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Study on synthesis of hierarchical ZSM-5 zeolite by seed method
Received date: 2023-11-22
Online published: 2024-05-15
Hierarchical nano-sized ZSM-5 aggregate zeolite was synthesized by seed-assisted method with sodium aluminate as aluminum source，silica sol as silicon source，Silicalite-1（S-1） as seeds and ammonium carbonate as auxiliary agent.The effects of the amount of ammonium carbonate，the amount of seed，the H2O/SiO2 ratio and the crystallization temperature on the physical properties of the hierarchical ZSM-5 zeolite were investigated.The characterization results of X-ray diffraction（XRD），scanning electron microscopy（SEM），and N2 adsorption-desorption indicated that the addition of ammonium carbonate reduced the pH value of the system，which slowed down the nucleation rate of the zeolite，and significantly reduced the relative crystallinity（RC） of ZSM-5.S-1 could increase the specific surface area and pore volume of ZSM-5 zeolite when it was added at a dosage of 5%~7%（mass fraction）.Furthermore，the H2O/SiO2 ratio had a significant effect on the morphology of ZSM-5 zeolite.The hierarchical ZSM-5 zeolite with more concentrated mesoporous distribution could be synthesized with H2O/SiO2 ratio of 45.Due to the improved accessibility of active centers and reactants，as well as the reduced residence time of reaction products in the pores，the zeolite exhibited excellent stability and selectivity for the alkylation of trimethylbenzene with methanol compared with the ZSM-5-180 zeolite.
Key words： seed-assisted method; ammonium carbonate; hierarchical; ZSM-5; alkylation
HAN Wenhua , HONG Luwei , LI Bin , ZHOU Wei , LIU Guanfeng , WANG Yinbin . Study on synthesis of hierarchical ZSM-5 zeolite by seed method[J]. Inorganic Chemicals Industry, 2024 , 56(5) : 128 -134 . DOI: 10.19964/j.issn.1006-4990.2023-0554
| 1 | 谢卓涵，韩贺，李孝国，等.纳米Ga-ZSM-5分子筛的合成及其在苯和稀乙烯烷基化反应中的应用［J］.无机盐工业，2022，54（2）：123-128. |
| XIE Zhuohan， HAN He， LI Xiaoguo，et al.Synthesis of nano Ga-ZSM-5 zeolite and its application in alkylation of benzene with dilute ethylene［J］.Inorganic Chemicals Industry，2022，54（2）：123-128. | |
| 2 | MENG Fanjun， WANG Xiao， WANG Shuhai，et al.Fluoride-treated HZSM-5 as a highly stable catalyst for the reaction of methanol to gasoline［J］.Catalysis Today，2017，298：226-233. |
| 3 | HAO Jing， CHENG Dangguo， CHEN Fengqiu，et al.N-Heptane catalytic cracking on ZSM-5 zeolite nanosheets：Effect of nanosheet thickness［J］.Microporous and Mesoporous Materials，2021，310：110647. |
| 4 | ZHAO Taotao， WANG Yaquan， SUN Chao，et al.Direct synthesis of hierarchical binder-free ZSM-5 and catalytic properties for MTP［J］.Microporous and Mesoporous Materials，2020，292：109731. |
| 5 | SUN Baochang， KANG Yingying， SHI Qin，et al.Synthesis of ZSM-5 by hydrothermal method with pre-mixing in a stirred-tank reactor［J］.The Canadian Journal of Chemical Engineering，2019，97（12）：3063-3073. |
| 6 | XING Aihua， ZHANG Nini， YUAN Delin，et al.Relationship between acidity，defective sites，and diffusion properties of nano-sheet ZSM-5 and its catalytic performance in the methanol to propylene reaction［J］.Industrial & Engineering Chemistry Research，2019，58（28）：12506-12515. |
| 7 | SHESTAKOVA D O， SASHKINA K A， PARKHOMCHUK E V.Template-free synthesis of hierarchical zeolite ZSM-5［J］.Petroleum Chemistry，2019，59（8）：838-844. |
| 8 | WU Zhijie， ZHAO Kaiqiang， ZHANG Yan，et al.Synthesis and consequence of aggregated nanosized ZSM-5 zeolite crystals for methanol to propylene reaction［J］.Industrial & Engineering Che- mistry Research，2019，58（25）：10737-10749. |
| 9 | 李孝国，米晓彤，曹辉，等.ZSM-5纳米薄片定向堆积合成分子筛团聚体［J］.无机盐工业，2022，54（1）：112-116. |
| LI Xiaoguo， MI Xiaotong， CAO Hui，et al.Synthesis of ZSM-5 aggregates assembled by oriented stacking nanosheets［J］.Inorganic Chemicals Industry，2022，54（1）：112-116. | |
| 10 | YANG K， YAN S， SANG Y，et al.Construction of hierarchical ZSM-5 zeolites by chelating-alkaline medium［J］.Materials Today Sustainability，2021，13：100070. |
| 11 | MENG F， WANG Y， WANG X.Methanol to gasoline over ZSM-5 zeolite treated with alkaline mixture with different ratios of TBA+/OH– ［J］.Kinetics and Catalysis，2018，59（3）：304-310. |
| 12 | BOUMEDIéNE B， NADJAT C， FATIHA D.The universal zeolite ZSM-5：Structure and synthesis strategies.A review［J］.Coordination Chemistry Reviews，2023，496：215397. |
| 13 | FENG Rui， YAN Xinlong， HU Xiaoyan，et al.Hierarchical ZSM-5 zeolite designed by combining desilication and dealumination with related study of n-heptane cracking performance［J］.Journal of Porous Materials，2018，25（6）：1743-1756. |
| 14 | CHEN Hengbao， WANG Yaquan， MENG Fanjun，et al.Aggregates of superfine ZSM-5 crystals：The effect of NaOH on the catalytic performance of methanol to propylene reaction［J］.Microporous and Mesoporous Materials，2017，244：301-309. |
| 15 | ZHOU Xiaoxia， CHEN Yu， GE Tongguang，et al.Sodium carbonate-assisted synthesis of hierarchically porous single-crystalline nanosized zeolites［J］.Science Bulletin，2017，62（14）：1018-1024. |
| 16 | ZHANG Hongbin， ZHAO Yang， ZHANG Hongxia，et al.Tailoring zeolite ZSM-5 crystal morphology/porosity through flexible utilization of silicalite-1 seeds as templates：Unusual crystallization pathways in a heterogeneous system［J］.Chemistry，2016，22（21）：7141-7151. |
| 17 | WANG Baorong， PENG Xinxin， ZHANG Wenfeng，et al.Hierarchical TS-1 synthesized via the dissolution-recrystallization process：Influence of ammonium salts［J］.Catalysis Communications，2017，101：26-30. |
| 18 | 洪鲁伟.纳米TS-1催化剂的改性及放大合成研究［D］.大连：大连理工大学，2014． |
| HONG Luwei.Modification and scale-up synthesis of nano-sized titanium silicalite-1［D］.Dalian：Dalian University of Technology，2014． | |
| 19 | HOU Zhanggui， MI Xiaotong， LI Xiaoguo，et al.Seed-assisted synthesis of ZSM-5 aggregates assembled from regularly stacked nanosheets and their performance in n-hexane aromatization［J］.Industrial & Engineering Chemistry Research，2021，60（32）：12100-12108. |
| 20 | ALONSO-DONCEL M， PERAL A， OCHOA-HERNáNDEZ C，et al.Tracking the evolution of embryonic zeolites into hierarchical ZSM-5［J］.Journal of Materials Chemistry A，2021，9（23）：13570-13587. |
| 21 | ZHANG Xinyan， DOU Tingting， WANG Yao，et al.Green synthesis of Cu-SSZ-13 zeolite by seed-assisted route for effective reduction of nitric oxide［J］.Journal of Cleaner Production，2019，236：117667. |
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