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This is the first comprehensive guide to the principles and techniques of chemical looping partial oxidation. With authoritative explanations from a pioneer of the chemical looping process, you will: • Gain a holistic overview of metal oxide reaction engineering, with coverage of ionic diffusion, nanostructure formation, morphological evolution, phase equilibrium, and recyclability properties of metal oxides during redox reactions • Learn about the gasification of solid fuels, the reforming of natural gas, and the catalytic conversion of methane to olefins • Understand the importance of reactor design and process integration in enabling metal oxide oxygen carriers to produce desired products • Discover other applications of catalytic metal oxides, including the production of maleic anhydride and solar energy conversions Aspen Plus® simulation software and results accompany the book online. This is an invaluable reference for researchers and industry professionals in the fields of chemical, energy and environmental engineering, and students studying process design and optimization.
The chemical looping partial oxidation process is developed for the efficient conversion of gaseous and solid fuels into syngas via partial oxidation. The chemical looping partial oxidation process converts the fuels into high purity syngas with flexible H2:CO ratio that is suitable for downstream fuel or chemical synthesis. In the chemical looping partial oxidation process, the fuels are partially oxidized in the reducer reactor by the oxygen carrier to generate high purity syngas. The reduced oxygen carrier is regenerated in a fluidized bed combustor via the oxidation reaction with air. Compared to the conventional syngas generation processes, the chemical looping partial oxidation process eliminates the need for additional steam or molecular oxygen from an air separation unit (ASU), resulting in an increased cold gas efficiency and decreased fuel consumption. The chemical looping partial oxidation process features the combination of an iron-titanium composite metal oxide (ITCMO) oxygen carrier and a co-current gas-solid moving bed reducer reactor. The ITCMO oxygen carrier is selected for the chemical looping partial oxidation process due to its desired thermodynamic and kinetic properties. Theoretical analysis aided by a modified Ellingham Diagram illustrates that syngas production is thermodynamically favored in the presence of ITCMO oxygen carrier. The co-current moving bed reducer design provides a desirable gas-solid contacting pattern that minimizes carbon deposition while maximizing the syngas yield. Experimental studies in a fixed bed reactor and a bench scale reactor successfully demonstrate the production of high purity syngas from methane and biomass with the combination of moving bed reducer and ITCMO oxygen carrier. Further scale-up of the chemical looping partial oxidation process is demonstrated in an integrated sub-pilot scale reactor system using non-mechanical gas sealing and solid circulation devices. A dynamic modeling scheme is developed for studying the transient behavior and the control of the chemical looping system. A hierarchical control system based on sliding mode control concept is developed for the chemical looping technologies to simplify process operation.
To view the benefits of chemical looping technology from a different perspective, exergy analysis is conducted on two of the five studied systems. Exergy is defined as the maximum work that can be derived during a process that brings a system into equilibrium with its environment. Exergy analysis pinpoints the locations of irreversibility and exergy destruction within a process system, hence providing a clearer view of the fundamental reasons for chemical looping to be more energy efficient than conventional processes.
Chemical looping partial oxidation is a process technology with the potential to enable clean, sustainable, and cost-effective valorization of hydrocarbon feedstocks to an array of chemical products. In the process scheme, the partial oxidation reaction is partitioned into separate reduction and oxidation reactions facilitated by an oxygen carrying chemical intermediate, referred to here as an oxygen carrier. By utilizing lattice oxygen donation from a metal oxide oxygen carrier in lieu of molecular oxygen, the hydrocarbon fuel can be efficiently converted to high purity syngas. The benefits and impacts of improving the efficiency of syngas generation are propagated through to downstream fuel and chemical synthesis processes. In this study, the chemical looping partial oxidation process for the thermochemical conversion of methane to syngas is investigated at the sub-pilot scale. Performance of the process and identification of viable operating conditions based on thermodynamic criteria is explored through process simulation. The design, construction, commissioning, and operation of a 15 kWth sub-pilot is detailed. In the unit, methane conversion of 99.64% and syngas purity of 97.13% are obtained with a product H2/CO ratio of 1.96. Co-reforming of methane with steam and CO2 is demonstrated, where net CO2 utilization is exhibited and flexible product H2/CO ratio of between 1.19 to 2.50 with high syngas purity is achieved. Finally, considerations for the design of the reactors during scale-up is discussed. The partial oxidation of biomass feedstocks towards the production of liquid fuels is investigated. Gasification of woody biomass and corncob biomass is studied at the sub-pilot scale where 89% carbon conversion and H2/CO ratio between 0.87 to 1.88 is demonstrated. Steam is shown to assist in the conversion of char in the moving bed reducer and suggestions toward commercial design are given. Adiabatic process simulation of the integration of the biomass to syngas process with the Fischer-Tropsch synthesis is investigated and it is shown that the chemical looping process can lead to 13.9% feedstock reduction and 5.7% increase in the lower heating value thermal efficiency relative to a competing gasification process. Finally, application electrical capacitance volume tomography is developed as a measurement technique to monitor and study the multiphase flow dynamics of the chemical looping process: critical to its scale-up and commercialization. A sensitivity gradient-based velocity profiling method is developed and applied to a gas-solid fluidized bed. The velocity profiles are validated against the cross-correlation technique and expected fluidized bed phenomena and breakdown of the method when tracking large objects is revealed and discussed.
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.
The first comprehensive guide to chemical looping partial oxidation processes, covering key principles, techniques, and applications.
Atmospheric-pressure plasmas continue to attract considerable research interest due to their diverse applications, including high power lasers, opening switches, novel plasma processing applications and sputtering, EM absorbers and reflectors, remediation of gaseous pollutants, excimer lamps, and other noncoherent light sources. Atmospheric-pressure plasmas in air are of particular importance as they can be generated and maintained without vacuum enclosure and without any additional feed gases. Non-Equilibrium Air Plasmas at Atmospheric Pressure reviews recent advances and applications in the generation and maintenance of atmospheric-pressure plasmas. With contributions from leading international researchers, the coverage includes advances in atmospheric-pressure plasma source development, diagnostics and characterization, air plasma chemistry, modeling and computational techniques, and an assessment of the status and prospects of atmospheric-pressure air plasma applications. The extensive application sections make this book attractive for practitioners in many fields where technologies based on atmospheric-pressure air plasmas are emerging.
Natural gas, which is mainly composed of methane, is an important industrial resource for syngas production. Nevertheless, the conventional methane to syngas conversion processes are highly energy intensive and suffer from low methane conversion. Chemical looping partial oxidation of methane is a promising alternative technology that consists two reactors connected by an oxygen carrier particle loop. This process has high syngas selectivity with higher energy efficiency, minimal environmental impact, and proper H2 to CO ratio for downstream operations. The major challenge for chemical looping processes is the development of high-performance oxygen carriers with high reactivity, recyclability, and recyclability. Our group employed novel iron-based oxygen carrier mixed with metal oxide support. The particles show extraordinary recyclability that sustained over 3000 redox cycles at 1000 oC without reactivity or mechanical deteriorates. Despite research efforts have been put into oxygen carrier development, there are still scopes for syngas yield and purification improvement, especially at low temperatures. In this dissertation, nanoscaled oxygen carriers are explored as oxygen carrier for chemical looping partial oxidation process. Nanoparticles have higher surface area and smaller size compared to bulk material, therefore increasing reaction rate by enhancing the surface reactivity and ionic diffusion. Mesoporous support was utilized to disperse and stabilize the nanoscaled oxygen carrier. The confinement effect of the mesopores of the support can separate the nanoparticles and prevent their aggregation during the reaction. SBA-15 supported iron oxides nanoparticles shows near 100% syngas selectivity and sustained over 75 redox cycles at 800 oC. Density functional theory calculations also indicate that nanoparticles have higher methane conversion rate and syngas selectivity. The effect of the mesoporous support structure on the reactivity of the oxygen carrier is also studied by both experiments and Dynamic Monte-Carlo simulations. With 2-D hexagonal cylindrical structure, SBA-15 can trap gas molecules and decrease the gas diffusion rate in the mesopores. While 3-D interconnected mesoporous support SBA-16 can decrease the congestion and trapping effect, therefore nanoparticles supported on SBA-16 show increased reaction rate compared with those on SBA-15. Dopant modification was also applied to nanoparticles. Nevertheless, doped iron oxide nanoparticles do not show extraordinary improvement in reactivity, stability, or selectivity, since the reactivity of the nanoparticles are not limited by surface active sites or ionic diffusivity. With the growing energy and environmental demands, chemical looping processes are facing more opportunities and challenges in oxygen carrier development. The research in this dissertation enlightens the chemical looping technology in the near future.
From Methane to Hydrogen-Making the Switch to a Cleaner Fuel Source The world's overdependence on fossil fuels has created environmental problems, such as air pollution and global warming, as well as political and economic unrest. With water as its only by-product and its availability in all parts of the world, hydrogen promises to be the next grea
Aline Leon ́ In the last years, public attention was increasingly shifted by the media and world governmentsto the conceptsof saving energy,reducingpollution,protectingthe - vironment, and developing long-term energy supply solutions. In parallel, research funding relating to alternative fuels and energy carriers is increasing on both - tional and international levels. Why has future energy supply become such a matter of concern? The reasons are the problems created by the world’s current energy supply s- tem which is mainly based on fossil fuels. In fact, the energystored in hydrocarb- based solid, liquid, and gaseous fuels was, is, and will be widely consumed for internal combustion engine-based transportation, for electricity and heat generation in residential and industrial sectors, and for the production of fertilizers in agric- ture, as it is convenient, abundant, and cheap. However, such a widespread use of fossil fuels by a constantly growing world population (from 2. 3 billion in 1939 to 6. 5 billion in 2006) gives rise to the two problems of oil supply and environmental degradation. The problemrelated to oil supply is caused by the fact that fossil fuels are not - newable primary energy sources: This means that since the rst barrel of petroleum has been pumped out from the ground, we have been exhausting a heritage given by nature.