| 1. |
- Cho, Paul In-Young, 1970, et al.
(författare)
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Carbon Formation on Nickel and Iron Oxide-Containing Oxygen Carriers for Chemical-Looping Combustion
- 2005
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Ingår i: Industrial & Engineering Chemistry Research. - : American Chemical Society (ACS). - 1520-5045 .- 0888-5885. ; 44:4, s. 668-676
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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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| 2. |
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| 3. |
- Cho, Paul In-Young, 1970, et al.
(författare)
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Defluidization conditions for fluidized-bed of iron, nickel, and manganese oxide containing oxygen-carriers for chemical-looping combustion
- 2006
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Ingår i: Industrial & Engineering Chemistry Research. - : American Chemical Society (ACS). - 1520-5045 .- 0888-5885. ; 45:3, s. 968-977
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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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| 4. |
- Keller, Martin, 1985, et al.
(författare)
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Investigation of Natural and Synthetic Bed Materials for Their Utilization in Chemical Looping Reforming for Tar Elimination in Biomass-Derived Gasification Gas
- 2014
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Ingår i: Energy & Fuels. - : American Chemical Society (ACS). - 1520-5029 .- 0887-0624. ; 28:6, s. 3833-3840
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Tidskriftsartikel (refereegranskat)abstract
- The removal of condensable hydrocarbons or tars from raw gas derived from biomass gasification presents an obstacle in the widespread application of biomass gasification. Hot catalytic tar cleaning as a secondary tar removal strategy is discussed as a tar cleaning technology. This can be realized in a dual-fluidized-bed reactor system, in which a catalytically active bed material is continuously regenerated. Such a process is termed chemical looping reforming (CLR). In such a process, it has been suggested that oxygen carrier particles employed for chemical looping combustion may be used, with the oxygen transfer from the particles to the gas promoting tar decomposition. Experiments were conducted in a small-scale, batch-wise fluidized-bed reactor with the aim of investigating a variety of bed materials for this process. The purpose of the present work is thus to conduct a screening study of a variety of bed materials based on the transition metals Fe, Mn, Ni, and Cu. The experiments were conducted in a batch fluidized bed, where the particles are exposed to reformer and regenerator conditions alternatingly. The conversion of ethylene from a synthetic gasification gas mixture was used as an indicator for the suitability of the materials for tar conversion. It was found that the natural material bauxite and the synthetic bed materials NiO/alpha-Al2O3, CuO/MgAl2O4, and La0.8Sr0.2FeO3/gamma-Al2O3 exhibit high ethylene conversion rates and, thus, possess promising properties for their application in CLR
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| 5. |
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| 6. |
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| 7. |
- Penthor, Stefan, et al.
(författare)
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The EU-FP7 Project SUCCESS - Scale-up of Oxygen Carrier for Chemical Looping Combustion using Environmentally Sustainable Materials
- 2017
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Ingår i: Energy Procedia. - : Elsevier BV. - 1876-6102. ; 114, s. 395-406
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Konferensbidrag (refereegranskat)abstract
- The paper gives a high level overview of the work performed in the EU-FP7 funded project SUCCESS (Scale-up of oxygen carrier for chemical looping combustion using environmentally sustainable materials). The project is the most recent one in a series of successful EU-funded research projects on the chemical looping combustion (CLC) technology. Its main objective is to perform the necessary research in order to demonstrate the CLC technology in the range of 10 MW fuel power input. The main focus is on scale-up of production of two different oxygen carrier materials using large scale equipment and industrially available raw materials. This will guarantee availability of oxygen carrier material at tonne scale. The scale-up of the two materials, a Cu and a Mn based, was successful and first tests with the Cu material have already been performed in four different pilot units up to 150 kW where the material showed excellent performance regarding fuel conversion. In addition to technology scale-up, extensive end-user evaluation is performed. This evaluation includes investigations on health, security and environmental impacts (HSE), a life cycle analysis and a techno-economic analysis to compare the CLC technology for steam generation against the current state-of-the-art technologies.
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| 8. |
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| 9. |
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| 10. |
- Abad, Alberto, 1972, et al.
(författare)
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The use of iron oxide as oxygen carrier in a chemical-looping reactor
- 2007
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Ingår i: Fuel. - : Elsevier BV. - 0016-2361. ; 86:7-8, s. 1021-1035
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Tidskriftsartikel (refereegranskat)abstract
- Chemical-looping combustion (CLC) is a method for the combustion of fuel gas with inherent separation of carbon dioxide. This technique involves the use of two interconnected reactors, an air reactor and a fuel reactor. The oxygen demanded in the fuel combustion is supplied by a solid oxygen carrier, which circulates between both reactors. Fuel gas and air are never mixed and pure CO2 can be obtained from the flue gas exit. This paper presents the results from the use of an iron-based oxygen-carrier in a continuously operating laboratory CLC unit, consisting of two interconnected fluidized beds. Natural gas or syngas was used as fuel, and the thermal power was between 100 and 300 W. Tests were performed at four temperatures: 1073, 1123, 1173 and 1223 K. The prototype was successfully operated for all tests and stable conditions were maintained during the combustion. The same particles were used during 60 h of hot fluidization conditions, whereof 40 h with combustion. The combustion efficiency of syngas was high, about 99% for all experimental conditions. However, in the combustion tests with natural gas, there was unconverted methane in the exit flue gases. Higher temperature and lower fuel flows increase the combustion efficiency, which ranged between 70% and 94% at 1123 K. No signs of agglomeration or mass loss were detected, and the crushing strength of the oxygen carrier particles did not change significantly. Complementary experiments in a batch fluidized bed were made to compare the reactivity of the oxygen carrier particles before and after the 40 h of operation, but the reactivity of the particles was not affected significantly.
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| 11. |
- Abanades, J. C., et al.
(författare)
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Emerging CO2 capture systems
- 2015
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Ingår i: International Journal of Greenhouse Gas Control. - : Elsevier BV. - 1750-5836. ; 40, s. 126-166
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Tidskriftsartikel (refereegranskat)abstract
- In 2005, the IPCC SRCCS recognized the large potential for developing and scaling up a wide range of emerging CO2 capture technologies that promised to deliver lower energy penalties and cost. These included new energy conversion technologies such as chemical looping and novel capture systems based on the use of solid sorbents or membrane-based separation systems. In the last 10 years, a substantial body of scientific and technical literature on these topics has been produced from a large number of R&D projects worldwide, trying to demonstrate these concepts at increasing pilot scales, test and model the performance of key components at bench scale, investigate and develop improved functional materials, optimize the full process schemes with a view to a wide range of industrial applications, and to carry out more rigorous cost studies etc. This paper presents a general and critical review of the state of the art of these emerging CO2 capture technologies paying special attention to specific process routes that have undergone a substantial increase in technical readiness level toward the large scales required by any CO2 capture system.
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| 12. |
- Adanez-Rubio, Inaki, et al.
(författare)
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Development of new Mn-based oxygen carriers using MgO and SiO 2 as supports for Chemical Looping with Oxygen Uncoupling (CLOU)
- 2023
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Ingår i: Fuel. - : Elsevier BV. - 0016-2361. ; 337
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Tidskriftsartikel (refereegranskat)abstract
- Chemical Looping with Oxygen Uncoupling (CLOU) is a technological adaptation of CLC, most applicable for the combustion of solid fuels. In the CLOU process, an oxygen carrier in the fuel reactor, avoiding the direct contact of the fuel with the air, releases the oxygen needed for the fuel combustion. The oxygen carrier is regenerated with air in the interconnected air reactor. The present work explores the behavior of the system Mn/Mg/Si as oxygen carriers for chemical-looping with oxygen uncoupling (CLOU). Six different mixed oxides of the system Mn/Mg/Si were investigated for the CLC/CLOU process. Materials were prepared by spray drying with different metal ratios used in the investigation. The properties of interest for the viability of these materials are the lattice oxygen supply for CLC and the gaseous oxygen release for CLOU, properties that were explored in a TGA. Further, the fluidization behavior and the mechanical resistance were investigated in a batch fluidized bed reactor. In the TGA it was observed that the most reactive oxygen carriers for the CLOU process were materials without Si in the structure, more specifically M24Mg76 and M48Mg51 which had a molar ratio of Mn/Mg of 0.17 and 0.51 respectively. It was also observed that for the oxygen carriers with Si in the composition, the regeneration was very poor. Oxygen carriers M24Mg76 and M48Mg51 were selected for batch fluidized bed reactor testing showing good behavior with respect to the CLOU reactivity, and mechanical stability. One of the materials, the M24Mg76 showed activation during the experiments in the batch fluidized bed reactor experiments, increasing the oxygen transport capacity by 20 % during the experiment. However, 10 vol% of O2 was needed to regenerate both oxygen carriers at 850 °C. No agglomeration tendencies were seen, and the attrition rate was low, obtaining high-extrapolated lifetime values. The fact that highly reactive oxygen carriers can be made with cheap and highly available metals oxides, i.e. Mn and Mg, makes this system very promising and a possible alternative to benchmark Cu-based CLOU materials.
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| 13. |
- Adanez-Rubio, Inaki, et al.
(författare)
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Investigation of Combined Supports for Cu-based Oxygen Carriers for Chemical-Looping with Oxygen Uncoupling (CLOU)
- 2013
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Ingår i: Energy & Fuels. - : American Chemical Society (ACS). - 1520-5029 .- 0887-0624. ; 27:7, s. 3918-3927
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Tidskriftsartikel (refereegranskat)abstract
- The chemical-looping with oxygen uncoupling (CLOU) process is a novel solution for efficient combustion with inherent separation of carbon dioxide. The process uses a metal oxide as an oxygen carrier to transfer oxygen from an air to a fuel reactor. In the fuel reactor, the metal oxide releases gas phase oxygen which oxidizes the fuel through normal combustion. In this study, Cu-based oxygen carrier materials that combine different supports of MgAl2O4, TiO2 and SiO2 are prepared and characterized with the objective of obtaining highly reactive and attrition resistant particles. The oxygen carrier particles were produced by spray-drying and were calcined at different temperatures ranging from 950 to 1030oC for 4 h. The chemical-looping performance of the oxygen carriers was examined in a batch fluidized-bed reactor in the temperature range of 900-950oC under alternating reducing and oxidizing conditions. The mechanical stability of the oxygen carriers was tested in a jet-cup attrition rig. All of the oxygen carriers showed oxygen uncoupling behaviour with oxygen concentrations close to equilibrium. During reactivity tests with methane, oxygen carriers with lower mechanical stability showed higher reactivity, yielding almost complete fuel conversion. Oxygen carrier materials based on support mixtures of MgAl2O4/TiO2, MgAl2O4/SiO2 and TiO2/SiO2 showed a combination of high mechanical stability, low attrition rates, good reactivity with methane and oxygen uncoupling behaviour.
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| 14. |
- Adanez-Rubio, Inaki, et al.
(författare)
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Use of a high-entropy oxide as an oxygen carrier for chemical looping
- 2024
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Ingår i: Energy. - 0360-5442. ; 298
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Tidskriftsartikel (refereegranskat)abstract
- One mixed oxide with 5 cations in equimolar proportions in the sublattice, to fulfil high-entropy oxide (HEO) criteria, has been developed and investigated as oxygen carrier for chemical looping combustion processes. As far as we know, nobody has explored this class of material for chemical looping combustion. Material is prepared by direct mixing of five metal oxides (CuO, Mn2O3, Fe2O3, TiO2, MgO), followed by calcination at 1000, 1100 and 1200 °C for 6 h in air. XRD characterization provides strong evidence that the synthesized oxygen carriers possess the hallmark properties of HEO, and SEM-EDX analysis shows an overall homogeneous metal distribution. Materials have one main cubic phase with the empirical formula MnCuMgFeTiO7, dominating under all conditions. One of the key objectives of this study is achieved, reduce chemical stress during redox cycles. Oxygen transfer capability is investigated by thermogravimetric analysis and batch fluidized bed reactor experiments for different fuels and atmospheres. Mass-based oxygen transport capacities for lattice oxygen and oxygen uncoupling are around 5.5 wt% and 1.1 wt%, respectively. This work opens up a new dimension for the future preparation of oxygen carriers for chemical looping processes, since the vast compositional space of HEO provides opportunities to tune both chemical and physical characteristics.
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| 15. |
- Andersson, Viktor, 1983, et al.
(författare)
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Alkali desorption from ilmenite oxygen carrier particles used in biomass combustion
- 2024
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Ingår i: Fuel. - 0016-2361 .- 1873-7153. ; 359
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Tidskriftsartikel (refereegranskat)abstract
- Oxygen-carrying fluidized bed materials are increasingly used in novel technologies for carbon capture and storage, and to improve the efficiency of fuel conversion processes. Potassium- and sodium-containing compounds are released during biomass combustion and may have both negative and positive effects on conversion processes. Ilmenite is an important oxygen carrier material with the ability to capture alkali in the form of titanates. This is a desirable property since it may reduce detrimental alkali effects including fouling, corrosion, and fluidized bed agglomeration. This study investigates the interactions of alkali-containing compounds with ilmenite particles previously used in an industrial scale (115 MWth) oxygen carrier aided combustion system. The ilmenite samples were exposed to temperatures up to 1000 °C under inert and oxidizing conditions while the alkali release kinetics were characterized using online alkali monitoring. Alkali desorption occurs between 630 and 800 °C, which is attributed to loosely bound alkali at or near the surface of the particles. Extensive alkali release is observed above 900 °C and proceeds during extended time periods at 1000 °C. The release above 900 °C is more pronounced under oxidizing conditions and approximately 9.1 and 3.2 wt% of the alkali content is emitted from the ilmenite samples in high and low oxygen activity, respectively. Detailed material analyses using scanning electron microscopy with energy dispersive X-ray spectroscopy and X-ray photoelectron spectroscopy were conducted before and after temperature treatment, which revealed that the concentrations of potassium, sodium and chlorine decrease at the outermost surface of the ilmenite particles during temperature treatment, and Cl is depleted to a deeper level in oxidizing conditions compared to inert. The implications for ilmenite-ash interactions, oxygen carrier aided combustion and chemical looping systems are discussed.
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| 16. |
- Andersson, Viktor, 1983, et al.
(författare)
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Alkali interactions with a calcium manganite oxygen carrier used in chemical looping combustion
- 2022
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Ingår i: Fuel Processing Technology. - : Elsevier BV. - 0378-3820 .- 1873-7188. ; 227
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Tidskriftsartikel (refereegranskat)abstract
- Chemical-Looping Combustion (CLC) of biofuels is a promising technology for cost-efficient CO2 separation and can lead to negative CO2 emissions when combined with carbon capture and storage. A potential challenge in developing CLC technology is the effects of alkali metal-containing compounds released during fuel conversion. This study investigates the interactions between alkali and an oxygen carrier (OC), CaMn0.775Ti0.125Mg0.1O3-δ, to better understand the fate of alkali in CLC. A laboratory-scale fluidized bed reactor is operated at 800–900 °C in oxidizing, reducing and inert atmospheres to mimic CLC conditions. Alkali is fed to the reactor as aerosol KCl particles, and alkali in the exhaust is measured online with a surface ionization detector. The alkali concentration changes with gas environment, temperature, and alkali loading, and the concentration profile has excellent reproducibility over repeated redox cycles. Alkali-OC interactions are dominated by alkali uptake under most conditions, except for a release during OC reduction. Uptake is significant during stable reducing conditions, and is limited under oxidizing conditions. The total uptake during a redox cycle is favored by a high alkali loading, while the influence of temperature is weak. The implications for the understanding of alkali behavior in CLC and further development are discussed.
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| 17. |
- Andersson, Viktor, 1983, et al.
(författare)
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Alkali-wall interactions in a laboratory-scale reactor for chemical looping combustion studies
- 2021
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Ingår i: Fuel Processing Technology. - : Elsevier BV. - 0378-3820 .- 1873-7188. ; 217
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Tidskriftsartikel (refereegranskat)abstract
- Alkali metal-containing compounds are readily released during thermal conversion of solid fuels, and may have both detrimental and beneficial effects on chemical looping combustion. Here, we characterize alkali interactions with the inner walls of a laboratory-scale reactor under oxidizing, reducing and inert conditions at temperatures up to 900 °C. KCl aerosol particles are continuously introduced to the stainless steel reactor and the alkali concentration is measured on-line with a surface ionization detector. Aerosol particles evaporate at temperatures above 500 °C and KCl molecules rapidly diffuse to the reactor wall. Up to 92% of the alkali reaching the wall below 700 °C remains adsorbed, while re-evaporation is important at higher temperatures, where up to 74% remains adsorbed. Transient changes in alkali concentration are observed during repeated redox cycles, which are associated with changes in chemical composition of the wall material. Metal oxides on the reactor wall are partially depleted under reducing conditions, which allow for the formation of a new potassium-rich phase that is stable in a reducing atmosphere, but not under inert conditions. The observed wall effects are concluded to be extensive and include major transient effects depending on gas composition, and the implications for laboratory studies and improved experimental methodology are discussed.
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| 18. |
- Andersson, Viktor, 1983, et al.
(författare)
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Design and first application of a novel laboratory reactor for alkali studies in chemical looping applications
- 2023
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Ingår i: Fuel Processing Technology. - 0378-3820. ; 252
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Tidskriftsartikel (refereegranskat)abstract
- Alkali compounds are readily released during biomass conversion and their complex interactions with reactor walls and sampling equipment makes detailed investigations challenging. This study evaluates a novel laboratory-scale fluidized bed reactor for chemical looping combustion (CLC) studies. The reactor design is based on detailed consideration of the behavior of alkali-containing molecules and aerosol particles and is guided by computational fluid dynamic simulations. The design allows for interactions between gaseous alkali and a fluidized bed, while minimizing alkali interactions with walls before and after the fluidized bed. The function of the laboratory reactor is demonstrated in experiments using online gas and alkali analysis. Alkali is continuously fed to the reactor as KOH or KCl aerosol with and without a fluidized bed of the oxygen carrier CaMn0.775Ti0.125Mg0.1O3-δ present in inert, reducing and oxidizing conditions at temperatures up to 900 °C. Alkali uptake by the OC is characterized in all conditions, and observed to sensitively depend on gas composition, reactor temperature and type of alkali compound. The experimental setup is concluded to have a significantly improved functionality compared to a previously used reactor, which opens up for detailed studies of interactions between alkali compounds and oxygen carriers used in CLC.
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| 19. |
- Andersson, Viktor, 1983, et al.
(författare)
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Gaseous alkali interactions with ilmenite, manganese oxide and calcium manganite under chemical looping combustion conditions
- 2024
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Ingår i: Fuel Processing Technology. - 0378-3820 .- 1873-7188. ; 254
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Tidskriftsartikel (refereegranskat)abstract
- Alkali species present in biomass pose significant challenges in chemical looping combustion (CLC) processes and other thermal conversion applications. The interactions between different alkali species and three common oxygen carrier (OC) materials that are considered to be state of the art in CLC applications have been investigated. A dedicated fluidized bed laboratory reactor was used to study interactions of KCl, NaCl, KOH, NaOH, K2SO4 and Na2SO4 with manganese oxide, calcium manganite and ilmenite. Alkali vapor was generated by injecting alkali salts under reducing, oxidizing and inert conditions at 900 °C. Gaseous species were measured online downstream of the reactor, and the efficiency of alkali uptake was determined under different conditions. The result show significant alkali uptake by all OCs under the studied conditions. Ilmenite shows near complete alkali uptake in reducing conditions, while manganese oxide and calcium manganite exhibited less effective alkali uptake, but have advantages in terms of fuel conversion and oxidizing efficiency. Alkali chlorides, sulfates and hydroxides show distinctly different behavior, with alkali hydroxides being efficiently captured all three investigate OC materials. The findings contribute to a deeper understanding of alkali behavior and offer valuable guidance for the design and optimization of CLC with biomass.
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| 20. |
- Arjmand, Mehdi, 1986, et al.
(författare)
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CaxLa1−xMn1−yMyO3−δ (M = Mg, Ti, Fe or Cu) as Oxygen Carriers for Chemical-Looping with Oxygen Uncoupling (CLOU)
- 2013
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Ingår i: Energy & Fuels. - : American Chemical Society (ACS). - 1520-5029 .- 0887-0624. ; 27:8, s. 4097-4107
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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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| 21. |
- Arjmand, Mehdi, 1986, et al.
(författare)
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CaZrO3 and SrZrO3-based CuO Oxygen Carriers for Chemical-Looping with Oxygen Uncoupling (CLOU)
- 2014
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Ingår i: Energy Procedia. - : Elsevier BV. - 1876-6102. ; 51, s. 75-84
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Konferensbidrag (refereegranskat)abstract
- The chemical-looping combustion (CLC) and chemical-looping with oxygen uncoupling (CLOU) processes are novel solutions for efficient combustion with inherent separation of carbon dioxide. In this work, oxygen carriers based on CuO supported by zirconates of SrZrO3 and CaZrO3 are investigated. The oxygen carriers were produced by mechanical homogenization of primary solids in a rotary evaporator followed by extrusion, drying and calcination at 950 and 1030 degrees C for 6 h. Their chemical-looping performance was evaluated in a laboratory-scale fluidized-bed reactor at 900 and 925 degrees C under cyclic oxidizing, inert (N-2) and reducing (CH4) conditions. All oxygen carriers exhibited rapid release of oxygen in the inert environment (CLOU) with high conversion of methane. The carrier calcined at 1030 degrees C with SrZrO3 as support showed no agglomeration or deactivation and exhibited the highest reactivity. Thus, the use of this oxygen carrier could be of interest for the CLOU process.
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| 22. |
- Arjmand, Mehdi, 1986, et al.
(författare)
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Evaluation of CuAl2O4 as an Oxygen Carrier in Chemical-Looping Combustion
- 2012
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Ingår i: Industrial & Engineering Chemistry Research. - : American Chemical Society (ACS). - 1520-5045 .- 0888-5885. ; 51:43, s. 13924-13934
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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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| 23. |
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| 24. |
- Arjmand, Mehdi, 1986, et al.
(författare)
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Investigation of Different Manganese Ores as Oxygen Carriers in Chemical-Looping Combustion (CLC) for Solid Fuels
- 2014
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Ingår i: Applied Energy. - : Elsevier BV. - 1872-9118 .- 0306-2619. ; 113, s. 1883-1894
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Tidskriftsartikel (refereegranskat)abstract
- The chemical-looping combustion (CLC) process is a novel solution for efficient combustion with direct capture 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 reacts with the solid oxygen carrier. In this work, six different manganese ores are investigated as oxygen carriers for CLC application. The chemical-looping characteristics of the oxygen carriers were evaluated in a laboratory-scale fluidized-bed reactor in the temperature range of 900-970oC during alternating reducing and oxidizing conditions. Three of the manganese ores showed a small oxygen release in inert environment between 850 and 950oC. During reactivity tests, the gas yield with methane increased with the temperature and complete conversion of 50% CO in H2 was obtained for all of the ores. The rates of char gasification of two fuels, namely Mexican petroleum coke and Swedish wood char, were compared for the different manganese ores at 970oC and with 50% H2O in N2 as fluidizing gas. Ilmenite and a manufactured Mn-oxide oxygen carrier consisting of Mn3O4 and MgO-stabilized ZrO2 as support were also included for comparison. The char gasification rate and the gas conversion were higher with the manganese ores and the Mn-oxide oxygen carrier compared to ilmenite. However, the higher reactivity of the manganese ores with H2 and the ensuing decrease in H2 inhibition for manganese ores is not sufficient to explain their higher rate of char gasification. Surface analysis of partially gasified petcoke particles in the presence of manganese ores showed formation of cavities and channels as well as a uniform distribution of potassium and sodium elements. The rate of char gasification also increased with the concentration of potassium and sodium impurities in the manganese ores. Thus the results suggest that the increased rate of char conversion for manganese ores is due to alkali-catalyzed steam gasification. The increase in rate of char gasification, in combination with potentially low costs of these materials suggests that manganese ores could be interesting materials for CLC with solid fuels.
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| 25. |
- Arjmand, Mehdi, 1986, et al.
(författare)
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Oxygen Release and Oxidation Rates of MgAl2O4-Supported CuO Oxygen Carrier for Chemical-Looping Combustion with Oxygen Uncoupling (CLOU)
- 2012
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Ingår i: Energy & Fuels. - : American Chemical Society (ACS). - 1520-5029 .- 0887-0624. ; 26:11, s. 6528-6539
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Tidskriftsartikel (refereegranskat)abstract
- The chemical-looping combustion (CLC) and chemical-looping with oxygen uncoupling (CLOU) processes are novel solutions for efficient combustion with inherent separation of carbon dioxide. These processes use a metal oxide as an oxygen carrier to transfer oxygen from an air reactor to a fuel reactor, where the fuel reacts with the solid oxygen carrier. When solid fuel is used in CLC, the char must be gasified by, e.g., steam to form H2 and CO, that can be subsequently oxidized to H2O and CO2 by the oxygen carrier. In the case of CLOU, the oxygen carrier releases oxygen gas in the fuel reactor. This enables a high rate of conversion of char from solid fuels, because it eliminates the need for the gasification step needed in normal CLC with solid fuels. In this work, the rate of oxygen release and oxidation of an oxygen carrier consisting of CuO supported by MgAl2O4 (40/60 wt %) for the CLOU process is investigated. The oxygen carrier was produced by freeze-granulation, calcined at 950 °C, and sieved to a size range of 125–180 μm. The reaction rates were obtained in a laboratory-scale fluidized-bed reactor in the temperature range of 850–900 °C, under alternating reducing and oxidizing conditions. The rate of oxygen release was obtained using devolatilized wood char as the fuel in N2 fluidization. Care was taken to obtain reliable measurements not affected by the availability of the fuel and temperature increase in the bed during combustion of the fuel with the released oxygen from the carrier. The Avrami–Erofeev mechanism was used to model the rates of oxygen release and the values of ko and Eapp were estimated to be 2.5 × 105 s–1 and 139.3 kJ mol–1, respectively. The rates of Cu2O oxidation were investigated in a flow of 5% O2 at the inlet of the reactor. However, it was observed that the oxidation rate is limited by the oxygen supply, indicating rapid conversion of the oxygen carrier. From the obtained reaction rates, the minimum total amount of the investigated oxygen carrier needed in the air and the fuel reactor is estimated to be between 69–139 kg MWth–1.
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