Experimental and Theoretical Study of the Interactions between Fe 2 O 3 /Al 2 O 3 and CO

The behavior of Fe 2 O 3 /Al 2 O 3 particles as oxygen carriers (OCs) for CO chemical looping combustion (CLC) under different reaction temperatures (700 °C, 800 °C, 900 °C, and 1000 °C) were tested in a lab-scale fluidized bed and a thermogravimetric analysis (TGA) unit. The results show that the oxygen carrier presents the highest reactivity at 800 °C, even after 30 cycles of redox reaction in a fluidized bed, while more obvious carbon deposition occurred for the case at 700 °C, and agglomeration for the case at 1000 °C. Moreover, the detailed behavior of the prepared Fe 2 O 3 /Al 2 O 3 particle was detected in the TGA apparatus at different reaction temperatures. Furthermore, temperature-programming TGA experiments were performed to investigate the influence of different CO concentrations and CO/CO 2 concentrations on the reaction between CO and OC during the chemical looping combustion processes. Based on these experimental behaviors of the prepared Fe 2 O 3 /Al 2 O 3 during the CLC of CO, the detailed models and electronic properties of the pure and reduced Fe 2 O 3 /Al 2 O 3 supported the slabs, CO adsorption, and oxidation, and the decomposition reactions on these surfaces were revealed using density functional theory (DFT) calculations which went deep into the nature of the synergetic effect of the support of Al 2 O 3 on the activity of Fe 2 O 3 for the CLC of CO.

[1]  Hua Wang,et al.  Direct conversion of methane to synthesis gas using lattice oxygen of CeO2–Fe2O3 complex oxides , 2010 .

[2]  Yongping Yang,et al.  Deep reduction behavior of iron oxide and its effect on direct CO oxidation , 2012 .

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

[4]  S. Bhattacharya,et al.  Use of Pyrite Cinder as an Iron-Based Oxygen Carrier in Coal-Fueled Chemical Looping Combustion , 2015 .

[5]  R. Moliner,et al.  Thermo catalytic decomposition of methane over Ni-Mg and Ni-Cu-Mg catalysts Effect of catalyst preparation method , 2007 .

[6]  Anders Lyngfelt,et al.  Chemical-looping with oxygen uncoupling using combined Mn-Fe oxides, testing in batch fluidized bed , 2011 .

[7]  N. Cai,et al.  AFM investigation of solid product layers of MgSO4 generated on MgO surfaces for the reaction of MgO with SO2 and O2 , 2011 .

[8]  Juan Adánez,et al.  Development of Cu-based oxygen carriers for chemical-looping combustion , 2004 .

[9]  Ming Luo,et al.  Reduction kinetics of iron-based oxygen carriers using methane for chemical-looping combustion , 2014 .

[10]  C. Dong,et al.  Reduction effect of α-Fe2O3 on carbon deposition and CO oxidation during chemical-looping combustion , 2016 .

[11]  Jun Xiao,et al.  Analysis of reactivity of Fe-based oxygen carrier with coal during chemical-looping combustion , 2009 .

[12]  Laihong Shen,et al.  Experimental investigation of hematite oxygen carrier decorated with NiO for chemical looping combustion of coal , 2012 .

[13]  White,et al.  Implementation of gradient-corrected exchange-correlation potentials in Car-Parrinello total-energy calculations. , 1994, Physical review. B, Condensed matter.

[14]  Lixia Ling,et al.  A density functional theory study on the interaction mechanism between H2S and the α-Fe2O3(0001) surface , 2013 .

[15]  A. Abad,et al.  Performance of a highly reactive impregnated Fe2O3/Al2O3 oxygen carrier with CH4 and H2S in a 500 Wth CLC unit , 2014 .

[16]  Surface structures of Fe3O4 (111), (110), and (001): A density functional theory study , 2010 .

[17]  B. Moghtaderi,et al.  Comprehensive Study of Fe2O3/Al2O3 Reduction with Ultralow Concentration Methane under Conditions Pertinent to Chemical Looping Combustion , 2015 .

[18]  N. Govind,et al.  A generalized synchronous transit method for transition state location , 2003 .

[19]  Oxygen release kinetics and mechanism study on Cu-, Co-, Mn-based oxygen carrier , 2013 .

[20]  A. Thursfield,et al.  La0.6Sr0.4Co0.2Fe0.8O3−δ microtubular membranes for hydrogen production from water splitting , 2012 .

[21]  Juan Adánez,et al.  Syngas combustion in a Chemical-Looping Combustion system using an impregnated Ni-based oxygen carrier , 2008 .

[22]  Beatriz Fidalgo,et al.  CO2 reforming of coke oven gas over a Ni/γAl2O3 catalyst to produce syngas for methanol synthesis , 2012 .

[23]  N. Cai,et al.  Interaction between Fe-based oxygen carriers and n-heptane during chemical looping combustion , 2013 .

[24]  A. Abad,et al.  Testing of a highly reactive impregnated Fe2O3/Al2O3 oxygen carrier for a SR–CLC system in a continuous CLC unit , 2012 .

[25]  C. Dong,et al.  Density functional theory study on activity of α-Fe2O3 in chemical-looping combustion system , 2011 .

[26]  C. Zheng,et al.  Characterization and evaluation of Fe2O3/Al2O3 oxygen carrier prepared by sol–gel combustion synthesis , 2011 .

[27]  K. Zhao,et al.  Thermodynamic analysis and thermogravimetric investigation on chemical looping gasification of biomass char under different atmospheres with Fe2O3 oxygen carrier , 2015 .

[28]  Juan Adánez,et al.  Progress in chemical-looping combustion and reforming technologies , 2012 .

[29]  Possibility of Morphological Control To Improve the Activity of Oxygen Carriers for Chemical Looping Combustion , 2015 .

[30]  J. Chaouki,et al.  TGA and kinetic modelling of Co, Mn and Cu oxides for chemical looping gasification (CLG) , 2014 .

[31]  Xingfu Song,et al.  Density Functional Theory Study on the Mechanism of Calcium Sulfate Reductive Decomposition by Carbon Monoxide , 2012 .

[32]  Malcolm L. H. Green,et al.  A study of carbon deposition on catalysts during the partial oxidation of methane to synthesis gas , 1993 .

[33]  A. Kierzkowska,et al.  Development of Iron Oxide Carriers for Chemical Looping Combustion Using Sol−Gel , 2010 .

[34]  Activity of Fe2O3 with a high index facet for bituminous coal chemical looping combustion: a theoretical and experimental study , 2016 .

[35]  Juan Adánez,et al.  Operation of a 10 kWth chemical-looping combustor during 200 h with a CuO-Al2O3 oxygen carrier , 2007 .

[36]  Maohong Fan,et al.  Progress in oxygen carrier development of methane-based chemical-looping reforming: A review , 2015 .

[37]  Q. Guo,et al.  Preparation and Characterization of Fe2O3/Al2O3 Using the Solution Combustion Approach for Chemical Looping Combustion , 2012 .

[38]  M. I. Pariente,et al.  Assessment of Fe2O3/SiO2 catalysts for the continuous treatment of phenol aqueous solutions in a fixed bed reactor , 2010 .

[39]  M. Rahimpour,et al.  Calcium promoted Fe/Al2O3 oxygen carrier for hydrogen production via cyclic chemical looping steam methane reforming process , 2015 .

[40]  C. Zheng,et al.  Chemical looping combustion of a Chinese anthracite with Fe2O3-based and CuO-based oxygen carriers , 2012 .

[41]  Mohammad. M. Hossain,et al.  Cu‐based mixed metal oxide catalysts for WGSR: Reduction kinetics and catalytic activity , 2013 .

[42]  B. Moghtaderi,et al.  Reduction Kinetics of Fe2O3/Al2O3 by Ultralow Concentration Methane under Conditions Pertinent to Chemical Looping Combustion , 2015 .

[43]  Wang,et al.  Accurate and simple analytic representation of the electron-gas correlation energy. , 1992, Physical review. B, Condensed matter.

[44]  Ivar M. Dahl,et al.  On the development of novel reactor concepts for chemical looping combustion , 2009 .

[45]  Anders Lyngfelt,et al.  Chemical-looping with oxygen uncoupling using CuO/ZrO2 with petroleum coke , 2009 .