Progress in preparation and application of short b-axis ZSM-5 molecular sieve

doi:10.11949/0438-1157.20221461

Abstract

Abstract:

As one of the most widely used catalysts, the ZSM-5 molecular sieve has always been the focus of scholars’ research. Due to its better diffusion performance along the b-axis straight channels compared to that along the a-axis and c-axis the zigzag channels, the control of their length plays an important role in improving the catalytic properties of molecular sieves. The main methods for controlling the anisotropic growth of ZSM-5 molecular sieves are reviewed, including structure-oriented methods and growth modification methods. The application of short b-axis ZSM-5 molecular sieves in catalytic fields such as MTP, MTH, and MTG is analyzed in detail. It is also pointed out that lamellar molecular sieves prepared with specific quaternary ammonium salts as structural directing agents have a uniform and good self-pillared structure and intercrystalline mesopores. Due to the high difficulty in preparing structural directing agents, it is more economical and environmentally friendly to partially replace quaternary ammonium salts with growth modifiers. The synthesis of specific growth modifiers is low in difficulty and cost, and the prepared molecular sieves have dispersed or agglomerated lamellar structures. The development of new processes to improve intercrystalline mesopores will enable them to have better diffusivity. The in-depth study of the precise regulation of the thickness and acidity of lamellar molecular sieves, the synthesis mechanism, and the influence of anisotropic length on catalytic performance to ensure efficient preparation of molecular sieves that take into account conversion, selectivity, and stability is of great significance to the development of short b-axis molecular sieves.

Key words: short b-axis, molecular sieve, catalysis, selectivity, stability

摘要：

ZSM-5分子筛作为应用最为广泛的催化剂之一，一直是研究关注的重点。由于其沿着b轴直通孔道相比于沿着a轴和c轴的Z形孔道具有更好的扩散性能，其长度的控制对改善分子筛的催化特性具有重要作用。综述了控制ZSM-5分子筛各向生长的主要方法，结构导向法和生长修饰法。对短b轴ZSM-5分子筛在MTP、MTH以及MTG等催化领域的应用进行了具体分析。并指出，特定季铵盐作为结构导向剂制备的片层分子筛，具有均匀良好的自柱撑结构和晶间介孔，由于结构导向剂制备难度较高，采用生长修饰剂部分取代季铵盐更加经济环保。特定生长修饰剂合成难度低且成本低廉，制备的分子筛具有分散或团聚片层结构，新工艺的开发以改善晶间介孔将使其具有更好的扩散性。对片层分子筛厚度和酸性的精准调控、合成机理以及各向长度对催化性能影响的深入研究，以保证高效制备兼顾转化率、选择性以及稳定性的分子筛对短b轴分子筛的发展具有重要意义。

关键词: 短b轴, 分子筛, 催化, 选择性, 稳定性

CLC Number:

TQ 426.61

Zijian WANG, Ming KE, Jiahan LI, Shuting LI, Jinru SUN, Yanbing TONG, Zhiping ZHAO, Jiaying LIU, Lu REN. Progress in preparation and application of short b-axis ZSM-5 molecular sieve[J]. CIESC Journal, 2023, 74(4): 1457-1473.

王子健, 柯明, 李佳涵, 李舒婷, 孙巾茹, 童燕兵, 赵治平, 刘加英, 任璐. 短b轴ZSM-5分子筛制备方法及应用研究进展[J]. 化工学报, 2023, 74(4): 1457-1473.

Figures/Tables 13

Fig.1 Schematic representation of the steps used to fabricate MFI films with b- and a-out-of-plane orientations[22]

Fig.2 Crystallization of MFI nanosheets: (a) Structure model for the single MFI nanosheet (Surfactant molecules are aligned along the straight channel of MFI framework. Two quaternary ammonium groups (indicated as a red sphere) are located at the channel intersections. One is inside the framework, and the other is at the pore mouth of the external surface); (b) Many MFI nanosheets form either multilamellar stacking along the b-axis; (c) A random assembly of unilamellar structure [31]

Fig.3 TEM images of ZSM-5- (C18-[D-C6]3-DC18) samples before and after calcined[16]

Fig.4 Schematic representation of the transformation mechanism of the amorphous frameworks to SCZN [(a), (b)] and the

Fig.5 SEM images of ZSM-5 zeolites synthesized[45]

Fig.6 The approach for the formation of the ZSM-5 zeolite under F medium[52]

Fig.7 The mechanism for the formation of C-ZSM-5 crystals[45]

Fig.8 Formation mechanism of the single-crystalline hierarchical plate-like ZSM-5 crystal for zeolite syntheses in one step (at 170℃) or in two steps (at 80℃ and then at 170℃)[63]

Fig.9 Average product selectivity (a) and catalyst lifetime (b) for MTP reactions over the ZSM-5 catalysts [glucose/SiO2 is Z5-A: 0, Z5-B: 0.12, Z5-C: 0.24; Z5-C loading P is Z5-CP: 1.5%(mass), Z5-CP2: 2.0%(mass), Z5-CP3: 3.0%(mass)][76]

Fig.10 Methanol conversion of samples[78]

Fig. 11 Catalytic conversion of methanol (a); Product selectivity (LPG, C5+ and aromatics) (b); TG profiles (c) and GC-MS chromatograms (d) of organic species retained in the spent catalysts of U-ZSM-5-0.03 and SH-ZSM-5 after the methanol conversion[81]

Fig. 12 n-Heptane cracking performance of ZSM-5 nanosheets with different b-axis thicknesses: Conversion of n-heptane as a function of time on stream (a); TG analysis of coke content over spent ZSM-5 nanosheets (b)[86]

Fig. 13 Catalytic efficiency of synthesised SCMZ, MZIN and conventional ZSM-5[34]

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[3]	Yuyuan ZHENG, Zhiwei GE, Xiangyu HAN, Liang WANG, Haisheng CHEN. Progress and prospect of medium and high temperature thermochemical energy storage of calcium-based materials [J]. CIESC Journal, 2023, 74(8): 3171-3192.
[4]	Lingding MENG, Ruqing CHONG, Feixue SUN, Zihui MENG, Wenfang LIU. Immobilization of carbonic anhydrase on modified polyethylene membrane and silica [J]. CIESC Journal, 2023, 74(8): 3472-3484.
[5]	Yaxin CHEN, Hang YUAN, Guanzhang LIU, Lei MAO, Chun YANG, Ruifang ZHANG, Guangya ZHANG. Advances in enzyme self-immobilization mediated by protein nanocages [J]. CIESC Journal, 2023, 74(7): 2773-2782.
[6]	Xiaoling TANG, Jiarui WANG, Xuanye ZHU, Renchao ZHENG. Biosynthesis of chiral epichlorohydrin by halohydrin dehalogenase based on Pickering emulsion system [J]. CIESC Journal, 2023, 74(7): 2926-2934.
[7]	Tan ZHANG, Guang LIU, Jinping LI, Yuhan SUN. Performance regulation strategies of Ru-based nitrogen reduction electrocatalysts [J]. CIESC Journal, 2023, 74(6): 2264-2280.
[8]	Bin CAI, Xiaolin ZHANG, Qian LUO, Jiangtao DANG, Liyuan ZUO, Xinmei LIU. Research progress of conductive thin film materials [J]. CIESC Journal, 2023, 74(6): 2308-2321.
[9]	Lei MAO, Guanzhang LIU, Hang YUAN, Guangya ZHANG. Efficient preparation of carbon anhydrase nanoparticles capable of capturing CO₂ and their characteristics [J]. CIESC Journal, 2023, 74(6): 2589-2598.
[10]	Wenchao XU, Zhigao SUN, Cuimin LI, Juan LI, Haifeng HUANG. Effect of surfactant E-1310 on the formation of HCFC-141b hydrate under static conditions [J]. CIESC Journal, 2023, 74(5): 2179-2185.
[11]	Hao GU, Fujian ZHANG, Zhen LIU, Wenxuan ZHOU, Peng ZHANG, Zhongqiang ZHANG. Desalination performance and mechanism of porous graphene membrane in temporal dimension under mechanical-electrical coupling [J]. CIESC Journal, 2023, 74(5): 2067-2074.
[12]	Zheng ZHANG, Yongping HE, Haidong SUN, Rongzi ZHANG, Zhengping SUN, Jinlan CHEN, Yixuan ZHENG, Xiao DU, Xiaogang HAO. Electrochemically switched ion exchange device with serpentine flow field for selective extraction of lithium [J]. CIESC Journal, 2023, 74(5): 2022-2033.
[13]	Tianhao BAI, Xiaowen WANG, Mengzi YANG, Xinwei DUAN, Jie MI, Mengmeng WU. Study on release and inhibition behavior of COS during high-temperature gas desulfurization process using Zn-based oxide derived from hydrotalcite [J]. CIESC Journal, 2023, 74(4): 1772-1780.
[14]	Rong WANG, Yonghong WANG, Xinru ZHANG, Jinping LI. Construction of 6FDA-based polyimide carbon molecular sieve membranes for gas separation and its application [J]. CIESC Journal, 2023, 74(4): 1433-1445.
[15]	Xiangshang CHEN, Zhenjie MA, Xihua REN, Yue JIA, Xiaolong LYU, Huayan CHEN. Preparation and mass transfer efficiency of three-dimensional network extraction membrane [J]. CIESC Journal, 2023, 74(3): 1126-1133.