Citation: Dong LI, Jia-Xin SONG, Lian KONG, Zhen ZHAO. Effect of P promoter on the oxidative dehydrogenation of ethane over Ni-Al-O catalysts[J]. Chinese Journal of Inorganic Chemistry, ;2023, 39(4): 637-648. doi: 10.11862/CJIC.2023.023 shu

Effect of P promoter on the oxidative dehydrogenation of ethane over Ni-Al-O catalysts

Dong LI ^{1, 2} ,
Jia-Xin SONG ^{1, 2} ,
Lian KONG ^2,, ,
Zhen ZHAO ^{1, 2,,}

1.
State Key Laboratory of Heavy Oil, China University of Petroleum, Beijing 102249, China
2.
College of Chemistry and Chemical Engineering, Institute of Catalysis for Energy and Environment, Shenyang Normal University, Shenyang 110034, China

Corresponding author: Lian KONG, konglian0907@163.com Zhen ZHAO, zhenzhao@cup.edu.cn; zhaozhen@synu.edu.cn
Received Date: 22 September 2022
Revised Date: 10 January 2023

Figures(11)

A series of phosphorus-modified Ni-Al-O catalysts (P_x-Ni-Al-O) were prepared by the one-pot hydrothermal method.The performance of the oxidative dehydrogenation of ethane to ethylene over series catalysts was evaluated by using O₂ as an oxidant.The results showed that the P incorporation can not only reduce the crystallite sizes of NiO, but also affect the interaction between Ni and Al.In the temperature range of 350-475℃, the selectivities towards ethylene over P-modified Ni-Al-O catalysts were higher than those over the unmodified catalyst, and the addition of the appropriate amount of P could also improve the ethane conversion.The selectivity and yield of ethylene over the P_0.15-Ni-Al-O catalyst were 61.4% and 31.9% at 475℃, respectively.Moreover, the P-modified catalyst showed a strong resistance to carbon deposition and remained the catalytic performance for 22 h after a continuous reaction.
- hydrothermal method,
- promoter P,
- Ni-Al-O catalyst,
- oxidative dehydrogenation of ethane
1. [1]
  Najari S, Saeidi S, Concepcion P, Dionysiou D D, Bhargava S K, Lee A F, Wilson K. Oxidative dehydrogenation of ethane: Catalytic and mechanistic aspects and future trends[J]. Chem. Soc. Rev., 2021,50(7):4564-4605. doi: 10.1039/D0CS01518K
2. [2]
  Li G M, Liu C, Cui X J, Yang Y H, Shi F. Oxidative dehydrogenation of light alkanes with carbon dioxide[J]. Green. Chem., 2021,23(2):689-707. doi: 10.1039/D0GC03705B
3. [3]
  Choudhary V R, Mulla S A R. Coupling of thermal cracking with noncatalytic oxidative conversion of ethane to ethylene[J]. AIChE J., 1997,43(6):1545-1550. doi: 10.1002/aic.690430617
4. [4]
  Solsona B, Concepción P, Nieto J M L, Dejoz A, Agouram S, Soriano M D, Tottes V., Jiménez J J, Castellón E R. Nickel oxide supported on porous clay heterostructures as selective catalysts for the oxidative dehydrogenation of ethane[J]. Catal. Sci. Technol., 2016,6(10):3419-3429. doi: 10.1039/C5CY01811K
5. [5]
  Cotillo M H, Unsihuay D, Santolalla-Vargas C E, Doig A P, Kou R S, Picasso G. Catalysts based on Ni-Fe oxides supported on γ-Al₂O₃ for the oxidative dehydrogenation of ethane[J]. Catal. Today, 2020,356:312-321. doi: 10.1016/j.cattod.2019.05.044
6. [6]
  RuiHerrera Y, Chen J E, Li H C, Cathy Y H. Generalized mechanistic framework for ethane dehydrogenation and oxidative dehydrogenation on molybdenum oxide catalysts[J]. ACS Catal., 2020,10(12):6952-6968. doi: 10.1021/acscatal.0c01073
7. [7]
  GE X, SUN Q, SHEN J Y. A Study on Cr/CeO₂ catalysts and their catalytic performance for dehydrogenation of ethane[J]. Chinese J. Inorg. Chem., 2004(8):987-990.
8. [8]
  Song G Z, Wang Q, Yang L, Liao D H, Li S. Oxidative dehydrogenation of ethane with CO₂ over Mo/LDO catalyst: The active species of Mo controlled by LDO[J]. Catalysts, 2022,12(5)493. doi: 10.3390/catal12050493
9. [9]
  Zhou Y L, Wei F F, Lin J, Li L, Li X Y, Qi H F, Pan X L, Liu X Y, Huang C D, Lin S, Wang X D. Sulfate-modified NiAl mixed oxides as effective C—H bond-breaking agents for the sole production of ethylene from ethane[J]. ACS Catal., 2020,10(14):7619-7629. doi: 10.1021/acscatal.0c02347
10. [10]
  Zhou Y L, Lin J, Li L, Tian M, Li X Y, Pan X L, Chen Y, Wang X D. Improving the selectivity of Ni-Al mixed oxides with isolated oxygen species for oxidative dehydrogenation of ethane with nitrous oxide[J]. J. Catal., 2019,377:438-448. doi: 10.1016/j.jcat.2019.07.050
11. [11]
  Solsona B, Concepción P, Demicol B, Hernández S, Delgado J J, Calvino J J, Nieto J M L. Selective oxidative dehydrogenation of ethane over SnO₂-promoted NiO catalysts[J]. J. Catal., 2012,295:104-114. doi: 10.1016/j.jcat.2012.07.028
12. [12]
  Heracleous E, Lemonidou A A. Ni-Me-O mixed metal oxides for the effective oxidative dehydrogenation of ethane to ethylene-effect of promoting metal Me[J]. J. Catal., 2010,270(1):67-75. doi: 10.1016/j.jcat.2009.12.004
13. [13]
  Zhu H B, Rosenfeld D C, Harb M, Anjum D H, Hedhili M N, Ould-Chikh S, Basset J M. Ni-M-O (M=Sn, Ti, W) catalysts prepared by a dry mixing method for oxidative dehydrogenation of ethane[J]. ACS Catal., 2016,6(5):2852-2866. doi: 10.1021/acscatal.6b00044
14. [14]
  Ducarme V, Martin G A. Low temperature oxidative dehydrogenation of ethane over Ni-based catalysts[J]. Catal. Lett., 1994,23:97-101. doi: 10.1007/BF00812135
15. [15]
  Santander J, López E, Diez A, Dennehy M, Pedernera M, Tonetto G. Ni-Nb mixed oxides: One-pot synthesis and catalytic activity for oxidative dehydrogenation of ethane[J]. Chem. Eng. J., 2014,255:185-194. doi: 10.1016/j.cej.2014.06.048
16. [16]
  Heracleous E, Lemonidou A A. Ni-Nb-O mixed oxides as highly active and selective catalysts for ethene production via ethane oxidative dehydrogenation. Part Ⅰ: Characterization and catalytic performance[J]. J. Catal., 2006,237(1):162-174.
17. [17]
  Heracleous E, Delimitis A, Nalbandian L, Lemonidou A A. HRTEM characterization of the nanostructural features formed in highly active Ni-Nb-O catalysts for ethane ODH[J]. Appl. Catal. A-Gen., 2007,325(2):220-226. doi: 10.1016/j.apcata.2007.02.030
18. [18]
  Heracleous E, Lee A F, Wilson K, Lemonidou A A. Investigation of Ni-based alumina-supported catalysts for the oxidative dehydrogenation of ethane to ethylene: Structural characterization and reactivity studies[J]. J. Catal., 2005,231(1):159-171. doi: 10.1016/j.jcat.2005.01.015
19. [19]
  Gaab S, Machli M, Find J, Grasselli R K, Lercher J A. Oxidative dehydrogenation of ethane over novel Li/Dy/Mg mixed oxides: Structure-activity study[J]. Top. Catal., 2003,23(1):151-158.
20. [20]
  Kong L, Li D, Zhao Z, Li J M, Zhao L L, Fan X Q, Xiao X, Xie Z A. Preparation, characterization, and catalytic performance of rod-like Ni-Nb-O catalysts for the oxidative dehydrogenation of ethane at low temperature[J]. Catal. Sci. Technol., 2019,9(13):3416-3425. doi: 10.1039/C9CY00519F
21. [21]
  Skoufa Z, Xantri G, Heracleous E. A study of Ni-Al-O mixed oxides as catalysts for the oxidative conversion of ethane to ethylene[J]. Appl. Catal. A-Gen., 2014,471:107-117. doi: 10.1016/j.apcata.2013.11.042
22. [22]
  Lin X Z, Li G C, Huang C J, Weng W Z, Wan H L. P-modified cobalt oxide: A novel and effective catalyst for oxidative dehydrogenation of propane[J]. Chin. Chem. Lett., 2013,24(9):789-792. doi: 10.1016/j.cclet.2013.05.013
23. [23]
  Ivan S B, Popescu I, Fechete I, Garin F, Pârvulescu V I, Marcu I C. The effect of phosphorus on the catalytic performance of nickel oxide in ethane oxidative dehydrogenation[J]. Catal. Sci. Technol., 2016,6(18):6953-6964. doi: 10.1039/C6CY00946H
24. [24]
  Ko J, Muhlenkamp J A, Bonita Y, LiBretto N J, Miller J T, Hicks J C, Schenider W F. Experimental and computational investigation of the role of P in moderating ethane dehydrogenation performance over Ni-based catalysts[J]. Ind. Eng. Chem. Res., 2020,59(28):12666-12676. doi: 10.1021/acs.iecr.0c00908
25. [25]
  Maiti A, Govind N, Kung P, Smith D K, Miller J E, Zhang C, Whitwell G. Effect of surface phosphorus on the oxidative dehydrogenation of ethane: A first-principles investigation[J]. J. Chem. Phys., 2002,117(17):8080-8088. doi: 10.1063/1.1510122
26. [26]
  El-Idrissi J, Kacimi M, Bozon-Verduraz F, Ziyad M. Oxidative dehydrogenation of ethane over Cr/TiO₂ modified by phosphorus[J]. Catal. Lett., 1998,56(4):221-225. doi: 10.1023/A:1019025600050
27. [27]
  Singh , R P, Banares M, Deo G. Effect of phosphorous modifier on V₂O₅/TiO₂ catalyst: ODH of propane[J]. J. Catal., 2005,233(2):388-398. doi: 10.1016/j.jcat.2005.05.010
28. [28]
  Khatib S J, Fierro J L G, Bañares M A. Effect of phosphorous additive on the surface chromium oxide species on alumina for propane oxidation to propylene[J]. Top. Catal., 2009,52(10):1459-1469. doi: 10.1007/s11244-009-9318-x
29. [29]
  Bai Z, Li P, Liu L P, Xiong G. Oxidative dehydrogenation of propane over MoO_x and PO_x supported on carbon nanotube catalysts[J]. ChemCatChem, 2012,4(2):260-264. doi: 10.1002/cctc.201100242
30. [30]
  Gao X X, Wang J, Xu A J, Jia M L. Oxidative dehydrogenation of propane over Ni-Al mixed oxides: Effect of the preparation methods on the activity of surface Ni(Ⅱ) species[J]. Catal. Lett., 2021,151(2):497-506. doi: 10.1007/s10562-020-03317-6
31. [31]
  Liu Y M, Cong P J, Doolen R D, Guan S H, Markov V, Woo L, Zeyß S, Dingerdissen U. Discovery from combinatorial heterogeneous catalysis: A new class of catalyst for ethane oxidative dehydrogenation at low temperatures[J]. Appl. Catal. A-Gen., 2003,254(1):59-66. doi: 10.1016/S0926-860X(03)00263-1
32. [32]
  Li J H, Li R G, Wang C C, Huang C J, Weng W Z, Wan H L. Oxidative dehydrogenation of ethane to ethylene over mesoporous Ni-based catalysts[J]. Chin. J. Catal., 2009,30(8):714-716. doi: 10.1016/S1872-2067(08)60122-9
33. [33]
  Solsona B, Nieto J M L, Concepción P, Dejoz A, Lvars F, Vázquez M I. Oxidative dehydrogenation of ethane over Ni-W-O mixed metal oxide catalysts[J]. J. Catal., 2011,280(1):28-39. doi: 10.1016/j.jcat.2011.02.010
34. [34]
  Zhu H B, Rosenfeld D C, Anjum D H, Sangaru S S, Saih Y, Chikh S O, Basset J M. Ni-Ta-O mixed oxide catalysts for the low temperature oxidative dehydrogenation of ethane to ethylene[J]. J. Catal., 2015,329:291-306. doi: 10.1016/j.jcat.2015.05.023
35. [35]
  Biju V, Khadar M A. Electronic structure of nanostructured nickel oxide using Ni2p XPS analysis[J]. J. Nanopart. Res., 2002,4(3):247-253. doi: 10.1023/A:1019949805751
36. [36]
  Veenendaal M A V, Sawatzky G A. Nonlocal screening effects in 2p X-ray photoemission spectroscopy core-level line shapes of transition metal compounds[J]. Phys. Rev. Lett., 1993,70(16):2459-2462. doi: 10.1103/PhysRevLett.70.2459
37. [37]
  Zhu H B, Dong H L, Laveille P, Saih Y, Caps V, Basset J M. Metal oxides modified NiO catalysts for oxidative dehydrogenation of ethane to ethylene[J]. Catal. Today, 2014,228:58-64. doi: 10.1016/j.cattod.2013.11.061
38. [38]
  Wang C, Cui X B, Liu J Y, Zhou X, Cheng X Y, Sun P, Hu X L, Li X W, Zheng J, Lu G Y. Design of superior ethanol gas sensor based on Al-doped NiO nanorod-flowers[J]. ACS Sens., 2016,1(2):131-136. doi: 10.1021/acssensors.5b00123
39. [39]
  Stoyanova M, Konova P, Nikolov P, Naydenov A, Christoskova S, Mehandjiev D. Alumina-supported nickel oxide for ozone decomposition and catalytic ozonation of CO and VOCs[J]. Chem. Eng. J., 2006,122(1/2):41-46.
40. [40]
  Iwamoto M, Yoda Y, Egashira M, Seiyama T. Study of metal oxide catalysts by temperature programmed desorption chemisorption of oxygen on nickel oxide[J]. J. Phys. Chem., 1976,80(18):1989-1994. doi: 10.1021/j100559a008
41. [41]
  Shi Z J, Lian Y F, Liao F H, Zhou X H, Gu Z N, Zhang Y G, Lijima S. Purification of single-wall carbon nanotubes[J]. Solid State Commun., 1999,112(1):35-37. doi: 10.1016/S0038-1098(99)00278-1
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