• Journal of Hydrogen and New Energy
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• v.28 no.5
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• pp.453-458
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• 2017

A study on the modeling of the methane Chemical Looping Reforming system was carried out. It is aimed to predict the temperature and concentration behavior of the product through modeling of oxygen carrier fixed bed reactors composed of multiple stacks. In order to design the reaction system, first of all, the flow rate of the hydrogen to be produced was calculated. The flow rate ratio of the oxidation/reduction reactor was calculated considering the heat of reaction between adjacent reactors. Finally, in this paper, kinetic model including empirical coefficients was suggested.

• Journal of Ceramic Processing Research
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• v.21 no.2
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• pp.148-156
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• 2020

We investigated NiFe2O4/Ce0.9Gd0.1O1.95 (GDC) composites as oxygen carrier materials for chemical looping hydrogen production (CLHP). CLHP is a promising technology to simultaneously capture carbon dioxide and produce hydrogen from fossil fuels. We found that increasing GDC content increased the amount of the hydrogen production of NiFe2O4/GDC composites. Moreover, the oxygen transfer rate for the re-dox reaction increased significantly with increasing GDC content. GDC may affect the reaction kinetics of NiFe2O4/GDC composites. The finely dispersed GDC particles on the surface of NiFe2O4 can increase the surface adsorption of reaction gases due to the oxygen vacancies on the surface of GDC, and enlarge the active sites by suppressing the grain growth of NiFe2O4. The NiFe2O4/15wt% GDC composite showed no significant degradation in the oxygen transfer capacity and reaction rate during several re-dox cycles. The calculated amount of hydrogen production for the NiFe2O4/15wt% GDC composite would be 2,702 L/day per unit mass (kg).

• Journal of Hydrogen and New Energy
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• v.26 no.6
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• pp.516-523
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• 2015

Nickel based oxygen transfer materials supported on two different YSZs were tested to evaluate their performance in methane chemical-looping reforming. The oxygen transfer materials of YSZs were selected with different amount of the doped yittrium in the $ZrO_2$ structure. The yittrium of 8 mol% stabilized the zirconia oxide to a cubic structure compare to the 3 mol% doping, which is known to be a good for oxygen transfer. Various nickel amounts (16wt.%, 32wt.%, 48wt.%) were loaded on the selected supports. The nickel amount of 32% shows the optimized catalyst structure with good physical properties and reducibility from the XRD, BET and H2-TPR analysis, especially when the support of 8YSZ was used. From the methane chemical-looping reforming, hydrogen was produced by methane decomposition catalyzed by Ni on both YSZs. Comparing two YSZ supports of 3YSZ and 8YSZ during the cycling tests, the catalyst with 8YSZ (Ni 32%) exhibits not only the higher methane conversion and hydrogen production but also a faster reaction rate reaching to the stable point.

• Journal of Ceramic Processing Research
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• v.21 no.1
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• pp.57-63
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• 2020

Chemical looping hydrogen production (CLHP) is an attractive technology for H₂ production due to its ability to produce H₂ and capture CO₂ from fossil fuels simultaneously. In this paper, we present MgFe₂O₄ as an oxygen carrier material with high efficiency, low cost, and stable properties for CLHP. The redox reactions occurred reversibly in the fuel, steam, and air reactor as MgFe₂O₄→MgO/Fe, MgO/Fe→MgO/Fe₃O₄, and MgO/Fe₃O₄→MgFe₂O₄, respectively. The oxygen transfer capacities of MgFe₂O₄ for 5% H₂/N₂ and 5% CO/N₂ gases were about 23 wt% at 900 ℃. Both the oxygen transfer capacity and rate were well maintained during 10 redox cycles at 900 ℃. No phase changes or agglomeration occurred as the redox cycle number increased. Similarly, MgFe₂O₄ did not exhibit significant degradation in its total amount or maximum rate of H₂ production during four redox cycles. The average calculated amount of H₂ production for MgFe₂O₄ was 2,806 L/day per unit mass (kg).

• Journal of Hydrogen and New Energy
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• v.22 no.4
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• pp.443-450
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• 2011

The three-reactor chemical-looping process (TRCL) for the production of hydrogen from natural gas is attractive for both $CO_2$ capture and hydrogen production. In this study, redox property of $Fe_2O_3$ and $WO_3$ supported with $ZrO_2$ and $MgAl_2O_4$ were studied with temperature programmed oxidation/reduction (TPO/R) experiment. All metal oxides were prepared by ball mill method. Metal oxides supported with $ZrO_2$ showed the good redox property in TPO and TPR tests. Reduction behavior was matched well the theoretical reduction mechanism. Metal oxides supported with $MgAl_2O_4$ formed a solid solution ($MgFe_{0.6}Al_{1.4}O_4$, $MgWO_4$). $Fe_2O_3$ showed more narrow reaction range and lower reaction temperature than $WO_3$.

• Korean Chemical Engineering Research
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• v.54 no.3
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• pp.394-403
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• 2016

$H_2$ production by chemical looping is an efficient method to convert hydrocarbon fuel into hydrogen with the simultaneous capture of concentrated $CO_2$. This process involves the use of an iron based oxygen carrier that transfers pure oxygen from oxidizing gases to fuels by alternating reduction and oxidation (redox) reactions. The enhanced reactivities of copper oxide doped iron-based oxygen carrier were reported, however, the fundamental understandings on the interaction between $Fe_2O_3$ and CuO are still lacking. In this study, we studied the effect of dopant of CuO to $Fe_2O_3/ZrO_2$ particle on the morphological changes and the associated reactivity using various methods such as SEM/EDX, XRD, BET, TPR, XPS, and TGA. It was found that copper oxide acted as a chemical promoter that change chemical environment in the iron based oxygen carrier as well as a structural promoter which inhibit the agglomeration. The enhanced reduction reactivity was mainly ascribed to the increase in concentration of $Fe^{2+}$ on the surface, resulting in formation of charge imbalance and oxygen vacancies. The CuO doped $Fe_2O_3/ZrO_2$ particle also showed the improved reactivity in the steam oxidation compared to $Fe_2O_3/ZrO_2$ particle probably due to acting as a structural promoter inhibiting the agglomeration of iron species.

• Clean Technology
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• v.17 no.1
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• pp.69-77
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• 2011

The intrinsic $CO_2$ separation and hydrogen production system is a novel concept using oxidation and reduction reactions of oxygen carrier for both $CO_2$ capture and high purity hydrogen production. The process consists of a fuel reactor (FR), a steam reactor (SR) and an air reactor (AR). The natural gas ($CH_4$) is oxidized to $CO_2$ and steam by the oxygen carrier in FR, whereas the steam is reduced to hydrogen by oxidation of the reduced oxygen carrier in SR. The oxygen carrier is fully oxidized by air in AR. In the present study, the chemical looping moving bed reactor having 200 L/h hydrogen production capacity is designed and the hydrodynamic properties were determined. Compared with other reactors, two moving bed reactors (FR, SR) were used to obtain high conversion and selectivity of the oxygen carrier. The desirable solid circulation rates are calculated to be in the range of $20{\sim}100kg/m^2s$ from the conceptual design. The solid circulation rate can be controlled by aeration in a loop-seal. To maintain the gas velocity in the moving beds (FR, SR) at the minimum fluidization velocity is found to be suitable for the stable operation. The solid holdup in moving beds decrease with increasing gas velocity and solid circulation rate.