Citation: LI Zhen-hua, QU Jiang-lei, WANG Wei-han, WANG Bao-wei, MA Xin-bin. Effect of CO₂ in syngas on methanation performance of Mo-based catalyst[J]. Journal of Fuel Chemistry and Technology, ;2016, 44(8): 985-992. shu

Effect of CO₂ in syngas on methanation performance of Mo-based catalyst

Key Lab for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China

Corresponding author: WANG Wei-han, wangwh@tju.edu.cn MA Xin-bin, xbma@tju.edu.cn
Received Date: 29 February 2016
Revised Date: 23 April 2016

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The methanation of synthesis gas is the key process of coal to natural gas. Considering the existence of CO₂ in the synthesis gas, it is important to investigate the influence of CO₂ on the sulfur-resistant methanation. In this paper, the effect of CO₂ on methanation activity of Mo-based catalysts was investigated at the reaction temperature of 550℃ and the gas space velocity of 5000h^-1 with the syngas containing 1.2% H₂S (volume ratio). The results show that the promoter Co and the cerium-aluminum composite support can improve the stability of the catalyst and reduce the deactivation. The CO₂ is proved to promote the reverse water gas shift reaction, which would inhibit the activity of MoO₃/Al₂O₃ catalyst more heavily than MoO₃-CoO/CeO₂-Al₂O₃ catalyst. When the CO₂ adding to the inlet gas is less than 10% for 20h, the catalyst activity could be restored to its original activity after stopping the addition of CO₂. However, as the added CO₂ in inlet gas is over 10%, more H₂O will be generated through reverse water gas shift reaction to damage the catalyst structure and decrease the active component, resulting in an irreversible loss of catalyst activity.
- sulfur-resistant methanation,
- Mo-based catalyst,
- carbon dioxide,
- deactivation,
- water-gas shift
1. [1]
  ZHANG Dong-ke. Energy options in sustainable development[J]. J Fuel Chem Technol, 2005,33(4):399-406.
2. [2]
  HU Liang-hua, FENG Zai-nan, YAO Ze-long, LIU Wei, SHEN Tu-liang, WANG Jun-feng. Aspen Plus simulation of coke oven gas methanation process[J]. Nat Gas Ind, 2013,38(3):53-57.
3. [3]
  SABATIER P, SENDERENS J B. New synthesis of methane[J]. CR Acad Sci Paris, 1902,134:514-516.
4. [4]
  SABATIER P, SENDERENS J B. Hydrogenation of CO over nickel to produce methane[J]. J Soc Chim Ind, 1902,21:504-506.
5. [5]
  HUANG Guo-bao, WANG Zhi-qing, LI Qing-feng, HUANG Jie-jie, FANG Yi-tian. Syngas methanation over nickel catalyst in liquid-phase[J]. J Fuel Chem Technol, 2014,42(8):952-957.
6. [6]
  MINCHENER A J. Coal gasification for advanced power generation[J]. Fuel, 2005,84(17):2222-2235. doi: 10.1016/j.fuel.2005.08.035
7. [7]
  SCHILDHAUER T J, SEEMANN M C, BIOLLAZ S M A. Fluidized bed methanation of wood-derived producer gas for the production of synthetic natural gas[J]. Ind Eng Chem Res, 2010,49(15):7034-7038. doi: 10.1021/ie100510m
8. [8]
  WU Qie-yi, QIN Tao, YAN Zhi.Method for synthesizing methane by using coke-oven gas:CN, 101391935 A[P].2009-03-25.
9. [9]
  HUANG Ming-jin, GUO Cheng-yu, YIN Ming-da.Methanation process for raw gas of synthetic ammonia:CN, 1313241 A[P].2001-09-19.
10. [10]
  GALLETTI C, SPECCHIAS , SARACCO G, SPECCHIA V. CO-selective methanation over Ru/γ-Al₂O₃ catalysts in H₂-rich gas for PEMFC applications[J]. Chem Eng Sci, 2010,65(1):590-596. doi: 10.1016/j.ces.2009.06.052
11. [11]
  XU Chao, WANG Xing-jun, HU Xian-hui, CHEN Xue-li, WANG Fu-chen. Study on the syngas methanation of nickel-based catalyst[J]. J Fuel Chem Technol, 2012,40(2):216-220.
12. [12]
  GAO J J, LIU Q, GU F N, LIU B, ZHONG Z Y, SU F B. Recent advances in methanation catalysts for the production of synthetic natural gas[J]. RSC Adv, 2015,5(29):22759-22776. doi: 10.1039/C4RA16114A
13. [13]
  GAO Ju-zhong. Application and development of coal gasification technologies[J]. Clean Coal Technol, 2013(1):65-71.
14. [14]
  YUAN Yong-tian, YIN Yan-hua, ZHOU Xu, ZHOU Jun-cheng. Methanation of thoree diffenent reaction systems of carbon oxides[J]. Chem Ind Eng Process, 2014,33(1):173-180.
15. [15]
  YI Li-li, MA Lei, LU Chun-shan, LI Xiao-nian. Study on the catalytic hydrogenation of carbon dioxide for methanation[J]. Chem Prod Technol, 2004,11(5):33-35.
16. [16]
  JIMÉNEZ V, SANCHEZ P, PANAGIOTOPOULOU P, VALVERDE J, ROMERO A. Methanation of CO, CO₂ and selective methanation of CO, in mixtures of CO and CO₂, over ruthenium carbon nanofibers catalysts[J]. Appl Catal A:Gen, 2010,390(1/2):35-44.
17. [17]
  PANAGIOTOPOULOU P, KONDARIDES D, VERKIOS X. Selective methanation of CO over supported noble metal catalysts:Effects of the nature of the metallic phase on catalytic performance[J]. Appl Catal A:Gen, 2008,344(1/2):45-54.
18. [18]
  ECKLE S, ANFANG H, BEHM R. What drives the selectivity for CO methanation in the methanation of CO₂-rich reformate gases on supported Ru catalysts[J]. Appl Catal A:Gen, 2011,391(1):325-333.
19. [19]
  WANG Cheng-xue, GONG Jie. Study on Ni-Mn-based catalysts for methanation of carbon dioxide[J]. Nat Gas Ind, 2011,36(1):4-15.
20. [20]
  WANG Er-dong, WANG Hai-yang, DING Guo-zhong, SHANG Yu-guang, LI Zhen-hua, WANG Bao-wei, MA Xin-bin, QIN Shao-dong, SUN Qi. Effect of reaction parameters on the activity of sulfur-resistant methanation catalyst[J]. Chem React Eng Technol, 2012,28(1):75-81.
21. [21]
  LI Z H, WANG H Y, WANG E D, LV J, SHANG Y G, DING G Z, WANG B W, MA X B, QIN S D, SU Q. The main factors controlling generation of synthetic natural gas by methanation of synthesis gas in the presence of sulphur-resistant Mo-based catalysts[J]. Kinet Catal, 2013,54(3):338-343. doi: 10.1134/S0023158413030117
22. [22]
  WANG B W, DING G Z, SHANG Y G, LV J, WANG H Y, WANG E D, LI Z H, MA X B, QIN S D, SUN Q. Effects of MoO₃ loading and calcination temperature on the activity of the sulphur-resistant methanation catalyst MoO₃/γ-Al₂O₃[J]. Appl Catal A:Gen, 2012,431-432(1):144-150.
23. [23]
  LIN C, WANG H Y, LI Z H, WANG B W, MA X B, QIN S D, SUN Q. Effect of a promoter on the methanation activity of Mo-based sulfur-resistant catalyst[J]. Front Chem Sci Eng, 2013,7(1):88-94. doi: 10.1007/s11705-013-1301-1
24. [24]
  WANG Bao-wei, SHANG Yu-guang, DING Guo-zhong, WANG Hai-yang, WANG Er-dong, LI Zhen-hua, MA Xin-bin, QIN Shao-dong, SUN Qi. Ceria-alumina composite support on the sulfur-resistant methanation activity of Mo-based catalyst[J]. J Fuel Chem Technol, 2012,40(11):1390-1396.
25. [25]
  CUI Xiao-xi, CAO Hui-bo, MENG Fan-hui, LI Zhong. Thermodynamic analysis for methanation of syngas[J]. Nat Gas Ind, 2012,37(5):15-19.
26. [26]
  CHENG Hong-gang, WANG Teng-da, ZHANG Kai, NIU Yu-guang, YANG Yong-ping. Thermodynamic analysis of carbon deposition on catalyst for the production of substitute natural gas[J]. J Fuel Chem Technol, 2013,41(8):978-984.
27. [27]
  DOU Bo-sheng, XIE Xiao-fan, WANG Yu-jie, SHI Xin. Sulfer loss and activity of Co-Mo-K/Al₂O₃ water gas shift catalyst[J]. Petrochem Technol, 1990(6):387-389.
28. [28]
  LAURENT E, DELMON B. Influence of water in the deactivation of a sulfided NiMo/γ-Al₂O₃ catalyst during hydrodeoxygenation[J]. J Catal, 1994,146(1):281-285. doi: 10.1016/0021-9517(94)90032-9
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Effect of CO2 in syngas on methanation performance of Mo-based catalyst

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Effect of CO₂ in syngas on methanation performance of Mo-based catalyst