Citation: 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[J]. Chinese Journal of Inorganic Chemistry, ;2024, 40(7): 1279-1289. doi: 10.11862/CJIC.20240026 shu

A superior methanol-to-propylene catalyst: Construction via synergistic regulation of pore structure and acidic property of high-silica ZSM-5 zeolite

Xingyang LI ¹ ,
Tianju LIU ¹ ,
Yang GAO ¹ ,
Dandan ZHANG ¹ ,
Yong ZHOU ^{1, 2,,} ,
Meng PAN ^1,,

1.
School of Chemical and Environmental Engineering, Anhui Polytechnic University, Wuhu, Anhui 241000, China
2.
Eco-materials and Renewable Energy Research Center, School of Physics, Nanjing University, Nanjing 210000, China

Corresponding author: Yong ZHOU, zhouyong1999@nju.edu.cn Meng PAN, panmeng@ahpu.edu.cn
Received Date: 19 January 2024
Revised Date: 19 April 2024

Figures(8)

Combined strategy of alkali treatment and chromium modification was used to synergistically regulate the pore structure and acidic property of the high-silica ZSM-5 zeolite. During the alkaline treatment, the abundant intergrowth boundaries constructed by adjusting the composition of the synthesis gel induced the formation of meso-pores. Thereby, the limitation of the conventional alkali treatment method coming from the framework Si/Al ratio of parent zeolite was circumvented. In the process of chromium modification, the unique hierarchical pore structure promoted the dispersion of chromium species in the catalyst. Thus, a deep modification of the acidic property was realized. As a result, a high-silica hierarchical zeolite catalyst with suitable acidities was obtained. During the catalytic conversion of methanol to propylene, the variation of the pore structure and acidic property caused obvious changes in the coke deposition behavior of the catalyst and the mass transfer of products. Consequently, the prepared catalyst exhibited excellent catalytic stability and a high selectivity towards propylene and total light olefins.
- methanol to propylene,
- hierarchical pore,
- acidity regulation,
- zeolite,
- catalytic performance
1. [1]
  Cui T L, Lv L B, Zhang W B, Li X H, Chen J S. Programmable synthesis of mesoporous ZSM-5 nanocrystals as selective and stable catalysts for the methanol-to-propylene process[J]. Catal. Sci. Technol., 2016,6(14):5262-5266. doi: 10.1039/C6CY00379F
2. [2]
  Kim H Y, Lee B, Lim D J, Choe C G, Lim H K. What is the best green propylene production pathway?: Technical, economic, and environmental assessment[J]. Green Chem., 2021,23(19):7635-7645. doi: 10.1039/D1GC01791H
3. [3]
  Yarulina I, Chowdhury A D, Meirer F, Weckhuysen B M, Gascon J. Recent trends and fundamental insights in the methanol-to-hydrocarbons process[J]. Nat. Catal., 2018,1(6):398-411. doi: 10.1038/s41929-018-0078-5
4. [4]
  Hwang A, Le T T, Shi Z, Dai H, Rimer J D, Bhan A. Effects of diffusional constraints on lifetime and selectivity in methanol-to-olefins catalysis on HSAPO-34[J]. J. Catal., 2019,369:122-132. doi: 10.1016/j.jcat.2018.10.031
5. [5]
  Khanmohammadi M, Amani S, Garmarudi A B, Niaei A. Methanol-to-propylene process: Perspective of the most important catalysts and their behavior[J]. Chin. J. Catal., 2016,37(3):325-339. doi: 10.1016/S1872-2067(15)61031-2
6. [6]
  Zhang W N, Zhi Y C, Huang J D, Wu X Q, Zeng S, Xu S T, Zheng A M, Wei Y X, Liu Z M. Methanol to olefins reaction route based on methylcyclopentadienes as critical intermediates[J]. ACS Catal., 2019,9(8):7373-7379. doi: 10.1021/acscatal.9b02487
7. [7]
  REN K, ZHANG L L, LI Z, FU Y J. Structure-activity relationship and reaction characteristics of propene aromatization catalyzed by ZSM-5[J]. Chinese J. Inorg. Chem., 2022,38(6):1090-1102.
8. [8]
  Yarulina I, De Wispelaere K, Bailleul S, Goetze J, Radersma M, Abou-Hamad E, Vollmer I, Goesten M, Mezari B, Hensen E J M, Martínez-Espín J S, Morten M, Mitchell S, Perez-Ramirez J, Olsbye U, Weckhuysen B M, Van Speybroeck V, Kapteijn F, Gascon J. Structure-performance descriptors and the role of Lewis acidity in the methanol-to-propylene process[J]. Nat. Chem., 2018,10(8):804-812. doi: 10.1038/s41557-018-0081-0
9. [9]
  Li H Y, Wang Y Q, Fan C Y, Sun C, Wang X, Wang C, Zhang X, Wang S H. Facile synthesis of a superior MTP catalyst: Hierarchical micro-meso-macroporous ZSM-5 zeolites[J]. Appl. Catal. A-Gen., 2018,551:34-48. doi: 10.1016/j.apcata.2017.12.007
10. [10]
  Kerstens D, Smeyers B, Van Waeyenberg J, Zhang Q, Yu J H, Sels B F. State of the art and perspectives of hierarchical zeolites: Practical overview of synthesis methods and use in catalysis[J]. Adv. Mater., 2020,32(44)e2004690. doi: 10.1002/adma.202004690
11. [11]
  Bai R S, Song Y, Li Y, Yu J H. Creating hierarchical pores in zeolite catalysts[J]. Trends Chem., 2019,1(6):601-611. doi: 10.1016/j.trechm.2019.05.010
12. [12]
  Qi R Y, Fu T J, Wan W L, Li Z. Pore fabrication of nano-ZSM-5 zeolite by internal desilication and its influence on the methanol to hydrocarbon reaction[J]. Fuel Process. Technol., 2017,155:191-199. doi: 10.1016/j.fuproc.2016.05.046
13. [13]
  Groen J C, Moulijn J A, Pérez-Ramírez J. Desilication: On the controlled generation of mesoporosity in MFI zeolites[J]. J. Mater. Chem., 2006,16(22):2121-2131. doi: 10.1039/B517510K
14. [14]
  Groen J C, Jansen J C, Moulijn J A, Pérez-Ramírez J. Optimal aluminum-assisted mesoporosity development in MFI zeolites by desilication[J]. J. Phys. Chem. B, 2004,108(35):13062-13065. doi: 10.1021/jp047194f
15. [15]
  Kalantari N, F Bekheet M, Nezhad P D F, Back J O, Farzi A, Penner S, Delibaş N, Schwarz S, Bernardi J, Salari D, Niaei A. Effect of chromium and boron incorporation methods on structural and catalytic properties of hierarchical ZSM-5 in the methanol-to-propylene process[J]. J. Ind. Eng. Chem., 2022,111:168-182. doi: 10.1016/j.jiec.2022.03.049
16. [16]
  Westgård Erichsen M, Svelle S, Olsbye U. The influence of catalyst acid strength on the methanol to hydrocarbons (MTH) reaction[J]. Catal. Today, 2013,215:216-223. doi: 10.1016/j.cattod.2013.03.017
17. [17]
  Zhang L, Tu R, Ren G Q, Li Z, Zhai S L, Xu Y C, Yu T. Manipulate the acidity of gallium doped silicalite-1 to optimize methanol to propene performance[J]. Chem. Eng. J., 2023,458141447. doi: 10.1016/j.cej.2023.141447
18. [18]
  Yarulina I, Bailleul S, Pustovarenko A, Martinez J R, Wispelaere K D, Hajek J, Weckhuysen B M, Houben K, Baldus M, Van Speybroeck V, Kapteijn F, Gascon J. Suppression of the aromatic cycle in methanol-to-olefins reaction over ZSM-5 by post-synthetic modification using calcium[J]. ChemCatChem, 2016,8(19):3057-3063. doi: 10.1002/cctc.201600650
19. [19]
  Groen J C, Peffer L A A, Moulijn J A, Pérez-Ramírez J. Mesoporosity development in ZSM-5 zeolite upon optimized desilication conditions in alkaline medium[J]. Colloid Surf. A-Physicochem. Eng. Asp., 2004,241(1):53-58.
20. [20]
  Janssens T V W. A new approach to the modeling of deactivation in the conversion of methanol on zeolite catalysts[J]. J. Catal., 2009,264(2):130-137. doi: 10.1016/j.jcat.2009.03.004
21. [21]
  Lee S, Choi M. Unveiling coke formation mechanism in MFI zeolites during methanol-to-hydrocarbons conversion[J]. J. Catal., 2019,375:183-192. doi: 10.1016/j.jcat.2019.05.030
22. [22]
  Armaroli T, Simon L J, Digne M, Montanari T, Bevilacqua M, Valtchev V, Patarin J, Busca G. Effects of crystal size and Si/Al ratio on the surface properties of H-ZSM-5 zeolites[J]. Appl. Catal. A-Gen., 2006,306:78-84. doi: 10.1016/j.apcata.2006.03.030
23. [23]
  Mozgawa W. The relation between structure and vibrational spectra of natural zeolites[J]. J. Mol. Struct., 2001,596(1):129-137.
24. [24]
  Mambrim J S T, Pastore H O, Davanzo C U, Vichi E J S, Nakamura O, Vargas H. Synthesis and characterization of chromium silicalite[J]. Chem. Mater., 1993,5(2):66-173.
25. [25]
  Svelle S, Sommer L, Barbera K, Vennestrøm P N R, Olsbye U, Lillerud K P, Bordiga S, Pan Y H, Beato P. How defects and crystal morphology control the effects of desilication[J]. Catal. Today, 2011,168(1):38-47. doi: 10.1016/j.cattod.2010.12.013
26. [26]
  Groen J C, Peffer L A A, Pérez-Ramı́rez J. Pore size determination in modified micro- and mesoporous materials[J]. Pitfalls and limitations in gas adsorption data analysis. Microporous Mesoporous Mat., 2003,60(1):1-17.
27. [27]
  Zhang R Z, Zhao P R, Han L N, Wang J C, Zhao L F. Seed-assisted template-free synthesis of nano-sized ZSM-5 via two-stage crystallization with related investigation of mechanism[J]. Microporous Mesoporous Mat., 2021,312110754. doi: 10.1016/j.micromeso.2020.110754
28. [28]
  Pan M, Jiang X B, Pang Y H, Pan X F, Zhang Q H, Yang R C, Zheng J J. One-step synthesis of hierarchical ZSM-5 zeolites with low defect density as long-lived MTH catalysts[J]. Appl. Catal. A-Gen., 2023,656:119132-119140. doi: 10.1016/j.apcata.2023.119132
29. [29]
  Verboekend D, Pérez-Ramírez J. Design of hierarchical zeolite catalysts by desilication[J]. Catal. Sci. Technol., 2011,1(6):879-890. doi: 10.1039/c1cy00150g
30. [30]
  Palčić A, Moldovan S, El Siblani H, Vicente A, Valtchev V. Defect sites in zeolites: Origin and healing[J]. Adv. Sci., 2022,9(4)2104414. doi: 10.1002/advs.202104414
31. [31]
  Liu Y H, Zhang Q, Li J Y, Wang X X, Terasaki O, Xu J, Yu J H. Protozeolite-seeded synthesis of single-crystalline hierarchical zeolites with facet-shaped mesopores and their catalytic application in methanol-to-propylene conversion[J]. Angew. Chem. Int. Ed., 2022,61(34)e202205716. doi: 10.1002/anie.202205716
32. [32]
  Kim J, Choi M, Ryoo R. Effect of mesoporosity against the deactivation of MFI zeolite catalyst during the methanol-to-hydrocarbon conversion process[J]. J. Catal., 2010,269(1):219-228. doi: 10.1016/j.jcat.2009.11.009
1. [1]
  Siyu HOU , Weiyao LI , Jiadong LIU , Fei WANG , Wensi LIU , Jing YANG , Ying ZHANG . Preparation and catalytic performance of magnetic nano iron oxide by oxidation co-precipitation method. Chinese Journal of Inorganic Chemistry, 2024, 40(8): 1577-1582. doi: 10.11862/CJIC.20230469
2. [2]
  Min WANG , Dehua XIN , Yaning SHI , Wenyao ZHU , Yuanqun ZHANG , Wei ZHANG . Construction and full-spectrum catalytic performance of multilevel Ag/Bi/nitrogen vacancy g-C₃N₄/Ti₃C₂T_x Schottky junction. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1123-1134. doi: 10.11862/CJIC.20230477
3. [3]
  Yongmei Liu , Lisen Sun , Zhen Huang , Tao Tu . Curriculum-Based Ideological and Political Design for the Experiment of Methanol Oxidation to Formaldehyde Catalyzed by Electrolytic Silver. University Chemistry, 2024, 39(2): 67-71. doi: 10.3866/PKU.DXHX202308020
4. [4]
  Qingqing SHEN , Xiangbowen DU , Kaicheng QIAN , Zhikang JIN , Zheng FANG , Tong WEI , Renhong LI . Self-supporting Cu/α-FeOOH/foam nickel composite catalyst for efficient hydrogen production by coupling methanol oxidation and water electrolysis. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1953-1964. doi: 10.11862/CJIC.20240028
5. [5]
  Kai CHEN , Fengshun WU , Shun XIAO , Jinbao ZHANG , Lihua ZHU . PtRu/nitrogen-doped carbon for electrocatalytic methanol oxidation and hydrogen evolution by water electrolysis. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1357-1367. doi: 10.11862/CJIC.20230350
6. [6]
  Juan WANG , Zhongqiu WANG , Qin SHANG , Guohong WANG , Jinmao LI . NiS and Pt as dual co-catalysts for the enhanced photocatalytic H₂ production activity of BaTiO₃ nanofibers. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1719-1730. doi: 10.11862/CJIC.20240102
7. [7]
  Zhiwen HU , Weixia DONG , Qifu BAO , Ping LI . Low-temperature synthesis of tetragonal BaTiO₃ for piezocatalysis. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 857-866. doi: 10.11862/CJIC.20230462
8. [8]
  Guimin ZHANG , Wenjuan MA , Wenqiang DING , Zhengyi FU . Synthesis and catalytic properties of hollow AgPd bimetallic nanospheres. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 963-971. doi: 10.11862/CJIC.20230293
9. [9]
  Zhuo WANG , Junshan ZHANG , Shaoyan YANG , Lingyan ZHOU , Yedi LI , Yuanpei LAN . Preparation and photocatalytic performance of CeO₂-reduced graphene oxide by thermal decomposition. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1708-1718. doi: 10.11862/CJIC.20240067
10. [10]
  Ping ZHANG , Chenchen ZHAO , Xiaoyun CUI , Bing XIE , Yihan LIU , Haiyu LIN , Jiale ZHANG , Yu'nan CHEN . Preparation and adsorption-photocatalytic performance of ZnAl@layered double oxides. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1965-1974. doi: 10.11862/CJIC.20240014
11. [11]
  Zijian Jiang , Yuang Liu , Yijian Zong , Yong Fan , Wanchun Zhu , Yupeng Guo . Preparation of Nano Zinc Oxide by Microemulsion Method and Study on Its Photocatalytic Activity. University Chemistry, 2024, 39(5): 266-273. doi: 10.3866/PKU.DXHX202311101
12. [12]
  Chuanming GUO , Kaiyang ZHANG , Yun WU , Rui YAO , Qiang ZHAO , Jinping LI , Guang LIU . Performance of MnO₂-0.39IrO_x composite oxides for water oxidation reaction in acidic media. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1135-1142. doi: 10.11862/CJIC.20230459
13. [13]
  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
14. [14]
  Wen YANG , Didi WANG , Ziyi HUANG , Yaping ZHOU , Yanyan FENG . La promoted hydrotalcite derived Ni-based catalysts: In situ preparation and CO₂ methanation performance. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 561-570. doi: 10.11862/CJIC.20230276
15. [15]
  Haiyuan Wang , Yiming Tang , Haoran Guo , Guohui Chen , Yajing Sun , Chao Zhao , Zhen Zhang . Comprehensive Chemistry Experimental Teaching Design Based on the Integration of Science and Education: Preparation and Catalytic Properties of Silver Nanomaterials. University Chemistry, 2024, 39(10): 219-228. doi: 10.12461/PKU.DXHX202404067
16. [16]
  Qiangqiang SUN , Pengcheng ZHAO , Ruoyu WU , Baoyue CAO . Multistage microporous bifunctional catalyst constructed by P-doped nickel-based sulfide ultra-thin nanosheets for energy-efficient hydrogen production from water electrolysis. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1151-1161. doi: 10.11862/CJIC.20230454
17. [17]
  Yufang GAO , Nan HOU , Yaning LIANG , Ning LI , Yanting ZHANG , Zelong LI , Xiaofeng LI . Nano-thin layer MCM-22 zeolite: Synthesis and catalytic properties of trimethylbenzene isomerization reaction. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1079-1087. doi: 10.11862/CJIC.20240036
18. [18]
  Xin Zhou , Zhi Zhang , Yun Yang , Shuijin Yang . A Study on the Enhancement of Photocatalytic Performance in C/Bi/Bi₂MoO₆ Composites by Ferroelectric Polarization: A Recommended Comprehensive Chemical Experiment. University Chemistry, 2024, 39(4): 296-304. doi: 10.3866/PKU.DXHX202310008
19. [19]
  Haihua Yang , Minjie Zhou , Binhong He , Wenyuan Xu , Bing Chen , Enxiang Liang . Synthesis and Electrocatalytic Performance of Iron Phosphide@Carbon Nanotubes as Cathode Material for Zinc-Air Battery: a Comprehensive Undergraduate Chemical Experiment. University Chemistry, 2024, 39(10): 426-432. doi: 10.12461/PKU.DXHX202405100
20. [20]
  Bing LIU , Huang ZHANG , Hongliang HAN , Changwen HU , Yinglei ZHANG . Visible light degradation of methylene blue from water by triangle Au@TiO₂ mesoporous catalyst. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 941-952. doi: 10.11862/CJIC.20230398

Get Citation

PDF

XML

Metrics

PDF Downloads(3)
Abstract views(336)
HTML views(34)

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