Influence of method of preparation on the activity of La-Ni-Ce mixed oxide catalysts for dry reforming of methane†

La–Nix–Ce1−x mixed oxide catalysts were prepared by a sol–gel method varying the Ni composition (0 ≤ x ≤ 1). The catalysts were characterized by X-ray diffraction (XRD), inductively coupled plasma optical emission spectroscopy (ICP-OES), BET surface area, X-ray photoelectron spectroscopy (XPS), temperature-programmed reduction (TPR), H2 chemisorption and Fourier transform infrared spectroscopy (FT-IR) techniques. CO2 reforming of methane was carried out at atmospheric pressure and 800 °C, maintaining a reactant CO2/CH4/N2 ratio of 80/80/80 (total flow rate = 240 ml min−1, GHSV of 28800 h−1). The catalysts offered higher activity even at lower Ni compositions. LaNi0.4Ce0.6O3. showed the highest conversion of CH4 and CO2. The H2/CO ratio in the syngas was stable at 0.85 ± 0.02. The performance of the sol–gel catalysts was compared with that of the hydrothermally prepared catalysts, reported earlier. High surface area and better Ni dispersion were found to be the reasons for superior activity of the sol–gel catalysts.

[1]  B. M. Reddy,et al.  Nano-Au/CeO2 catalysts for CO oxidation: Influence of dopants (Fe, La and Zr) on the physicochemical properties and catalytic activity , 2014 .

[2]  Sudarno,et al.  CeO2–SiO2 supported nickel catalysts for dry reforming of methane toward syngas production , 2013 .

[3]  A. Vinu,et al.  Nanocrystalline Ce1−xSmxO2−δ (x = 0.4) solid solutions: structural characterization versus CO oxidation , 2013 .

[4]  G. Moradi,et al.  Effects of Partial Substitution of Ni by Cu in LaNiO3 Perovskite Catalyst for Dry Methane Reforming , 2012 .

[5]  C. Pirez,et al.  Highly efficient and stable CeNiH(Z)O(Y) nano-oxyhydride catalyst for H2 production from ethanol at room temperature. , 2011, Angewandte Chemie.

[6]  Hua Wang,et al.  Preparation and characterization of Ce1-x NixO2 as oxygen carrier for selective oxidation methane to syngas in absence of gaseous oxygen , 2010 .

[7]  H. Arandiyan,et al.  Effects of Lanthanum Substitution by Strontium and Calcium in La-Ni-Al Perovskite Oxides in Dry Reforming of Methane , 2008 .

[8]  F. Mondragón,et al.  CO2 reforming of methane over Ni-Mg-Al-Ce mixed oxides derived from hydrotalcites: Mg/Ni ratio effect , 2008 .

[9]  J. Mawdsley,et al.  Rare earth-first-row transition metal perovskites as catalysts for the autothermal reforming of hydrocarbon fuels to generate hydrogen , 2008 .

[10]  A. Salker,et al.  Preparation, characterization and catalytic CO oxidation studies on LaNi1−xCoxO3 system , 2007 .

[11]  Xiaolai Wang,et al.  Catalytic performances of NiO–CeO2 for the reforming of methane with CO2 and O2 , 2006 .

[12]  J. Assaf,et al.  Structural features of La1-xCexNiO3 mixed oxides and performance for the dry reforming of methane , 2006 .

[13]  Suttichai Assabumrungrat,et al.  Catalytic dry reforming of methane over high surface area ceria , 2005 .

[14]  S. Assabumrungrat,et al.  Synthesis gas production from dry reforming of methane over CeO2 doped Ni/Al2O3: Influence of the doping ceria on the resistance toward carbon formation , 2005 .

[15]  S. C. Dhingra,et al.  K-, CeO2-, and Mn-promoted Ni/Al2O3 catalysts for stable CO2 reforming of methane , 2005 .

[16]  Shudong Wang,et al.  La-Ce-Ni-O monolithic perovskite catalysts potential for gasoline autothermal reforming system , 2005 .

[17]  Hyun-Seog Roh,et al.  Comparative Study on Partial Oxidation of Methane over Ni/ZrO2, Ni/CeO2 and Ni/Ce–ZrO2 Catalysts , 2002 .

[18]  Lidia Pino,et al.  Catalytic partial-oxidation of methane on a ceria-supported platinum catalyst for application in fuel cell electric vehicles , 2002 .

[19]  M. A. Peña,et al.  Chemical structures and performance of perovskite oxides. , 2001, Chemical reviews.

[20]  Antonio Monzón,et al.  Methane reforming with CO2 over Ni/ZrO2–CeO2 catalysts prepared by sol–gel , 2000 .

[21]  A. Kiennemann,et al.  Characterisation of the solid solution La(Ni,Fe)O3 prepared via a sol-gel related method using propionic acid , 1999 .

[22]  Malcolm L. H. Green,et al.  Recent advances in the conversion of methane to synthesis gas , 1995 .

[23]  L. Schmidt,et al.  Comparison of monolith-supported metals for the direct oxidation of methane to syngas , 1994 .

[24]  R. Burch,et al.  Investigation of the synthesis of oxygenates from carbon monoxide/hydrogen mixtures on supported rhodium catalysts , 1992 .

[25]  L. Haack,et al.  Characterization of high-temperature calcined lanthanum-modified alumina by X-ray photoelectron spectroscopy and X-ray diffraction , 1992 .

[26]  F. Solymosi,et al.  Catalytic reaction of CH4 with CO2 over alumina-supported Pt metals , 1991 .

[27]  J. Fierro.  STRUCTURE AND COMPOSITION OF PEROVSKITE SURFACE IN RELATION TO ADSORPTION AND CATALYTIC PROPERTIES , 1990 .

[28]  P. Ganguly,et al.  Infrared and Mössbauer spectroscopic study of the metal-insulator transition in some oxides of perovskite structure☆ , 1986 .