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Citation: LIAN Mengshui, WANG Yali, ZHAO Mingquan, LI Qianqian, WENG Weizheng, XIA Wensheng, WAN Huilin. Stability of Ni/SiO2 in Partial Oxidation of Methane: Effects of W Modification[J]. Acta Physico-Chimica Sinica, ;2019, 35(6): 607-615. doi: 10.3866/PKU.WHXB201805054 shu

Stability of Ni/SiO2 in Partial Oxidation of Methane: Effects of W Modification

  • Fujian Province Key Laboratory of Theoretical and Computational Chemistry, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, State Key Laboratory of Physical Chemistry of Solid State Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian Province, P. R. China

  • Corresponding author: XIA Wensheng, wsxia@xmu.edu.cn WAN Huilin, hlwan@xmu.edu.cn
  • Received Date: 20 May 2018
    Revised Date: 12 June 2018
    Accepted Date: 20 June 2018
    Available Online: 11 June 2018

    Fund Project: The project was supported by the National Natural Science Foundation of China (21373169), and PCSIRT (IRT1036)the National Natural Science Foundation of China 21373169PCSIRT IRT1036

  • With the discovery and large-scale exploitation of natural gas resources such as shale gas and combustible ice, which are mainly composed of methane, their effective utilization has become a national strategic interest. Partial oxidation of methane (POM) to synthesis gas is one of the important methods for the utilization of natural gas and shale gas resources. The commonly used Ni/SiO2 catalyst for POM easily deactivates due to carbon deposition on the surface. To solve this problem, a urea precipitation method was employed in this work to prepare Ni-based catalysts modified with different amounts of tungsten (at W/Ni molar ratios of 0, 0.01, 0.03, 0.05, 0.07, and 0.10), and the catalyst stability in POM as well as the role of W were investigated. From characterizations such as X-ray diffraction (XRD), transmission electron microscopy (TEM), temperature-programmed reduction (H2-TPR), and X-ray photoelectron spectroscopy (XPS), we obtained the following results. The amount of W added to the Ni-based catalysts has a significant influence on their catalytic performances in POM and their physicochemical properties. The particle size of Ni in the catalysts decreases with W addition, and the Ni particle distribution on the support surfaces becomes more uniformed; however, the catalytic activity for POM is not significantly influenced. However, W-modified Ni-based catalysts show an increasing improvement in their stability in POM with increasing W/Ni molar ratio, with an optimum at the W/Ni molar ratio of 0.07; at the W/Ni molar ratio of 0.10, they exhibit a rapid deactivation in POM in a short time. Although interactions between Ni and SiO2 in the as-prepared catalysts are weak, the presence of adequate tungsten (W/Ni molar ratio of 0.05 and above) in the Ni-based catalysts can reduce the Ni particle size to some extent, and lead to the formation of strong interactions between Ni and W, which leads to an improvement in the dispersion of Ni on the support surface and imparts resistance for Ni particle growth in the POM reaction. The increased interaction between Ni and W changes the chemical state or oxygen affinity of Ni particles on the catalyst surfaces, and some of the partially oxidized Ni species (Niδ+) on the catalyst surfaces coexist with reduced Ni species (Ni0) during POM. Using an adequate amount of W-modified Ni catalysts results in almost no carbon deposition on the surfaces during POM, but using only a moderate amount results in good catalytic behavior and stability in POM. This finding suggests that the presence of W can not only enhance the anti-coking ability of the Ni-based catalysts and sustain their good stability in POM if the W content is low (i.e., W/Ni molar ratio of 0.07 and below), but also lead to the deactivation of W-modified catalysts in POM if the W content is high (i.e., W/Ni molar ratio of 0.10 and above), due to high oxygen affinity or the presence of more Ni species in oxidized form. In addition, α-WC (tungsten carbide) was identified using XRD to be formed on the surface of the moderate-amount W-modified Ni catalysts after POM, and it could inhibit or eliminate carbon deposition on the Ni-based catalyst surfaces. The catalytic performance evaluation of the catalysts in POM under a long time period confirmed that α-WC is stable.
  • 加载中
    1. [1]

      Chai, R. J.; Zhang, Z. Q.; Chen, P. J.; Zhao, G. F.; Liu, Y.; Lu, Y. Microporous Mesoporous Mater. 2017, 253, 123. doi: 10.1016/j.micromeso.2017.07.005  doi: 10.1016/j.micromeso.2017.07.005

    2. [2]

      Luo, Z.; Kriz, D. A.; Miao, R.; Kuo, C. H.; Zhong, W.; Guild, C.; He, J. K.; Willis, B.; Dang, Y. L.; Suib, S. L.; et al. Appl. Catal. A 2018, 554, 54. doi: 10.1016/j.apcata.2018.01.020  doi: 10.1016/j.apcata.2018.01.020

    3. [3]

      Wang, F.; Li, W. Z.; Lin, J. D.; Chen, Z. Q.; Wang, Y. Appl. Catal. B 2018, 231, 292. doi: 10.1016/j.apcatb.2018.03.018  doi: 10.1016/j.apcatb.2018.03.018

    4. [4]

      Guo, S. S.; Wang, J. W.; Ding, C. M.; Duan, Q. L.; Ma, Q.; Zhang, K.; Liu, P. Int. J. Hydrog. Energy 2018, 43, 6603. doi: 10.1016/j.ijhydene.2018.02.035  doi: 10.1016/j.ijhydene.2018.02.035

    5. [5]

      Yang, M. H.; Wu, H. H.; Wu, H. Y.; Huang, C. J.; Weng, W. Z.; Chen, M. S.; Wan, H. L. RSC Adv. 2016, 6, 81237. doi: 10.1039/c6ra15358e  doi: 10.1039/c6ra15358e

    6. [6]

      Kim, D.; Park, G. A.; Lim, J.; Ha, K. S. Chem. Eng. J. 2017, 316, 1011. doi: 10.1016/j.cej.2017.02.014  doi: 10.1016/j.cej.2017.02.014

    7. [7]

      Rodemerck, U.; Schneider, M.; Linke, D. Catal. Commun. 2017, 102, 98. doi: 10.1016/j.catcom.2017.08.031  doi: 10.1016/j.catcom.2017.08.031

    8. [8]

      Li, L.; He, S. C.; Song, Y. Y.; Zhao, J.; Ji, W. J.; Au, C. T. J. Catal. 2012, 288, 54. doi: 10.1016/j.jcat.2012.01.004  doi: 10.1016/j.jcat.2012.01.004

    9. [9]

      Wang, F. G.; Han, B. L.; Zhang, L. J.; Xu, L. L.; Yu, H.; Shi, W. D. Appl. Catal. B 2018, 235, 26. doi: 10.1016/j.apcatb.2018.04.069  doi: 10.1016/j.apcatb.2018.04.069

    10. [10]

      Ashok, J.; Bian, Z.; Wang, Z.; Kawi, S. Catal. Sci. Technol. 2018, 8, 1730. doi: 10.1039/c7cy02475d  doi: 10.1039/c7cy02475d

    11. [11]

      Li, Q.; Hou, Y. H.; Dong, L. Y.; Huang, M. X.; Weng, W. Z.; Xia, W. S.; Wan, H. L. Acta Phys. -Chim. Sin. 2013, 29, 2245.  doi: 10.3866/PKU.WHXB201308201

    12. [12]

      Wu, H. J.; Pantaleo, G.; La Parola, V.; Venezia, A. M.; Collard, X.; Aprile, C.; Liotta, L. F. Appl. Catal. B 2014, 156–157, 350. doi: 10.1016/j.apcatb.2014.03.018  doi: 10.1016/j.apcatb.2014.03.018

    13. [13]

      Zhu, J. Q.; Peng, X. X.; Yao, L.; Tong, D. M.; Hu, C. W. Catal. Sci. Technol. 2012, 2, 529. doi: 10.1039/c1cy00333j  doi: 10.1039/c1cy00333j

    14. [14]

      Wang, Y. L.; Li, Q.; Weng, W. Z.; Xia, W. S.; Wan, H. L. Acta Phys. -Chim. Sin. 2016, 32, 2776.  doi: 10.3866/PKU.WHXB201608302

    15. [15]

      Zhao, X. Y.; Li, H. R.; Zhang, J. P.; Shi, L. Y.; Zhang, D. S. Int. J. Hydrog. Energy 2016, 41, 2447. doi: 10.1016/j.ijhydene.2015.10.111  doi: 10.1016/j.ijhydene.2015.10.111

    16. [16]

      Zhang, S. H.; Shi, C.; Chen, B. B.; Zhang, Y. L.; Qiu, J. S. Catal. Commun. 2015, 69, 123. doi: 10.1016/j.catcom.2015.06.003  doi: 10.1016/j.catcom.2015.06.003

    17. [17]

      Claridge, J. B.; York, A. P. E.; Brungs, A. J.; Marquez-Alvarez, C.; Sloan, J.; Tsang, S. C.; Green, M. L. H. J. Catal. 1998, 180, 85. doi: 10.1006/jcat.1998.2260  doi: 10.1006/jcat.1998.2260

    18. [18]

      Li, J. F.; Xiao, B.; Yan, R.; Yi, R. J. Chem. Eng. 2007, 35, 53.

    19. [19]

      Jiang, J. T.; Wei, X. J.; Xu, C. Y.; Zhou, Z. X.; Zhen, L. J. Magn. Magn. Mater. 2013, 334, 111. doi: 10.1016/j.jmmm.2012.12.036  doi: 10.1016/j.jmmm.2012.12.036

    20. [20]

      Ding, C. M.; Wang, J. W.; Ai, G. G.; Liu, S. B.; Liu, P.; Zhang, K.; Han, Y. L.; Ma, X. S. Fuel 2016, 175, 1. doi: 10.1016/j.fuel.2016.02.024  doi: 10.1016/j.fuel.2016.02.024

    21. [21]

      He, S. F.; Zheng, X. M.; Mo, L. Y.; Yu, W. J.; Wang, H.; Luo, Y. M. MRS Bull. 2014, 49, 108. doi: 10.1016/j.materresbull.2013.08.051  doi: 10.1016/j.materresbull.2013.08.051

    22. [22]

      Xia, W. S.; Hou, Y. H.; Chang, G.; Weng, W. Z.; Han, G. B.; Wan, H. L. Int. J. Hydrog. Energy 2012, 37, 8343. doi: 10.1016/j.ijhydene.2012.02.141  doi: 10.1016/j.ijhydene.2012.02.141

    23. [23]

      Solsona, B.; López Nieto, J. M.; Concepción, P.; Dejoz, A.; Ivars, F.; Vázquez, M. I. J. Catal. 2011, 280, 28. doi: 10.1016/j.jcat.2011.02.010  doi: 10.1016/j.jcat.2011.02.010

    24. [24]

      Venugopal, A.; Naveen Kumar, S.; Ashok, J.; Hari Prasad, D.; Durga Kumari, V.; Prasad, K. B. S.; Subrahmanyam, M. Int. J. Hydrog. Energy 2007, 32, 1782. doi: 10.1016/j.ijhydene.2007.01.007  doi: 10.1016/j.ijhydene.2007.01.007

    25. [25]

      Arbag, H.; Yasyerli, S.; Yasyerli, N.; Dogu, T.; Dogu, G. Top. Catal. 2013, 56, 1695. doi: 10.1007/s11244-013-0105-3  doi: 10.1007/s11244-013-0105-3

    26. [26]

      Theofanidis, S. A.; Galvita, V. V.; Poelman, H.; Marin, G. B. ACS Catal. 2015, 5, 3028. doi: 10.1021/acscatal.5b00357  doi: 10.1021/acscatal.5b00357

    27. [27]

      Xia, W. S.; Chang, G.; Hou, Y. H.; Weng, W. Z.; Wan, H. L. Acta Phys. -Chim. Sin. 2011, 27, 1567.  doi: 10.3866/PKU.WHXB20110627

    28. [28]

      Xia, W. S.; Chen, R. F.; Wang, Y. L.; Li, Q.; Weng, W. Z.; Wan, H. L. Xiamen Univ. J. Nat. Sci. Ed. 2015, 54, 17.  doi: 10.6043/j.issn.0438-0479.2015.05.17

    29. [29]

      Mohammadzadeh Valendar, H.; Yu, D. W.; Barati, M.; Rezaie, H. J. Therm. Anal. Calorim. 2016, 128, 553. doi: 10.1007/s10973-016-5883-y  doi: 10.1007/s10973-016-5883-y

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