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Supported nickel catalysts for low temperature methane steam reforming: comparison between metal additives and support modification

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Abstract

The effect of Ag (1 wt%) and Au (1 wt%) on the catalytic properties of Ni/Al2O3 (7 wt% Ni) for methane steam reforming (MSR) was studied in parallel with the effect of CeO2 (6 wt%) and La2O3 (6 wt%) addition. The addition of 1 wt% Ag to the alumina supported nickel catalyst drastically decreased its catalytic properties at temperatures lower than 600 °C, due to the blockage of metal catalytic centers by silver deposition. The addition of Au and CeO2 (La2O3) to the nickel catalyst improved the methane conversion, CO2 selectivity and hydrogen production at low reaction temperatures (t < 600 °C). At 700 °C under our working conditions, the additives have no important effect in hydrogen production by MSR. The best hydrogen production at low temperatures was obtained for Ni–Au/Al2O3, due to the higher CO2 selectivity, cumulated with slightly higher methane conversion in comparison with Ni/CeO2–Al2O3. At high temperature, Ni/CeO2–Al2O3 is stable for 48 h on stream. Ni–Au/Al2O3 and Ni–Ag/Al2O3 are mainly deactivated due to the temperature effect on Au and Ag nanoparticles and less through coke formation. On Ni/Al2O3 and Ni/La2O3–Al2O3, crystalline, graphitic carbon was deposited after 48 h of reaction leading to catalyst partial deactivation. On the Ni/CeO2–Al2O3 surface, a porous amorphous form of deposited carbon was found, which does not decrease its catalytic activity after 48 h of reaction.

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References

  1. Bartels JR, Pate MB, Olson NK (2010) An economic survey of hydrogen production from conventional and alternative energy sources. Int J Hydrogen Energy 35:8371–8384

    Article  CAS  Google Scholar 

  2. Moon DJ (2008) Hydrogen production by catalytic reforming of gaseous hydrocarbons. Catal Surv Asia 12:188–202

    Article  CAS  Google Scholar 

  3. Holladay JD, Hu J, King DL, Wang Y (2009) An overview of hydrogen production technologies. Catal Today 139:244–260

    Article  CAS  Google Scholar 

  4. Rostrup-Nielsen JR (1984) Catalytic steam reforming. In: Anderson JR, Boudart M (eds) Catalysis: science and technology. Springer, New York

    Google Scholar 

  5. Mehta V, Cooper JS (2003) Review and analysis of PEM fuel cell design and manufacturing. J Power Sources 114:32–53

    Article  CAS  Google Scholar 

  6. Barelli L, Bidini G, Gallorini F, Servili S (2008) Hydrogen production through sorption-enhanced steam methane reforming and membrane technology: a review. Energy 33:554–570

    Article  CAS  Google Scholar 

  7. Chen Y, Cui P, Xiong G, Xu H (2010) Novel nickel based catalysts for low temperature hydrogen production from methane steam reforming in membrane reformer. Asia-Pac J Chem Eng 5:93–100

    Article  Google Scholar 

  8. Iulianelli A, Manzolini G, De Falco M, Campanari S, Longo T, Liguori S et al (2010) H2 production by low pressure methane steam reforming in a Pd–Ag membrane reactor over a Ni-based catalyst: experimental and modeling. Int J Hydrogen Energy 35:11514–11524

    Article  CAS  Google Scholar 

  9. Matsumura Y, Nakamori T (2004) Steam reforming of methane over nickel catalysts at low reaction temperature. Appl Catal 258:107–114

    Article  CAS  Google Scholar 

  10. Chin Y-H, King D, Roh H-S, Wang Y, Heald SM (2006) Structure and reactivity investigations on supported bimetallic Au–Ni catalysts used for hydrocarbon steam reforming. J Catal 244:153–162

    Article  CAS  Google Scholar 

  11. Parizotto NV, Rocha KO, Damyanova S, Passos FB, Zanchet D, Marques CMP et al (2007) Alumina supported Ni catalysts modified with silver for the steam reforming of methane: effect of Ag on the control of coke formation. Appl Catal A 330:12–22

    Article  CAS  Google Scholar 

  12. Parizotto NV, Fernandez RF, Marques CMP, Bueno JMC (2007) Promoter effect of Ag and La on stability of Ni/Al2O3 catalysts in reforming of methane processes. Stud Sci Surf Catal 167:421–426

    Article  CAS  Google Scholar 

  13. Triantafyllopoulos NC, Neophytides SG (2006) Dissociative adsorption of CH4 on NiAu/YSZ: the nature of adsorbed carbonaceous species and the inhibition of graphitic C formation. J Catal 239:187–199

    Article  CAS  Google Scholar 

  14. Araujo JCS, Zanchet D, Rinaldi R, Schuchardt U, Hori CE, Fiero JLG, Bueno JMC (2008) The effects of La2O3 on the structural properties of La2O3–Al2O3 prepared by sol–gel method and on the catalytic performance of Pt/La2O3–Al2O3 towards steam reforming and partial oxidation of methane. Appl Catal B 84:552–562

    Article  CAS  Google Scholar 

  15. Cassinelli WH, Feio LSF, Araujo JCS, Hori CE, Noronha FB, Marques CMP et al (2008) Effect of CeO2 and La2O3 on the activity of CeO2–La3O3/Al2O3 supported Pd catalysts for steam reforming of methane. Catal Lett 120:86–94

    Article  CAS  Google Scholar 

  16. Yang R, Xing C, Lv C, Shi L, Tsubaki N (2010) Promotional effect of La2O3 and CeO2 an Ni/γ-Al2O3 catalysts for CO2 reforming of CH4. Appl Catal A 385:92–100

    Article  Google Scholar 

  17. Chen J, Wang R, Zhang J, He F, Han S (2005) Effects of preparation methods on properties of Ni/CeO2–Al2O3 catalysts for methane reforming with carbon dioxide. J Mol Catal A 235:302–310

    Article  CAS  Google Scholar 

  18. Koo KY, Roh HS, Jung UH, Yoon WL (2009) CeO2 promoted Ni/Al2O3 catalyst in combined steam and carbon dioxide reforming of methane for gas to liquid (GTL) process. Catal Lett 130:217–221

    Article  CAS  Google Scholar 

  19. Zhuang Q, Qin Y, Chang L (1991) Promoting effect of cerium oxide in supported nickel catalysts for hydrocarbon steam reforming. Appl Catal 70:1–8

    Article  CAS  Google Scholar 

  20. Seo JG, Youn MH, Bang Y, song IK (2011) Hydrogen production by steam reforming of simulated liquefied natural gas (LNG) over mesoporous nickel–M–alumina (M = Ni, Ce, La, Y, Cs, Fe, Co and Mg) aerogel catalysts. Int J Hydrogen Energy 36:3505–3514

    Article  CAS  Google Scholar 

  21. Xu J, Zhou W, Wang J, Li Z, Ma J (2009) Characterization and analysis of carbon deposited during the dry reforming of methane over Ni/La2O3/Al2O3 catalysts. Chin J Catal 30:1076–1084

    Article  CAS  Google Scholar 

  22. Lazar MD, Dan M, Mihet M, Almasan V, Rednic V, Borodi G (2011) Hydrogen production by low temperature methane steam reforming using Ag and Au modified alumina supported nickel catalysts. Rev Roum Chim 56(6):637–642

    CAS  Google Scholar 

  23. Dan M, Lazar MD, Rednic V, Almasan V (2011) Methane steam reforming over Ni/Al2O3 promoted by CeO2 and La2O3. Rev Roum Chim 56(6):643–649

    CAS  Google Scholar 

  24. Froment GF, Bischoff KB (1990) Chemical reactor analysis and design, 2nd edn. Willey, New York

    Google Scholar 

  25. Kuemmerle EA, Heger GJ (1999) The structures of C–Ce2O3+δ, Ce7O12 and Ce11O20. J Solid State Chem 147:485–500

    Article  Google Scholar 

  26. Sanchez-Sanchez MC, Navarro RM, Fierro JLG (2007) Ethanol steam reforming over Ni/La–Al2O3 catalysts: influence on lanthanum loading. Catal Today 129:336–345

    Article  CAS  Google Scholar 

  27. Scheffer B, Molhoek P, Moulijn JA (1989) Temperature programmed reduction of NiO–WO3/Al2O3 hydrodesulphurization catalyst. Appl Catal 46:11–17

    Article  CAS  Google Scholar 

  28. Maniecki TP, Stadnichenko AI, Maniukievich W, Bawolak K, Mierczynski P, Boronin AI, Jozviak WK (2010) An active phase transformation of surface Ni–Au/Al2O3 catalyst during partial oxidation of methane to synthesis gas. Kinet Catal 51:573–578

    Article  CAS  Google Scholar 

  29. Li C, Chen YW (1995) Temperature programmed reduction studies of nickel oxide/alumina catalysts: effects of the preparation methods. Thermochim Acta 256:457–462

    Article  CAS  Google Scholar 

  30. Lu Z, Guo Y, Zhang Q, Yagi M, Hatakeyama J, Li H, Chen J, Sakurai M, Karneyama H (2008) A novel catalyst with plate-type anodic alumina supports, Ni/NiAl2O4/γ-Al2O3/alloy, for steam reforming of methane. Appl Catal A 347:200–207

    Article  Google Scholar 

  31. Holmblad PM, Hvolbaek Larsen J, Chorkendorff I (1996) Modification of Ni(111) reactivity toward CH4, CO, and D2 by two dimensional alloying. J Chem Phys 104:7289–7296

    Article  CAS  Google Scholar 

  32. Craciun R, Shereck B, Gorte RJ (1998) Kinetic studies of methane steam reforming on ceria-supported Pd. Catal Lett 51:149–153

    Article  CAS  Google Scholar 

  33. Zhang ZL, Verykios XE (1994) Carbon dioxide reforming of methane to synthesis gas over supported Ni catalysts. Catal Today 21:589–595

    Article  CAS  Google Scholar 

  34. Aparicio LM (1997) Transient isotopic studies and microkinetic modeling of methane reforming over nickel catalysts. J Catal 165(2):262–274

    Article  CAS  Google Scholar 

Download references

Acknowledgments

This research was supported by the Romanian ANCS Department: PN II Program under contract 21004/2007.

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Authors and Affiliations

  1. National Institute for Research and Development of Isotopic and Molecular Technologies, 65-103 Donath Street, 400293, Cluj-Napoca, Romania

    Monica Dan, Maria Mihet, Alexandru R. Biris, Petru Marginean, Valer Almasan, George Borodi & Mihaela D. Lazar

  2. Applied Science Department, UALR Nanotechnology Center, University of Arkansas at Little Rock, Little Rock, AR, 72204, USA

    Fumiya Watanabe & Alexandru S. Biris

Authors
  1. Monica Dan
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  2. Maria Mihet
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  3. Alexandru R. Biris
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  4. Petru Marginean
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  5. Valer Almasan
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  7. Fumiya Watanabe
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  9. Mihaela D. Lazar
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Correspondence to Mihaela D. Lazar.

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Dan, M., Mihet, M., Biris, A.R. et al. Supported nickel catalysts for low temperature methane steam reforming: comparison between metal additives and support modification. Reac Kinet Mech Cat 105, 173–193 (2012). https://doi.org/10.1007/s11144-011-0406-0

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