Efficient catalytic abatement of greenhouse gases: Methane reforming with CO2 using a novel and thermally stable Rh–CeO2 catalyst

Abstract 2% Rh–CeO 2 catalyst was synthesized using the hard template method and characterized by means of N 2 adsorption/desorption, XRD and H 2 -TPR methods. The prepared powdered catalyst exhibited high thermal stability and high surface area with negligible sintering during 24-h exposure to 973 K in an inert atmosphere. During the temperature programmed methane dry reforming reaction between 473 and 1073 K, an increase in the molar H 2 /CO ratio from 0.3 at 623 K to as high as 0.96 at 1073 K was observed. Besides H 2 and CO, H 2 O was identified among reaction products, originating from the simultaneously occurring reverse water-gas shift reaction. During the isothermal test performed at 923 K, the 2% Rh–CeO 2 catalyst exhibited stable performance and produced syngas with the average H 2 /CO ratio equal to 0.62. A relative drop of catalyst activity equal to 11% was observed within 70-h time on stream at 1023 K, with the average H 2 /CO ratio at the reactor outlet equal to 0.71.

[1]  J. R. Rostrup-Nielsen,et al.  Aspects of CO2-reforming of Methane , 1994 .

[2]  D. Zhao,et al.  Fast preparation of highly ordered nonsiliceous mesoporous materials via mixed inorganic precursors. , 2002, Chemical communications.

[3]  A. Veen,et al.  Autothermal reforming of ethanol for hydrogen production over an Rh/CeO2 catalyst , 2008 .

[4]  Y. Schuurman,et al.  A transient kinetic study of the carbon dioxide reforming of methane over supported Ru catalysts , 1999 .

[5]  Hengyong Xu,et al.  Role of redox couples of Rh0/Rhδ+ and Ce4+/Ce3+ in CH4/CO2 reforming over Rh–CeO2/Al2O3 catalyst , 2006 .

[6]  A. Pintar,et al.  TPR, TPO, and TPD examinations of Cu0.15Ce0.85O(2-y) mixed oxides prepared by co-precipitation, by the sol-gel peroxide route, and by citric acid-assisted synthesis. , 2005, Journal of colloid and interface science.

[7]  T. Uchijima,et al.  Role of support in reforming of CH4 with CO2 over Rh catalysts , 1994 .

[8]  Qianer Zhang,et al.  Dissociation of methane on different transition metals , 1998 .

[9]  R. Ryoo,et al.  Synthesis of thermally stable mesoporous cerium oxide with nanocrystalline frameworks using mesoporous silica templates. , 2003, Chemical communications.

[10]  F. Kleitz,et al.  Design of Mesoporous Silica at Low Acid Concentrations in Triblock Copolymer-Butanol-Water Systems , 2005 .

[11]  Janez Levec,et al.  Comparison of water–gas shift reaction activity and long-term stability of nanostructured CuO-CeO2 catalysts prepared by hard template and co-precipitation methods , 2009 .

[12]  Yanhui Yang,et al.  Carbon dioxide reforming of methane to synthesis gas over Ni-MCM-41 catalysts , 2009 .

[13]  A. Trovarelli,et al.  Catalytic Properties of Ceria and CeO2-Containing Materials , 1996 .

[14]  M. Ocsachoque,et al.  Role of CeO2 in Rh/α-Al2O3 Catalysts for CO2 Reforming of Methane , 2011 .

[15]  S. Yaşyerli,et al.  Ru incorporated Ni–MCM-41 mesoporous catalysts for dry reforming of methane: Effects of Mg addition, feed composition and temperature , 2011 .

[16]  J. Bitter,et al.  The state of Zirconia Suported Platinum Catalysts for CO2/CH4 Reforming , 1997 .

[17]  V. Perrichon,et al.  Reversibility of hydrogen chemisorption on a ceria-supported rhodium catalyst , 1992 .

[18]  J. White,et al.  Temperature-programmed desorption of carbon monoxide and carbon dioxide from platinum/ceria: an important role for lattice oxygen in carbon monoxide oxidation , 1987 .

[19]  Shaobin Wang,et al.  Role of CeO2 in Ni/CeO2–Al2O3 catalysts for carbon dioxide reforming of methane , 1998 .

[20]  J. Lapszewicz,et al.  Study of mixed steam and CO2 reforming of CH4 to syngas on MgO-supported metals , 1994 .

[21]  Wojciech M. Budzianowski,et al.  Negative Net CO2 Emissions from Oxy-Decarbonization of Biogas to H2 , 2010 .

[22]  Tae-Wan Kim,et al.  MCM-48-like large mesoporous silicas with tailored pore structure: facile synthesis domain in a ternary triblock copolymer-butanol-water system. , 2005, Journal of the American Chemical Society.

[23]  J. Richardson,et al.  Carbon dioxide reforming with Rh and Pt–Re catalysts dispersed on ceramic foam supports , 2003 .

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

[25]  O. Levenspiel Chemical Reaction Engineering , 1972 .

[26]  Wuzong Zhou,et al.  Preparation of three-dimensional chromium oxide porous single crystals templated by SBA-15. , 2003, Chemical communications.

[27]  Hai-Yan Wang,et al.  Nano-MgO: novel preparation and application as support of Ni catalyst for CO2 reforming of methane , 2001 .

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

[29]  M. Soria,et al.  Thermodynamic and experimental study of combined dry and steam reforming of methane on Ru/ ZrO2-La2O3 catalyst at low temperature , 2011 .

[30]  Jacob A. Moulijn,et al.  Mitigation of CO2 by Chemical Conversion: Plausible Chemical Reactions and Promising Products , 1996 .

[31]  M. Patterson,et al.  The effect of carbon monoxide on the oxidation of four C6 to C8 hydrocarbons over platinum, palladium and rhodium , 2000 .

[32]  Jiqing Lu,et al.  High-surface area CuO-CeO2 catalysts prepared by a surfactant-templated method for low-temperature CO oxidation , 2007 .

[33]  J. Longanbach,et al.  A Perspective on Syngas from Coal , 1991 .

[34]  Yutaka Nakashimada,et al.  Recent development of anaerobic digestion processes for energy recovery from wastes. , 2007, Journal of bioscience and bioengineering.

[35]  J. Fierro,et al.  Hydrogen production reactions from carbon feedstocks: fossil fuels and biomass. , 2007, Chemical reviews.

[36]  Eva Pongrácz,et al.  Catalytic activation of CO2: Use of secondary CO2 for the production of synthesis gas and for methanol synthesis over copper-based zirconia-containing catalysts , 2009 .

[37]  M. Bradford,et al.  Catalytic reforming of methane with carbon dioxide over nickel catalysts II. Reaction kinetics , 1996 .

[38]  Wojciech M. Budzianowski,et al.  An oxy-fuel mass-recirculating process for H2 production with CO2 capture by autothermal catalytic oxyforming of methane , 2010 .