia Zhou , Huaying Zhong . Experimental Design of Computational Materials Science Combined with Machine Learning. University Chemistry, 2025, 40(3): 171-177. doi: 10.12461/PKU.DXHX202406004
6. [6]
  Huanhuan XIE , Yingnan SONG , Lei LI . Two-dimensional single-layer BiOI nanosheets: Lattice thermal conductivity and phonon transport mechanism. Chinese Journal of Inorganic Chemistry, 2025, 41(4): 702-708. doi: 10.11862/CJIC.20240281
7. [7]
  Shiyang He , Dandan Chu , Zhixin Pang , Yuhang Du , Jiayi Wang , Yuhong Chen , Yumeng Su , Jianhua Qin , Xiangrong Pan , Zhan Zhou , Jingguo Li , Lufang Ma , Chaoliang Tan . 铂单原子功能化的二维Al-TCPP金属-有机框架纳米片用于增强光动力抗菌治疗. Acta Physico-Chimica Sinica, 2025, 41(5): 100046-. doi: 10.1016/j.actphy.2025.100046
8. [8]
  Baohua LÜ , Yuzhen LI . Anisotropic photoresponse of two-dimensional layered α-In₂Se₃(2H) ferroelectric materials. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1911-1918. doi: 10.11862/CJIC.20240105
9. [9]
  Runhua Chen , Qiong Wu , Jingchen Luo , Xiaolong Zu , Shan Zhu , Yongfu Sun . 缺陷态二维超薄材料用于光/电催化CO₂还原的基础与展望. Acta Physico-Chimica Sinica, 2025, 41(3): 2308052-. doi: 10.3866/PKU.WHXB202308052
10. [10]
  Juntao Yan , Liang Wei . 2D S-Scheme Heterojunction Photocatalyst. Acta Physico-Chimica Sinica, 2024, 40(10): 2312024-. doi: 10.3866/PKU.WHXB202312024
11. [11]
  Ran HUO , Zhaohui ZHANG , Xi SU , Long CHEN . Research progress on multivariate two dimensional conjugated metal organic frameworks. Chinese Journal of Inorganic Chemistry, 2024, 40(11): 2063-2074. doi: 10.11862/CJIC.20240195
12. [12]
  Fan JIA , Wenbao XU , Fangbin LIU , Haihua ZHANG , Hongbing FU . Synthesis and electroluminescence properties of Mn²⁺ doped quasi-two-dimensional perovskites (PEA)₂Pb_yMn_1-yBr₄. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1114-1122. doi: 10.11862/CJIC.20230473
13. [13]
  Yongzhi LI , Han ZHANG , Gangding WANG , Yanwei SUI , Lei HOU , Yaoyu WANG . A two-dimensional metal-organic framework for the determination of nitrofurantoin and nitrofurazone in aqueous solution. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 245-253. doi: 10.11862/CJIC.20240307
14. [14]
  .
  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
  . CCS Chemistry, 2025, 7(0): -.
15. [15]
  Jie ZHAO , Huili ZHANG , Xiaoqing LU , Zhaojie WANG . Theoretical calculations of CO₂ capture and separation by functional groups modified 2D covalent organic framework. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 275-283. doi: 10.11862/CJIC.20240213
16. [16]
  Pei Li , Yuenan Zheng , Zhankai Liu , An-Hui Lu . Boron-Containing MFI Zeolite: Microstructure Control and Its Performance of Propane Oxidative Dehydrogenation. Acta Physico-Chimica Sinica, 2025, 41(4): 100034-. doi: 10.3866/PKU.WHXB202406012
17. [17]
  Jiali CHEN , Guoxiang ZHAO , Yayu YAN , Wanting XIA , Qiaohong LI , Jian ZHANG . Machine learning exploring the adsorption of electronic gases on zeolite molecular sieves. Chinese Journal of Inorganic Chemistry, 2025, 41(1): 155-164. doi: 10.11862/CJIC.20240408
18. [18]
  Xingyang LI , Tianju LIU , Yang GAO , Dandan ZHANG , Yong ZHOU , Meng PAN . A superior methanol-to-propylene catalyst: Construction via synergistic regulation of pore structure and acidic property of high-silica ZSM-5 zeolite. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1279-1289. doi: 10.11862/CJIC.20240026
19. [19]
  Yikai Wang , Xiaolin Jiang , Haoming Song , Nan Wei , Yifan Wang , Xinjun Xu , Cuihong Li , Hao Lu , Yahui Liu , Zhishan Bo . 氰基修饰的苝二酰亚胺衍生物作为膜厚不敏感型阴极界面材料用于高效有机太阳能电池. Acta Physico-Chimica Sinica, 2025, 41(3): 2406007-. doi: 10.3866/PKU.WHXB202406007
20. [20]
  Weihan Zhang , Menglu Wang , Ankang Jia , Wei Deng , Shuxing Bai . 表面硫物种对钯-硫纳米片加氢性能的影响. Acta Physico-Chimica Sinica, 2024, 40(11): 2309043-. doi: 10.3866/PKU.WHXB202309043

Get Citation

PDF

XML

Metrics

PDF Downloads(24)
Abstract views(2130)
HTML views(458)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Preparation of MFI Zeolite Nanosheets and b-Oriented MFI Zeolite Film

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

Metrics

通讯作者: 陈斌, bchen63@163.com