Citation: Pei Li, Yuenan Zheng, Zhankai Liu, An-Hui Lu. Boron-Containing MFI Zeolite: Microstructure Control and Its Performance of Propane Oxidative Dehydrogenation[J]. Acta Physico-Chimica Sinica, ;2025, 41(4): 240601. doi: 10.3866/PKU.WHXB202406012 shu

Boron-Containing MFI Zeolite: Microstructure Control and Its Performance of Propane Oxidative Dehydrogenation

State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Liaoning Key Laboratory for Catalytic Conversion of Carbon Resources, Dalian University of Technology, Dalian 116024, Liaoning Province, China

Corresponding author: An-Hui Lu, anhuilu@dlut.edu.cn
Received Date: 12 June 2024
Revised Date: 10 July 2024
Accepted Date: 29 July 2024

Fund Project: the State Key Program of National Natural Science Foundation of China 21733002National Key Research and Development Project 2021YFA1500301National Science Foundation for Young Scientists of China 22302030China Postdoctoral Science Foundation 2023M730467

Boron-containing zeolites can catalyze the oxidative dehydrogenation of propane (ODHP) to produce propylene. Enhancing the quantity of active boron-oxygen species and regulating the positioning of these species within the zeolite are the main challenges in developing efficient boron-based catalysts. In this study, a boron-containing zeolite catalyst with exposed (010) crystal facets, referred to as the MFI-type boron-containing zeolite (BMFI), was synthesized using a urea-assisted hydrothermal method. The research indicates that the addition of an appropriate amount of urea can regulate the morphology of the zeolite, with its short-axis flake-like structure enhancing the accessibility of active boron sites and anchoring a higher content of active boron-oxygen species through hydrogen bonding, which significantly improves the ODHP activity and olefin selectivity of the catalyst. The propane conversion rate reached 20%, with a propylene selectivity of 62.3% and a total olefin selectivity of 81.3% at 520 ℃. Compared to the ellipsoidal boron-containing catalyst formed without urea, the flake-like BMFI catalyst exhibited nearly a 20-fold increase in the reaction rate of propane. The flake-like BMFI possesses a greater number of framework tetrahedrally coordinated boron (B[4]) and defective boron species (B[3]^a and B[3]^b), and active boron structural evolution occurred during the reaction process, with B[3]^a and B[3]^b being the active sites for the catalytic reaction. This study provides a reference for the structural design and regulation of boron-based catalysts for the oxidative dehydrogenation of light alkanes.
- Alkane dehydrogenation,
- Oxidative dehydrogenation of propane,
- Boron-based catalyst,
- Zeolite,
- Urea,
- Morphology regulation
1. [1]
  Sattler, J. J. H. B.; Ruiz-Martinez, J.; Santillan-Jimenez, E.; Weckhuysen, B. M. Chem. Rev. 2014, 114 (20), 10613. doi: 10.1021/cr5002436 doi: 10.1021/cr5002436
2. [2]
  Phung, T. K.; Pham, T. L. M.; Vu, K. B.; Busca, G. J. Environ. Chem. Eng 2021, 9 (4), 105673. doi: 10.1016/j.jece.2021.105673 doi: 10.1016/j.jece.2021.105673
3. [3]
  Shen, S. S.; Liu, X. L.; Guo, Y.; Wang, Y. Q. Acta Phys. -Chim. Sin. 2023, 39 (7), 85. doi: 10.3866/PKU.WHXB202209043 doi: 10.3866/PKU.WHXB202209043
4. [4]
  Carter, J. H.; Bere, T.; Pitchers, J. R.; Hewes, D. G.; Vandegehuchte, B. D.; Kiely, C. J.; Taylor, S. H.; Hutchings, G. J. Green Chem. 2021, 23 (24), 9747. doi: 10.1039/d1gc03700e doi: 10.1039/d1gc03700e
5. [5]
  Zhang, T. Acta Phys. -Chim. Sin. 2022, 38 (8), 12. doi: 10.3866/PKU.WHXB202012009 doi: 10.3866/PKU.WHXB202012009
6. [6]
  Grant, J. T.; Carrero, C. A.; Goeltl, F.; Venegas, J.; Mueller, P.; Burt, S. P.; Specht, S. E.; McDermott, W. P.; Chieregato, A.; Hermans, I. Science 2016 354 (6319), 1570. doi: 10.1126/science.aaf7885 doi: 10.1126/science.aaf7885
7. [7]
  Shi, L.; Wang, D.; Song, W.; Shao, D.; Zhang, W. P.; Lu, A. H. ChemCatChem 2017, 9 (10), 1788. doi: 10.1002/cctc.201700004 doi: 10.1002/cctc.201700004
8. [8]
  Gao, X.; Liu, M.; Huang, Y.; Xu, W.; Zhou, X.; Yao, S. ACS Catal. 2023, 13 (14), 9667. doi: 10.1021/acscatal.3c00728 doi: 10.1021/acscatal.3c00728
9. [9]
  Yan, H.; Alayoglu, S.; Wu, W.; Zhang, Y.; Weitz, E.; Stair, P. C.; Notestein, J. M. ACS Catal. 2021, 11 (15), 9370. doi: 10.1021/acscatal.1c02168 doi: 10.1021/acscatal.1c02168
10. [10]
  Tian, J.; Li, J.; Qian, S.; Zhang, Z.; Wan, S.; Wang, S.; Lin, J.; Wang, Y. Appl. Catal. A-Gen. 2021, 623, 118271. doi: 10.1016/j.apcata.2021.118271 doi: 10.1016/j.apcata.2021.118271
11. [11]
  Grant, J. T.; McDermott, W. P.; Venegas, J. M.; Burt, S. P.; Micka, J.; Phivilay, S. P.; Carrero, C. A.; Hermans, I. ChemCatChem 2017, 9 (19), 3623. doi: 10.1002/cctc.201701140 doi: 10.1002/cctc.201701140
12. [12]
  Lu, W. -D.; Qiu, B.; Liu, Z. -K.; Wu, F.; Lu, A. -H. Catal 2023, 13 (6), 1696. doi: 10.1039/d2cy02098j doi: 10.1039/d2cy02098j
13. [13]
  Xu, B. Acta Phys. -Chim. Sin. 2023, 39 (1), 7. doi: 10.3866/PKU.WHXB202012030 doi: 10.3866/PKU.WHXB202012030
14. [14]
  Gao, X.; Zhu, L.; Yang, F.; Zhang, L.; Xu, W.; Zhou, X.; Huang, Y.; Song, H.; Lin, L.; Wen, X.; et al. Nat. Commun. 2023, 14 (1), 1478. doi: 10.1038/s41467-023-37261-x doi: 10.1038/s41467-023-37261-x
15. [15]
  Gao, B.; Qiu, B.; Zheng, M.; Liu, Z.; Lu, W. -D.; Wang, Q.; Xu, J.; Deng, F.; Lu, A. -H. ACS Catal. 2022, 12 (12), 7368. doi: 10.1021/acscatal.2c01622 doi: 10.1021/acscatal.2c01622
16. [16]
  Qian, H.; Sun, F.; Zhang, W.; Huang, C.; Wang, Y.; Fang, K. Catal 2022, 12 (6), 1996. doi: 10.1039/d1cy01792f doi: 10.1039/d1cy01792f
17. [17]
  Zhou, H.; Yi, X. Y.; Hui, Y.; Wang, L.; Chen, W.; Qin, Y. C.; Wang, M.; Ma, J. B.; Chu, X. F.; Wang, Y. Q.; et al. Science 2021, 372 (6537), 76. doi: 10.1126/science.abe7935 doi: 10.1126/science.abe7935
18. [18]
  Qiu, B.; Lu, W. -D.; Gao, X. -Q.; Sheng, J.; Yan, B.; Ji, M.; Lu, A. -H. J. Catal. 2022, 408, 133. doi: 10.1016/j.jcat.2022.02.017 doi: 10.1016/j.jcat.2022.02.017
19. [19]
  Shan, Z.; Wang, H.; Meng, X.; Liu, S.; Wang, L.; Wang, C.; Li, F.; Lewis, J. P.; Xiao, F. -S. Chem. Commun. 2011, 47 (3), 1048. doi: 10.1039/c0cc03613g doi: 10.1039/c0cc03613g
20. [20]
  Ping, C.; Zhu, Q.; Ma, W.; Hu, C.; Zhang, Y. J. Porous Mater. 2022, 29 (6), 1919. doi: 10.1007/s10934-022-01303-4 doi: 10.1007/s10934-022-01303-4
21. [21]
  Li, W.; Qiu, M.; Li, W.; Ge, L.; Zhang, K.; Chen, X. Sustain. Energy Fuels 2022, 6 (10), 2462. doi: 10.1039/d2se00365a doi: 10.1039/d2se00365a
22. [22]
  Zhu, J.; Yan, S.; Xu, G.; Zhu, X.; Yang, F. J. Solid State Chem. 2023, 318, 123772. doi: 10.1016/j.jssc.2022.123772 doi: 10.1016/j.jssc.2022.123772
23. [23]
  Zhou, Z.; Jiang, R.; Chen, X.; Wang, X.; Hou, H. J. Solid State Chem. 2021, 298, 122132. doi: 10.1016/j.jssc.2021.122132 doi: 10.1016/j.jssc.2021.122132
24. [24]
  Roberto Millini, G. P. a. G. B. Top. Catal. 1999, 9 (1-2), 13. doi: 10.1023/A:1019198119365 doi: 10.1023/A:1019198119365
25. [25]
  Sayed, M. B.; Auroux, A.; Vedrine, J. C. J. Catal. 1989, 116 (1), 1. doi: 10.1016/0021-9517(89)90070-5 doi: 10.1016/0021-9517(89)90070-5
26. [26]
  Yue, Q.; Liu, C.; Zhao, H.; Liu, H.; Ruterana, P.; Zhao, J.; Qin, Z.; Mintova, S. Nano Res. 2023, 16 (10), 12196. doi: 10.1007/s12274-023-5749-0 doi: 10.1007/s12274-023-5749-0
27. [27]
  Tian, H.; He, H.; Gao, P.; Guo, X.; Tang, X.; Chang, Y.; Zha, F.; Chen, H. Appl. Surf. Sci. 2023, 608, 155158. doi: 10.1016/j.apsusc.2022.155158 doi: 10.1016/j.apsusc.2022.155158
28. [28]
  Qiu, B.; Lu, W. -D.; Gao, X. -Q.; Sheng, J.; Ji, M.; Wang, D.; Lu, A. -H. J. Catal. 2023, 417, 14. doi: 10.1016/j.jcat.2022.11.031 doi: 10.1016/j.jcat.2022.11.031
29. [29]
  Dorn, R. W.; Cendejas, M. C.; Chen, K.; Hung, I.; Altvater, N. R.; McDermott, W. P.; Gan, Z.; Hermans, I.; Rossini, A. J. ACS Catal. 2020, 10 (23), 13852. doi: 10.1021/acscatal.0c03762 doi: 10.1021/acscatal.0c03762
30. [30]
  Altvater, N. R.; Dorn, R. W.; Cendejas, M. C.; McDermott, W. P.; Thomas, B.; Rossini, A. J.; Hermans, I. Angew. Chem. Int. Ed. 2020, 59 (16), 6546. doi: 10.1002/anie.201914696 doi: 10.1002/anie.201914696
31. [31]
  Tian, H.; Li, W.; He, L.; Zhong, Y.; Xu, S.; Xiao, H.; Xu, B. Nat. Commun. 2023, 14 (1), 6520. doi: 10.1038/s41467-023-42403-2 doi: 10.1038/s41467-023-42403-2
32. [32]
  Lu, W. -D.; Wang, D.; Zhao, Z.; Song, W.; Li, W. -C.; Lu, A. -H. ACS Catal. 2019, 9 (9), 8263. doi: 10.1021/acscatal.9b02284 doi: 10.1021/acscatal.9b02284
33. [33]
  Coudurier, G.; Vedrine, J. C. Pure Appl. Chem. 1986, 58 (10), 1389. doi: 10.1351/pac198658101389 doi: 10.1351/pac198658101389
1. [1]
  Jiahui YU , Jixian DONG , Yutong ZHAO , Fuping ZHAO , Bo GE , Xipeng PU , Dafeng ZHANG . The morphology control and full-spectrum photodegradation tetracycline performance of microwave-hydrothermal synthesized BiVO₄:Yb³⁺,Er³⁺ photocatalyst. Journal of Fuel Chemistry and Technology, 2025, 53(3): 348-359. doi: 10.1016/S1872-5813(24)60514-1
2. [2]
  Jiatong Hu , Qiyi Wang , Ruiwen Tang , Jiajing Feng . Photocatalytic Journey of Perylene Diimides in a Competitive Arena. University Chemistry, 2025, 40(5): 328-333. doi: 10.12461/PKU.DXHX202407015
3. [3]
  Qin ZHU , Jiao MA , Zhihui QIAN , Yuxu LUO , Yujiao GUO , Mingwu XIANG , Xiaofang LIU , Ping NING , Junming GUO . Morphological evolution and electrochemical properties of cathode material LiAl_0.08Mn_1.92O₄ single crystal particles. Chinese Journal of Inorganic Chemistry, 2024, 40(8): 1549-1562. doi: 10.11862/CJIC.20240022
4. [4]
  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. Acta Physico-Chimica Sinica, 2024, 40(9): 2308019-0. doi: 10.3866/PKU.WHXB202308019
5. [5]
  Qing Li , Guangxun Zhang , Yuxia Xu , Yangyang Sun , Huan Pang . P-Regulated Hierarchical Structure Ni₂P Assemblies toward Efficient Electrochemical Urea Oxidation. Acta Physico-Chimica Sinica, 2024, 40(9): 2308045-0. doi: 10.3866/PKU.WHXB202308045
6. [6]
  Xuejie Wang , Guoqing Cui , Congkai Wang , Yang Yang , Guiyuan Jiang , Chunming Xu . Research Progress on Carbon-based Catalysts for Catalytic Dehydrogenation of Liquid Organic Hydrogen Carriers. Acta Physico-Chimica Sinica, 2025, 41(5): 100044-0. doi: 10.1016/j.actphy.2024.100044
7. [7]
  Yuhao SUN , Qingzhe DONG , Lei ZHAO , Xiaodan JIANG , Hailing GUO , Xianglong MENG , Yongmei GUO . Synthesis and antibacterial properties of silver-loaded sod-based zeolite. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 761-770. doi: 10.11862/CJIC.20230169
8. [8]
  Lele Feng , Xueying Bai , Jifeng Pang , Hongchen Cao , Xiaoyan Liu , Wenhao Luo , Xiaofeng Yang , Pengfei Wu , Mingyuan Zheng . Single-atom Pd boosted Cu catalysts for ethanol dehydrogenation. Acta Physico-Chimica Sinica, 2025, 41(9): 100100-0. doi: 10.1016/j.actphy.2025.100100
9. [9]
  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
10. [10]
  Mingjie Lei , Wenting Hu , Kexin Lin , Xiujuan Sun , Haoshen Zhang , Ye Qian , Tongyue Kang , Xiulin Wu , Hailong Liao , Yuan Pan , Yuwei Zhang , Diye Wei , Ping Gao . Accelerating the reconstruction of NiSe₂ by Co/Mn/Mo doping for enhanced urea electrolysis. Acta Physico-Chimica Sinica, 2025, 41(8): 100083-0. doi: 10.1016/j.actphy.2025.100083
11. [11]
  Wenjuan Tan , Yong Ye , Xiujuan Sun , Bei Liu , Jiajia Zhou , Hailong Liao , Xiulin Wu , Rui Ding , Enhui Liu , Ping Gao . Building P-Poor Ni₂P and P-Rich CoP₃ Heterojunction Structure with Cation Vacancy for Enhanced Electrocatalytic Hydrazine and Urea Oxidation. Acta Physico-Chimica Sinica, 2024, 40(6): 2306054-0. doi: 10.3866/PKU.WHXB202306054
12. [12]
  Bing WEI , Jianfan ZHANG , Zhe CHEN . Research progress in fine tuning of bimetallic nanocatalysts for electrocatalytic carbon dioxide reduction. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 425-439. doi: 10.11862/CJIC.20240201
13. [13]
  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
14. [14]
  Yiping HUANG , Liqin TANG , Yufan JI , Cheng CHEN , Shuangtao LI , Jingjing HUANG , Xuechao GAO , Xuehong GU . Hollow fiber NaA zeolite membrane for deep dehydration of ethanol solvent by vapor permeation. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 225-234. doi: 10.11862/CJIC.20240224
15. [15]
  Zhiquan Zhang , Baker Rhimi , Zheyang Liu , Min Zhou , Guowei Deng , Wei Wei , Liang Mao , Huaming Li , Zhifeng Jiang . Insights into the Development of Copper-Based Photocatalysts for CO₂ Conversion. Acta Physico-Chimica Sinica, 2024, 40(12): 2406029-0. doi: 10.3866/PKU.WHXB202406029
16. [16]
  Shanghua Li , Malin Li , Xiwen Chi , Xin Yin , Zhaodi Luo , Jihong Yu . High-Stable Aqueous Zinc Metal Anodes Enabled by an Oriented ZnQ Zeolite Protective Layer with Facile Ion Migration Kinetics. Acta Physico-Chimica Sinica, 2025, 41(1): 100003-0. doi: 10.3866/PKU.WHXB202309003
17. [17]
  Hao GUO , Tong WEI , Qingqing SHEN , Anqi HONG , Zeting DENG , Zheng FANG , Jichao SHI , Renhong LI . Electrocatalytic decoupling of urea solution for hydrogen production by nickel foam-supported Co₉S₈/Ni₃S₂ heterojunction. Chinese Journal of Inorganic Chemistry, 2024, 40(11): 2141-2154. doi: 10.11862/CJIC.20240085
18. [18]
  Hanxue LIU , Shijie LI , Meng REN , Xuling XUE , Hongke LIU . Design and antitumor properties of dehydroabietic acid functionalized cyclometalated iridium(Ⅲ) complex. Chinese Journal of Inorganic Chemistry, 2025, 41(8): 1483-1494. doi: 10.11862/CJIC.20250031
19. [19]
  .
  CCS Chemistry | 超分子活化底物为自由基促进高效选择性光催化氧化
  . CCS Chemistry, 2025, 7(10.31635/ccschem.025.202405229): -.
20. [20]
  Zhanggui DUAN , Yi PEI , Shanshan ZHENG , Zhaoyang WANG , Yongguang WANG , Junjie WANG , Yang HU , Chunxin LÜ , Wei ZHONG . Preparation of UiO-66-NH₂ supported copper catalyst and its catalytic activity on alcohol oxidation. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 496-506. doi: 10.11862/CJIC.20230317

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(716)
HTML views(56)

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