Citation: Shanshan Shen, Xiaohui Liu, Yong Guo, Yanqin Wang. Performance Enhancement of Pt/Silicalite-1 by in situ Doped Fe for Propane Dehydrogenation[J]. Acta Physico-Chimica Sinica, ;2023, 39(7): 220904. doi: 10.3866/PKU.WHXB202209043 shu

Performance Enhancement of Pt/Silicalite-1 by in situ Doped Fe for Propane Dehydrogenation

Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China

Corresponding author: Yanqin Wang, wangyanqin@ecust.edu.cn
Received Date: 29 September 2022
Revised Date: 21 November 2022
Accepted Date: 21 November 2022
Available Online: 24 November 2022
Fund Project: the National Natural Science Foundation of China 21832002

As one of the most common bulk chemicals, propylene is widely used in industrial production. Given developments in shale gas exploration technology, propane direct dehydrogenation (PDH) has emerged as a potential route. Pt-based catalysts are considered highly active catalysts for PDH, but their use is limited by a number of challenges. Herein, in situ Fe-doped Silicalite-1 zeolite supports were synthesized using the hydrothermal method, after which the corresponding Pt-based catalysts were prepared by impregnation and used for PDH. For comparison, Pt/Silicalite-1 and co-impregnated Pt1Fe2/Silicalite-1 catalysts were also prepared. Compared with that of Pt/Silicalite-1, the catalytic performance of Pt/Fe-Silicalite-1 prepared by in situ Fe-doping was significantly enhanced, whereas that of the co-precipitated Pt1Fe2/Silicalite-1 catalyst decreased. The selectivity and catalytic stability of the reaction over the Pt/Fe-Silicalite-1 catalyst were greatly improved, although the initial conversion of propane was slightly low. After 8 h, the propane conversion rate stabilized at 43.7% and the propylene selectivity reached 98.0%. More importantly, the catalyst maintained its performance over 80 h without an obvious decline. Propane conversion increased with increasing reaction temperature, while propene selectivity was maintained at a comparable level. The reaction kinetics of PDH were determined, and the results demonstrated that the apparent activation energy of the Pt/Fe-Silicalite-1 catalyst was 97.0 kJ·mol⁻¹; this value was the lowest obtained among the catalysts investigated and indicated the relative ease of propane activation over the catalyst. A series of characterization techniques, such as X-ray diffraction (XRD), N₂ sorption, scanning electron microscopy (SEM), and transmission electron microscopy (TEM), were used to explore the structural characteristics of the catalysts. The in situ Fe-doped Silicalite-1 zeolite supports retained their MFI structure but had a small particle size. UV-Vis spectroscopy revealed a large amount of Fe₂O₃ particles on the Pt1Fe2/Silicalite-1 surface; by contrast, Pt/Fe-Silicalite-1 possessed isolated tetrahedrally and octahedrally coordinated Fe³⁺ in the Fe-Silicalite-1 framework, as well as small oligomeric Fe species, such as Fe_xO_y, inside the zeolite pores. H₂-TPR revealed strong interactions between the Fe species and support in the Pt/Fe-Silicalite-1 catalyst. CO-DRIFT and X-ray photoelectron spectroscopy (XPS) indicated that the in situ incorporation of Fe not only improved the formation of Pt on the platform sites with high saturation, which prevented the deep-cracking of propane, but also enriched the electron cloud density on Pt by promoting electron transfer from Fe to Pt, thus enhancing the desorption of propylene and preventing coke formation. In addition, Fe sites in the support could anchor Pt to prevent their aggregation and improve the stability of Pt/Fe-Silicalite-1. Thus, high conversion and selectivity were obtained even after 80 h of reaction.
- Propane dehydrogenation,
- Silicalite-1,
- Pt-based catalyst,
- In situ doped Fe
1. [1]
  Bhasin, M. M.; McCain, J. H.; Vora, B. V.; Imai, T.; Pujadó, P. R. Appl. Catal. A 2001, 221, 397. doi: 10.1016/S0926-860X(01)00816-X doi: 10.1016/S0926-860X(01)00816-X
2. [2]
  Atanga, M. A.; Rezaei, F.; Jawad, A.; Fitch, M.; Rownaghi, A. A. Appl. Catal. B 2018, 220, 429. doi: 10.1016/j.apcatb.2017.08.052 doi: 10.1016/j.apcatb.2017.08.052
3. [3]
  Qi, W.; Yan, P.; Su, D. S. Acc. Chem. Res. 2018, 51, 640. doi: 10.1021/acs.accounts.7b00475 doi: 10.1021/acs.accounts.7b00475
4. [4]
  Zhao, Z.; Ge, G.; Li, W.; Guo, X.; Wang, G. Chin. J. Chem. 2016, 37, 644. doi: 10.1016/S1872-2067(15)61065-8 doi: 10.1016/S1872-2067(15)61065-8
5. [5]
  Hu, Z. -P.; Yang, D.; Wang, Z.; Yuan, Z. -Y. Chin. J. Chem. 2019, 40, 1233. doi: 10.1016/S1872-2067(19)63360-7 doi: 10.1016/S1872-2067(19)63360-7
6. [6]
  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, 9747. doi: 10.1039/D1GC03700E doi: 10.1039/D1GC03700E
7. [7]
  Shan, Y. -L.; Zhu, Y. -A.; Sui, Z. -J.; Chen, D.; Zhou, X. -G. Catal. Sci. Technol. 2015, 5, 3991. doi: 10.1039/C5CY00230C doi: 10.1039/C5CY00230C
8. [8]
  Zhu, J.; Yang, M. -L.; Yu, Y.; Zhu, Y. -A.; Sui, Z. -J.; Zhou, X. -G.; Holmen, A.; Chen, D. ACS Catal. 2015, 5, 6310. doi: 10.1021/acscatal.5b01423 doi: 10.1021/acscatal.5b01423
9. [9]
  Jiang, F.; Zeng, L.; Li, S.; Liu, G.; Wang, S.; Gong, J. ACS Catal. 2015, 5, 438. doi: 10.1021/cs501279v doi: 10.1021/cs501279v
10. [10]
  Zhao, T.; Shen, S.; Liu, X.; Guo, Y.; Pao, C. -W.; Chen, J. -L.; Wang, Y. Catal. Sci. Technol. 2019, 9, 4451. doi: 10.1039/C9CY90066G doi: 10.1039/C9CY90066G
11. [11]
  Searles, K.; Chan, K. W.; Mendes Burak, J. A.; Zemlyanov, D.; Safonova, O.; Copéret, C. J. Am. Chem. Soc. 2018, 140, 11674. doi: 10.1021/jacs.8b05378 doi: 10.1021/jacs.8b05378
12. [12]
  Shi, L.; Deng, G. -M.; Li, W. -C.; Miao, S.; Wang, Q. -N.; Zhang, W. -P.; Lu, A. -H. Angew. Chem., Int. Ed. 2015, 54, 13994. doi: 10.1002/anie.201507119 doi: 10.1002/anie.201507119
13. [13]
  Sattler, J. J. H. B.; Gonzalez-Jimenez, I. D.; Luo, L.; Stears, B. A.; Malek, A.; Barton, D. G.; Kilos, B. A.; Kaminsky, M. P.; Verhoeven, T. W. G. M.; Koers, E. J.; et al. Angew. Chem. Int. Ed. 2014, 53, 9251. doi: 10.1002/anie.201404460 doi: 10.1002/anie.201404460
14. [14]
  Sokolov, S.; Stoyanova, M.; Rodemerck, U.; Linke, D.; Kondratenko, E. V. J. Catal. 2012, 293, 67. doi: 10.1016/j.jcat.2012.06.005 doi: 10.1016/j.jcat.2012.06.005
15. [15]
  Cesar, L. G.; Yang, C.; Lu, Z.; Ren, Y.; Zhang, G.; Miller, J. T. ACS Catal. 2019, 9, 5231. doi: 10.1021/acscatal.9b00549 doi: 10.1021/acscatal.9b00549
16. [16]
  Zhang, B.; Zheng, L.; Zhai, Z.; Li, G.; Liu, G. ACS Appl. Mater. Interfaces 2021, 13, 16259. doi: 10.1021/acsami.0c22865 doi: 10.1021/acsami.0c22865
17. [17]
  Liu, X.; Wang, X.; Zhen, S.; Sun, G.; Pei, C.; Zhao, Z. -J.; Gong, J. Chem. Sci. 2022, 13, 9537. doi: 10.1039/D2SC03723H doi: 10.1039/D2SC03723H
18. [18]
  Ye, C.; Peng, M.; Wang, Y.; Zhang, N.; Wang, D.; Jiao, M.; Miller, J. T. ACS Appl. Mater. Interfaces 2020, 12, 25903. doi: 10.1021/acsami.0c05043 doi: 10.1021/acsami.0c05043
19. [19]
  Iglesias-Juez, A.; Beale, A. M.; Maaijen, K.; Weng, T. C.; Glatzel, P.; Weckhuysen, B. M. J. Catal. 2010, 276, 268. doi: 10.1016/j.jcat.2010.09.018 doi: 10.1016/j.jcat.2010.09.018
20. [20]
  Nykänen, L.; Honkala, K. ACS Catal. 2013, 3, 3026. doi: 10.1021/cs400566y doi: 10.1021/cs400566y
21. [21]
  Wang, Y.; Hu, Z. -P.; Lv, X.; Chen, L.; Yuan, Z. -Y. J. Catal. 2020, 385, 61. doi: 10.1016/j.jcat.2020.02.019 doi: 10.1016/j.jcat.2020.02.019
22. [22]
  Liu, L.; Díaz, U.; Arenal, R.; Agostini, G.; Concepción, P.; Corma, A. Nat. Mater. 2017, 16, 132. doi: 10.1038/nmat4757 doi: 10.1038/nmat4757
23. [23]
  Liu, L.; Liu, J.; Zeng, Y.; Tan, S. J.; Do, D. D.; Nicholson, D. Chem. Eng. J. 2019, 370, 866. doi: 10.1016/j.cej.2019.03.262 doi: 10.1016/j.cej.2019.03.262
24. [24]
  Han, S. W.; Park, H.; Han, J.; Kim, J. -C.; Lee, J.; Jo, C.; Ryoo, R. ACS Catal. 2021, 11, 9233. doi: 10.1021/acscatal.1c01808 doi: 10.1021/acscatal.1c01808
25. [25]
  Zhao, D.; Tian, X. X.; Doronkin, D. E.; Han, S. L.; Kondratenko, V. A.; Grunwaldt, J. -D.; Perechodjuk, A.; Vuong, T. H.; Rabeah, J.; Eckelt, E.; et al. Nature 2021, 599, 234. doi: 10.1038/s41586-021-03923-3 doi: 10.1038/s41586-021-03923-3
26. [26]
  Song, S. J.; Yang, K.; Zhang, P.; Wu, Z. J.; Li, J.; Su, H.; Dai, H.; Xu, C. M.; Li, Z. X.; Liu, J.; et al. ACS Catal. 2022, 12, 5997. doi: 10.1021/acscatal.2c00928 doi: 10.1021/acscatal.2c00928
27. [27]
  Sun, Q. M.; Wang, N.; Fan, Q. Y.; Zeng, L.; Mayoral, A.; Miao, S.; Yang, R.; Jiang, Z.; Zhou, W.; Zhang, J. C.; et al. Angew. Chem. Int. Ed. 2020, 59, 19450. doi: 10.1002/anie.202003349 doi: 10.1002/anie.202003349
28. [28]
  Li, J.; Zhao, Z.; Fan, X.; Liu, J.; Wei, Y.; Duan, A.; Xie, Z.; Liu, Q. J. Catal. 2017, 352, 361. doi: 10.1016/j.jcat.2017.05.024 doi: 10.1016/j.jcat.2017.05.024
29. [29]
  Zhu, H.; Anjum, D. H.; Wang, Q.; Abou-Hamad, E.; Emsley, L.; Dong, H.; Laveille, P.; Li, L.; Samal, A. K.; Basset, J. -M. J. Catal. 2014, 320, 52. doi: 10.1016/j.jcat.2014.09.013 doi: 10.1016/j.jcat.2014.09.013
30. [30]
  Tolek, W.; Suriye, K.; Praserthdam, P.; Panpranot, J. Catal. Today 2020, 358, 100. doi: 10.1016/j.cattod.2019.08.047 doi: 10.1016/j.cattod.2019.08.047
31. [31]
  Wang, T.; Jiang, F.; Liu, G.; Zeng, L.; Zhao, Z. -J.; Gong, J. AIChE J. 2016, 62, 4365. doi: 10.1002/aic.15339 doi: 10.1002/aic.15339
32. [32]
  Hu, P.; Lang, W. -Z.; Yan, X.; Chu, L. -F.; Guo, Y. -J. J. Catal. 2018, 358, 108. doi: 10.1016/j.jcat.2017.12.004 doi: 10.1016/j.jcat.2017.12.004
33. [33]
  Tang, Y.; Wei, Y. C.; Wang, Z. Y.; Zhang, S. R.; Li, Y. T.; Nguyen, L.; Li, Y. X.; Zhou, Y.; Shen, W. J.; Tao F. F.; et al. J. Am. Chem. Soc. 2019, 141, 7283. doi: 10.1021/jacs.8b10910 doi: 10.1021/jacs.8b10910
34. [34]
  Wu, L.; Ren, Z.; He, Y.; Yang, M.; Yu, Y.; Liu, Y.; Tan, L.; Tang, Y. ACS Appl. Mater. Interfaces 2021, 13, 48934. doi: 10.1021/acsami.1c15892 doi: 10.1021/acsami.1c15892
35. [35]
  Iwasaki, M.; Yamazaki, K.; Banno, K.; Shinjoh, H. J. Catal. 2008, 260, 205. doi: 10.1016/j.jcat.2008.10.009 doi: 10.1016/j.jcat.2008.10.009
36. [36]
  Santhosh Kumar, M.; Schwidder, M.; Grünert, W.; Bentrup, U.; Brückner, A. J. Catal. 2006, 239, 173. doi: 10.1016/j.jcat.2006.01.024 doi: 10.1016/j.jcat.2006.01.024
37. [37]
  Xu, Z.; Yue, Y.; Bao, X.; Xie, Z.; Zhu, H. ACS Catal. 2020, 10, 818. doi: 10.1021/acscatal.9b03527 doi: 10.1021/acscatal.9b03527
38. [38]
  Lundwall, M. J.; McClure, S. M.; Goodman, D. W. J. Phys. Chem. C 2010, 114, 7904. doi: 10.1021/jp9119292 doi: 10.1021/jp9119292
39. [39]
  Aksoy, M.; Metin, Ö. ACS Appl. Nano Mater. 2020, 3, 6836. doi: 10.1021/acsanm.0c01208 doi: 10.1021/acsanm.0c01208
40. [40]
  Liao, T. -W.; Yadav, A.; Ferrari, P.; Niu, Y.; Wei, X. -K.; Vernieres, J.; Hu, K. -J.; Heggen, M.; Dunin-Borkowski, R. E.; Palmer, R. E.; et al. Chem. Mater. 2019, 31, 10040. doi: 10.1021/acs.chemmater.9b02824 doi: 10.1021/acs.chemmater.9b02824
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