Chemical Looping Dry Reforming as Novel, Intensified Process for CO2 Activation

Chemical looping dry reforming (CLDR) is a novel, intensified route for CO2 activation. Two nanostructured carriers (Fe-BHA and Fe@SiO2) are synthesized, characterized, and evaluated with regard to activity and stability in thermogravimetric and fixed-bed CLDR reactor studies over a temperature range of ~500–800 °C. Fe-barium hexaaluminate (Fe-BHA) shows fast redox kinetics and stable operation over multiple CLDR cycles, while Fe@SiO2 exhibits poor activity for CO generation due to a partial loss of the core-shell structure and formation of silicates. While the latter could be removed via a two-step oxidation scheme, carrier utilization remained well below that of Fe-BHA (~ 51 % versus ~ 15 %). However, the two-step oxidation configuration turns the net endothermic CLDR process into a net exothermic process, opening up a highly efficient autothermal process alternative.

[1]  Rahul Solunke,et al.  Nanocomposite oxygen carriers for chemical-looping combustion of sulfur-contaminated synthesis gas , 2009 .

[2]  Hongguang Jin,et al.  A NEW ADVANCED POWER-GENERATION SYSTEM USING CHEMICAL-LOOPING COMBUSTION , 1994 .

[3]  A. Lyngfelt,et al.  A fluidized-bed combustion process with inherent CO2 separation; Application of chemical-looping combustion , 2001 .

[4]  A. Lyngfelt,et al.  The use of iron oxide as an oxygen carrier in chemical-looping combustion of methane with inherent separation of CO2 , 2001 .

[5]  Todd H. Gardner,et al.  Carbon capture and utilization via chemical looping dry reforming , 2011 .

[6]  A. Cao,et al.  Stabilizing metal nanoparticles for heterogeneous catalysis. , 2010, Physical chemistry chemical physics : PCCP.

[7]  Rahul Solunke,et al.  Integrating desulfurization with CO2-capture in chemical-looping combustion , 2011 .

[8]  Peter G. Loutzenhiser,et al.  CO2 Splitting via Two-Step Solar Thermochemical Cycles with Zn/ZnO and FeO/Fe3O4 Redox Reactions II: Kinetic Analysis , 2008 .

[9]  G. Somorjai,et al.  Thermally stable Pt/mesoporous silica core-shell nanocatalysts for high-temperature reactions. , 2009, Nature materials.

[10]  Mohammad. M. Hossain,et al.  Chemical-looping combustion (CLC) for inherent CO2 separations—a review , 2008 .

[11]  A. Lyngfelt,et al.  Comparison of iron-, nickel-, copper- and manganese-based oxygen carriers for chemical-looping combustion , 2004 .

[12]  H. Arai,et al.  Thermal stabilization of catalyst supports and their application to high-temperature catalytic combustion , 1996 .

[13]  Marie Anheden,et al.  Exergy analysis of chemical-looping combustion systems , 1998 .

[14]  Tobias Mattisson,et al.  Integrated hydrogen and power production with CO2 capture using chemical-looping reforming-redox reactivity of particles of CuO, Mn 2O3, NiO, and Fe2O3 using SiO 2 as a support , 2005 .

[15]  K. Eguchi,et al.  Effect of additives on the surface area of oxide supports for catalytic combustion , 1986 .

[16]  Liang-Shih Fan,et al.  Syngas Redox (SGR) Process to Produce Hydrogen from Coal Derived Syngas , 2007 .

[17]  L. Fan,et al.  Calcium Looping Process (CLP) for Enhanced Noncatalytic Hydrogen Production with Integrated Carbon Dioxide Capture , 2010 .

[18]  Olav Bolland,et al.  A quantitative comparison of gas turbine cycles with CO2 capture , 2007 .

[19]  S. D. Kim,et al.  Reaction kinetics of reduction and oxidation of metal oxides for hydrogen production , 2008 .

[20]  G. Veser,et al.  Hydrogen Production via Chemical Looping Steam Reforming in a Periodically Operated Fixed-Bed Reactor , 2010 .

[21]  Alan W. Weimer,et al.  Likely near-term solar-thermal water splitting technologies , 2004 .

[22]  T. Engelder,et al.  Natural gas: Should fracking stop? , 2011, Nature.

[23]  Jens Wolf,et al.  Comparison of nickel- and iron-based oxygen carriers in chemical looping combustion for CO2 capture in power generation , 2005 .

[24]  M. Kirchhoff,et al.  Engineering high-temperature stable nanocomposite materials , 2005, Nanotechnology.

[25]  Xiaoming Zheng,et al.  Production of synthesis gas via methane reforming with CO2 on noble metals and small amount of noble-(Rh-) promoted Ni catalysts , 2006 .

[26]  Sotiris E. Pratsinis,et al.  Hydrothermal stability of pure and modified microporous silica membranes , 1995, Journal of Materials Science.

[27]  Jin-Hong Kim,et al.  Effect of metal particle size on coking during CO2 reforming of CH4 over Ni–alumina aerogel catalysts , 2000 .

[28]  Jens Wolf,et al.  Part-load analysis of a chemical looping combustion (CLC) combined cycle with CO2 capture , 2007 .

[29]  E. Tanabe,et al.  Specific performance of silica-coated Ni catalysts for the partial oxidation of methane to synthesis gas , 2007 .

[30]  A. Steinfeld Solar hydrogen production via a two-step water-splitting thermochemical cycle based on Zn/ZnO redox reactions , 2002 .

[31]  G. Veser,et al.  Supported nanocomposite catalysts for high-temperature partial oxidation of methane , 2008 .

[32]  M. Schmal,et al.  Study of Ni and Pt catalysts supported on α-Al2O3 and ZrO2 applied in methane reforming with CO2 , 2007 .

[33]  Subhash Bhatia,et al.  Catalytic Technology for Carbon Dioxide Reforming of Methane to Synthesis Gas , 2009 .

[34]  W. Chueh,et al.  High-Flux Solar-Driven Thermochemical Dissociation of CO2 and H2O Using Nonstoichiometric Ceria , 2010, Science.