Development and Performance of a Cu-based Oxygen-carrier for Chemical-looping Combustion of Soil Fuels PDF Download

Author: S. Y. Chuang
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Languages : en
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Author: Cheng Lung Chung
Publisher:
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Category : Chemical engineering
Languages : en
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This dissertation presents investigations of chemical looping technology as a transformative process for combustion of fossil fuels for power generation with CO2 capture. Specifically, the dissertation seeks to synthesize and characterize a low-cost iron-based oxygen carrier that can be employed in a commercial chemical looping combustion system with realistic material lifetime and adequate resistance to toxicity from pollutants from fossil fuels such as coal. Two secondary metal oxides (Al2O3 and TiO2) as support materials for Fe2O3 and their respective reaction-induced morphological changes are presented. A novel iron-based oxygen carrier was consequently identified to be sustainable over 3000 redox cycles in high temperatures (1000 °C) at the lab scale without chemical and physical degradation. Oxygen carrier of the same design also exhibited high resistance toward attrition from circulation and fluidization in two pilot-scale demonstration units under representative conditions. Tolerance of the active ingredients of the iron-based oxygen carriers against common toxic elements in the fossil fuel feedstock, such as alkaline and sulfur compounds from conversion of coal, through multiple fixed bed experiments under conditions representative of the counter-current moving bed reducer and thermogravimetric experiments up to 9000 ppm of H2S. The likelihood of agglomeration and interaction of alkaline metals (Na, K) with the iron-based oxygen carriers were found to be extremely low under normal operating conditions. Instead, proper distribution of coal was more crucial to avoid agglomeration caused by melting of SiO2. Sulfur deposition on iron-based oxygen carriers, although observed, was reversible through regeneration with air and did not result in degradation in the recyclability of the oxygen carriers. A potential pathway for sulfur emission via the combustor spent air was also identified. The sulfur emission and distribution of the Coal-Direct Chemical Looping (CDCL) 25 kWth sub-pilot unit which utilized the iron-based oxygen carriers was determined with a custom heat-traced gas sampling system. More than 69% of the total amount of atomic sulfur from high sulfur coal was converted to SO2 and H2S in the reducer flue gas stream while less than 5% was released as SO2 in the combustor spent air. The missing atomic sulfur in the balance was attributed to sulfur retained in coal ash as inorganic sulfur compounds. A flue gas clean-up system targeting both H2S and SO2 is therefore recommended to meet the quality of CO2-rich stream for transportation and sequestration in a commercial CDCL system. The projected sulfur emission in the combustor spent air was under the US EPA sulfur emission regulation safe to be released to the atmosphere without a costly acid removal system. The findings demonstrate the robustness of the CDCL system, together with the iron-based oxygen carriers, to handle high sulfur coal without severe performance and economic penalties.

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Languages : en
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Chemical Looping Combustion (CLC) is one promising fuel-combustion technology, which can facilitate economic CO2 capture in coal-fired power plants. It employs the oxidation/reduction characteristics of a metal, or oxygen carrier, and its oxide, the oxidizing gas (typically air) and the fuel source may be kept separate. This topical report discusses the results of four complementary efforts: (5.1) the development of process and economic models to optimize important design considerations, such as oxygen carrier circulation rate, temperature, residence time; (5.2) the development of high-performance simulation capabilities for fluidized beds and the collection, parameter identification, and preliminary verification/uncertainty quantification; (5.3) the exploration of operating characteristics in the laboratoryscale bubbling bed reactor, with a focus on the oxygen carrier performance, including reactivity, oxygen carrying capacity, attrition resistance, resistance to deactivation, cost and availability; and (5.4) the identification of kinetic data for copper-based oxygen carriers as well as the development and analysis of supported copper oxygen carrier material. Subtask 5.1 focused on the development of kinetic expressions for the Chemical Looping with Oxygen Uncoupling (CLOU) process and validating them with reported literature data. The kinetic expressions were incorporated into a process model for determination of reactor size and oxygen carrier circulation for the CLOU process using ASPEN PLUS. An ASPEN PLUS process model was also developed using literature data for the CLC process employing an iron-based oxygen carrier, and the results of the process model have been utilized to perform a relative economic comparison. In Subtask 5.2, the investigators studied the trade-off between modeling approaches and available simulations tools. They quantified uncertainty in the high-performance computing (HPC) simulation tools for CLC bed applications. Furthermore, they performed a sensitivity analysis for velocity, height and polydispersity and compared results against literature data for experimental studies of CLC beds with no reaction. Finally, they present an optimization space using simple non-reactive configurations. In Subtask 5.3, through a series of experimental studies, behavior of a variety of oxygen carriers with different loadings and manufacturing techniques was evaluated under both oxidizing and reducing conditions. The influences of temperature, degree of carrier conversion and thermodynamic driving force resulting from the difference between equilibrium and system O2 partial pressures were evaluated through several experimental campaigns, and generalized models accounting for these influences were developed to describe oxidation and oxygen release. Conversion of three solid fuels with widely ranging reactivities was studied in a small fluidized bed system, and all but the least reactive fuel (petcoke) were rapidly converted by oxygen liberated from the CLOU carrier. Attrition propensity of a variety of carriers was also studied, and the carriers produced by freeze granulation or impregnation of preformed substrates displayed the lowest rates of attrition. Subtask 5.4 focused on gathering kinetic data for a copper-based oxygen carrier to assist with modeling of a functioning chemical looping reactor. The kinetics team was also responsible for the development and analysis of supported copper oxygen carrier material.

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Languages : en
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Chemical Looping Combustion (CLC) could totally negate the necessity of pure oxygen by using oxygen carriers for purification of CO2 stream during combustion. It splits the single fuel combustion reaction into two linked reactions using oxygen carriers. The two linked reactions are the oxidation of oxygen carriers in the air reactor using air, and the reduction of oxygen carriers in the fuel reactor using fuels (i.e. coal). Generally metal/metal oxides are used as oxygen carriers and operated in a cyclic mode. Chemical looping combustion significantly improves the energy conversion efficiency, in terms of the electricity generation, because it improves the reversibility of the fuel combustion process through two linked parallel processes, compared to the conventional combustion process, which is operated far away from its thermo-equilibrium. Under the current carbon-constraint environment, it has been a promising carbon capture technology in terms of fuel combustion for power generation. Its disadvantage is that it is less mature in terms of technological commercialization. In this DOE-funded project, accomplishment is made by developing a series of advanced copper-based oxygen carriers, with properties of the higher oxygen-transfer capability, a favorable thermodynamics to generate high purity of CO2, the higher reactivity, the attrition-resistance, the thermal stability in red-ox cycles and the achievement of the auto-thermal heat balance. This will be achieved into three phases in three consecutive years. The selected oxygen carriers with final-determined formula were tested in a scaled-up 10kW coal-fueled chemical looping combustion facility. This scaled-up evaluation tests (2-day, 8-hour per day) indicated that, there was no tendency of agglomeration of copper-based oxygen carriers. Only trace-amount of coke or carbon deposits on the copper-based oxygen carriers in the fuel reactor. There was also no evidence to show the sulphidization of oxygen carriers in the system by using the high-sulfur-laden asphalt fuels. In all, the scaled-up test in 10 kW CLC facility demonstrated that the preparation method of copper-based oxygen carrier not only help to maintain its good reactivity, also largely minimize its agglomeration tendency.

Author: Ronald W. Breault
Publisher: John Wiley & Sons
ISBN: 3527342028
Category : Business & Economics
Languages : en
Pages : 488

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This comprehensive and up-to-date handbook on this highly topical field, covering everything from new process concepts to commercial applications. Describing novel developments as well as established methods, the authors start with the evaluation of different oxygen carriers and subsequently illuminate various technological concepts for the energy conversion process. They then go on to discuss the potential for commercial applications in gaseous, coal, and fuel combustion processes in industry. The result is an invaluable source for every scientist in the field, from inorganic chemists in academia to chemical engineers in industry.

Author: Liang-Shih Fan
Publisher: John Wiley & Sons
ISBN: 1118063139
Category : Technology & Engineering
Languages : en
Pages : 353

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This book presents the current carbonaceous fuel conversion technologies based on chemical looping concepts in the context of traditional or conventional technologies. The key features of the chemical looping processes, their ability to generate a sequestration-ready CO2 stream, are thoroughly discussed. Chapter 2 is devoted entirely to the performance of particles in chemical looping technology and covers the subjects of solid particle design, synthesis, properties, and reactive characteristics. The looping processes can be applied for combustion and/or gasification of carbon-based material such as coal, natural gas, petroleum coke, and biomass directly or indirectly for steam, syngas, hydrogen, chemicals, electricity, and liquid fuels production. Details of the energy conversion efficiency and the economics of these looping processes for combustion and gasification applications in contrast to those of the conventional processes are given in Chapters 3, 4, and 5.Finally, Chapter 6 presents additional chemical looping applications that are potentially beneficial, including those for H2 storage and onboard H2 production, CO2 capture in combustion flue gas, power generation using fuel cell, steam-methane reforming, tar sand digestion, and chemicals and liquid fuel production. A CD is appended to this book that contains the chemical looping simulation files and the simulation results based on the ASPEN Plus software for such reactors as gasifier, reducer, oxidizer and combustor, and for such processes as conventional gasification processes, Syngas Chemical Looping Process, Calcium Looping Process, and Carbonation-Calcination Reaction (CCR) Process. Note: CD-ROM/DVD and other supplementary materials are not included as part of eBook file.

Author: Eli A. Goldstein
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Languages : en
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Development of a model that can be used to predict oxidation rates of copper to cuprous and cupric oxide (Cu2O and CuO, respectively) in the air reactor of a Chemical Looping Combustion (CLC) system is the primary focus of this thesis. The proposed oxidation model, which is based in Wagner Theory and defect chemistry, describes the fundamental processes occurring during copper oxidation. Consequently, it provides better predictive capabilities over a wide range of temperatures and pressures, as well as characteristic particle geometries (spheres, cylinders and plates) than the phenomenological models that are currently being used to predict oxidation rates of copper-based oxygen carriers used in CLC systems. In addition to developing this oxidation model, cuprous and cupric oxide reduction experiments with gaseous fuels like carbon monoxide, hydrogen and methane, and solid fuels like char, wyodak coal, and corn stover, were performed to characterize reaction rates in the fuel reactor of CLC systems. Oxidation rates obtained from the oxidation model, and measured rates from the reduction experiments were used to estimate the size and oxygen carrier loading for a 10 MWth CLC system.

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Languages : en
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Chemical looping combustion (CLC) is a combustion technology that utilizes oxygen from oxygen carriers (OC), such as metal oxides, instead of air to combust fuels. The use of natural minerals as oxygen carriers has advantages, such as lower cost and availability. Eight materials, based on copper or iron oxides, were selected for screening tests of CLC processes using coal and methane as fuels. Thermogravimetric experiments and bench-scale fixed-bed reactor tests were conducted to investigate the oxygen transfer capacity, reaction kinetics, and stability during cyclic reduction/oxidation reaction. Most natural minerals showed lower combustion capacity than pure CuO/Fe2O3 due to low-concentrations of active oxide species in minerals. In coal CLC, chryscolla (Cu-based), magnetite, and limonite (Fe-based) demonstrated better reaction performances than other materials. The addition of steam improved the coal CLC performance when using natural ores because of the steam gasification of coal and the subsequent reaction of gaseous fuels with active oxide species in the natural ores. In methane CLC, chryscolla, hematite, and limonite demonstrated excellent reactivity and stability in 50-cycle thermogravimetric analysis tests. Fe2O3-based ores possess greater oxygen utilization but require an activation period before achieving full performance in methane CLC. Particle agglomeration issues associated with the application of natural ores in CLC processes were also studied by scanning electron microscopy (SEM).

Author: Egwono Kelvin Okpoko
Publisher:
ISBN:
Category :
Languages : en
Pages : 0

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Author: Yitao Zhang
Publisher:
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Category : Chemical engineering
Languages : en
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With the rising concern of climate change, extensive research has been conducted in recent years on the mitigation of global warming. Greenhouse gas emissions are considered as the key driver of global warming. Among the various greenhouse gases, CO2 is the major contributor to the greenhouse effect. Therefore, mitigation of CO2 emission is the key to address global warming. Chemical looping is an energy conversion technology that can directly produce a concentrated CO2 stream, ready for sequestration and utilization, without the need for an individual CO2 separation step, and thus, has the potential to drastically reduce the energy consumption and cost associated with CO2 capture in carbonaceous fuel energy conversion systems. In this dissertation, process modeling and analysis are conducted on solid fuel power production processes to quantify the energy penalty and exergy losses associated with CO2 capture technologies, including state-of-the-art solvent-based CO2 absorption, oxy-combustion using high purity oxygen, and chemical looping combustion technology. Following the comparison of various power production processes using solid fuel with and without CO2 capture, a comprehensive analysis is performed to investigate the effect of varying operation conditions on the performance of chemical looping combustion reactor system. The coal-direct chemical looping process is a chemical looping combustion technology using moving bed reducer configuration that can directly use coal as the feedstock without requiring upstream gasification steps. An integrated 250 kWth coal-direct chemical looping pilot unit using iron-based oxygen carriers has been constructed and demonstrated for long-term continuous operations. The principles for the design and operation of the primary reactor system are discussed in this dissertation. The results of a successful 288-hour continuous demonstration with pulverized bituminous coal are reported. The results from the pilot unit highlight the concept of the chemical looping combustion process as a promising solid fuel combustion technology with CO2 capture. To investigate chemical looping technology for hydrogen production, process simulation and analysis is performed on two distinct configurations for chemical looping H2 generation process. The simulation results of two chemical looping H2 generation configurations are compared with the conventional steam-methane reforming system to underscore the attractiveness of the chemical looping configurations.