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1.
  • Cho, Paul, 1970-, et al. (författare)
  • Carbon Formation on Nickel and Iron Oxide-Containing Oxygen Carriers for Chemical-Looping Combustion
  • 2005
  • Ingår i: Industrial & Engineering Chemistry Research. - 0888-5885. ; 44:4, s. 668-676
  • Tidskriftsartikel (refereegranskat)abstract
    • For combustion with CO2 capture, chemical-looping combustion with inherent separation of CO2 is a promising technology. Two interconnected fluidized beds are used as reactors. In the fuel reactor, a gaseous fuel is oxidized by an oxygen carrier, e.g., metal oxide particles, producing carbon dioxide and water. The reduced oxygen carrier is then transported to the air reactor, where it is oxidized with air back to its original form before it is returned to the fuel reactor. Carbon deposition on oxygen-carrier particles was investigated to assess whether it could have adverse effects on the process. The oxygen-carrier particles used were based on oxides of nickel and iron and produced by freeze granulation. They were sintered at 1300 degreesC for 4 h and sieved to a size range of 125-180 mum. The study of carbon deposition was performed in a laboratory fluidized-bed reactor, simulating a chemical-looping combustion system by exposing the sample to alternating reducing and oxidizing conditions. The particles with nickel oxide were tested at 750, 850, and 950 degreesC, and the particles with iron oxide at 950 degreesC. On the oxygen carrier with nickel oxide, only minor amounts of carbon formed during most of the reduction. However, when more than 80% of the oxygen available was consumed, significant carbon formation started. The formation of carbon was also clearly correlated to low conversion of the fuel. No carbon was formed on the oxygen carrier based on iron oxide. The interpretation for the actual application of this process is that carbon formation should not be a problem, because the process should be run under conditions of high conversions of the fuel.
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3.
  • Cho, Paul, 1970-, et al. (författare)
  • Defluidization conditions for fluidized-bed of iron, nickel, and manganese oxide containing oxygen-carriers for chemical-looping combustion
  • 2006
  • Ingår i: Industrial & Engineering Chemistry Research. - 0888-5885. ; 45:3, s. 968-977
  • Tidskriftsartikel (refereegranskat)abstract
    • For combustion with CO2 capture, chemical-looping combustion with inherent separation Of CO2 is a promising technology. Chemical-looping combustion uses oxygen carriers that are composed of metal oxide to transfer oxygen from the combustion air to the fuel. The defluidization of oxygen-carrier particles was investigated to improve the understanding of when particle agglomeration may occur. The study was made in a laboratory fluidized-bed reactor at 950 degrees C, simulating a chemical-looping combustion system by exposing the sample to reducing and oxidizing conditions in an alternating manner. The oxygen-carrier particles used were based on oxides of iron, nickel, and manganese and produced by freeze granulation. For iron oxide particles, there was no defluidization of the bed when the content of available oxygen in the particle was high. The defluidization occurred during the oxidation period after long reduction periods, in which a significant reduction of the magnetite to wustite occurred. This is an important observation, because the reduction to wustite is not expected in chemical-looping combustion with high fuel conversion. Thus, laboratory experiments with iron oxide performed with long reduction times may give an unduly exaggerated impression of the risks of agglomeration. For nickel oxide, the defluidization was dependent on the sintering temperature with no defluidization in experiments conducted with particles sintered at 1300 and 1400 degrees C. The nickel oxide particles that were sintered at 1500 degrees C only defluidized once in a total of 49 cycles, whereas the particles that were sintered at 1600 degrees C defluidized already in the first cycle. For the nickel oxide particles, it was not possible to see any effect of the length of the reducing period on the defluidization. There was no defluidization of the manganese oxide particles. The defluidization of the bed leads to agglomeration for the iron oxide particles, but not for the particles of nickel oxide, where the bed was still loosely packed. Carbon was formed on the particles based on nickel oxide and manganese oxide.
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9.
  • Arjmand, Mehdi, 1986-, et al. (författare)
  • CaxLa1−xMn1−yMyO3−δ (M = Mg, Ti, Fe or Cu) as Oxygen Carriers for Chemical-Looping with Oxygen Uncoupling (CLOU)
  • 2013
  • Ingår i: Energy & Fuels. - 0887-0624. ; DOI: 10.1021/ef3020102
  • Tidskriftsartikel (refereegranskat)abstract
    • Perovskite materials of the type CaxLa1−xMn1−yMyO3−δ (M = Mg, Ti, Fe or Cu) have been investigated as oxygen carriers for the chemical-looping with oxygen uncoupling (CLOU) process. The oxygen carrier particles were produced by mechanical homogenization of primary solids in a rotary evaporator followed by extrusion and calcination at 1300°C for 6 h. The chemical-looping characteristics of the substituted perovskites developed in this work were evaluated in a laboratory-scale fluidized-bed reactor in the temperature range of 900−1000°C during alternating reducing and oxidizing conditions. The oxygen carriers showed oxygen releasing behaviour (CLOU) in inert atmosphere between 900−1000°C. In addition, their reactivity with methane was high, approaching complete gas yield for all of the materials at 950°C, the exception being the Cu-doped perovskite which defluidized during reduction. The rates of oxygen release were also investigated using devolatilized wood char as solid fuel, and were found to be similar. The required solids inventory in the fuel reactor for the perovskite oxygen carriers is estimated to be 325 kg/MWth. All of the formulations exhibited high rates of oxidation and high degree of stability with no particle fragmentation or agglomeration. The high reactivity and favourable oxygen uncoupling properties make these oxygen carriers promising candidates for the CLOU process.
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10.
  • Arjmand, Mehdi, 1986-, et al. (författare)
  • Evaluation of CuAl2O4 as an Oxygen Carrier in Chemical-Looping Combustion
  • 2012
  • Ingår i: Industrial & Engineering Chemistry Research. - 1520-5045. ; 51:43
  • Tidskriftsartikel (refereegranskat)abstract
    • The chemical-looping combustion (CLC) process is a novel solution for efficient combustion with intrinsic separation of carbon dioxide. The process uses a metal oxide as an oxygen carrier to transfer oxygen from an air to a fuel reactor where the fuel, or gasification products of the fuel, reacts with the solid oxygen carrier. In this work, copper(II) aluminate (CuAl2O4) was assessed as a potential oxygen carrier using methane as fuel. The carrier particles were produced by freeze–granulation and calcined at 1050 °C for a duration of 6 h. The chemical-looping characteristics were evaluated in a laboratory-scale fluidized-bed reactor in the temperature range of 900–950 °C during 45 alternating redox cycles. The oxygen carrier exhibited reproducible and stable reactivity behavior in this temperature range. Neither agglomeration nor defluidization was noticed in any of the cycles carried out at 900–925 °C. However, after reactivity tests at 950 °C, soft agglomeration and particle fragmentation were observed. Systematic phase analysis of the Cu–Al–O system during the redox cycle was carried out as a function of duration of reduction and oxygen concentration during the oxidation period. It was found that the CuAl2O4 is reduced to copper(I) aluminate (CuAlO2; delafossite), Cu2O, and elemental Cu. The CuAlO2 phase is characterized by slow kinetics for oxidation into CuO and CuAl2O4. Despite this kinetic limitation, complete conversion of methane with reproducible reactivity of the oxygen carrier is achieved. Thus, CuAl2O4 could be a potential oxygen carrier for chemical-looping combustion.
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