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Chemical looping technologies can be used as an advanced reforming technology, capable of efficiently generating syngas to serve as a feedstock in a variety of important chemical industries. The pressure of the syngas feedstock to downstream chemical synthesis reactors is an important characteristic that can dictate the products and overall plant economics. While most chemical synthesis reactors, such as Fischer-Tropsch and methanol synthesis reactors, operate at high pressures, most chemical looping reforming studies have been conducted under atmospheric conditions. The high thermodynamic yields from the atmospheric chemical looping reformer run counter to the high conversion of the pressurized downstream reactors. Therefore, this study seeks to quantify the impact of the operating conditions of the chemical looping reformer on the overall system yields. Specifically, The Ohio State University methane to syngas process is analyzed, which uses a cocurrent moving bed fuel/reducer reactor and a fluidized bed air/combustor reactor. The syngas generation results are compared under a variety of operating conditions with the pressure varied between 1 and 30 atm. Initial studies are compared in an isothermal analysis to study the effect of variables, independent of operating temperature. The resulting isothermal analysis is used to guide an adiabatic reactor configuration in an attempt to develop an autothermal chemical looping system. The gas feedstocks, solid feedstocks, operating temperature, feedstock preheating conditions, and system pressure are all analyzed. The results of the autothermal chemical looping system are then integrated into a ~5000 MWth natural gas to liquid fuels plant, in which a chemical looping reformer replaces an autothermal reformer reactor. The study shows that operation of the chemical looping process allows for equivalent syngas yield compared to the autothermal reformer with a 7-13% reduction in natural gas feedstock. Lastly, a novel operating strategy is described in which the chemical looping reducer operates at higher pressure and the chemical looping combustor operates at atmospheric conditions. Such an operating strategy takes advantage of the air and natural gas feedstock pressures to the chemical looping system and is able to eliminate a significant amount of compression energy and equipment. Using the differential operating strategy allows equivalent syngas production to the baseline with a 7% decrease in natural gas usage and ~200 MWe increase in electricity production. A capital cost comparison of the equivalent pressure and differential pressure chemical looping systems indicate a 29% reduction in capital costs when using the differential pressure chemical looping system.
The importance of syngas and hydrogen (H2) along with the abundance of natural gas underlines the need for an energy efficiency and economical means of syngas and H2 production from natural gas. The conventional processes for syngas and H2 production consist of several unit operations and are very energy intensive. Additionally, these processes have a lot of CO2 emissions which is a major drawback considering the concern for global warming cause by greenhouse effect. Chemical looping process is an attractive alternative to the conventional processes. It has better exergy efficiency and reduces the downstream processing steps by inherent separation of the products. The reducing and oxidizing gases are either spatially or temporally separation which minimizes the safety hazard of forming a flammable mixture at high temperature. Despite several research efforts in application of chemical looping for syngas and H2 production there still exists scope for improvement in terms of syngas yield and overall process efficiency. In this thesis, the three major aspects of chemical looping process: oxygen carriers, reactor configuration and process configuration, are explored for strategies to enhance syngas and H2 yield. A co-current moving bed reactor configuration is simulated experimentally and theoretically for copper-iron oxygen carriers in addition to testing 5 different process configurations for the overall system. CH4 conversion and dry syngas purity of 99.5% and 97.5%, respectively, is observed in a U-tube fixed bed reactor where a co-current moving bed reactor solids profile is mimicked using copper oxide (20 wt%) - iron oxide (60 wt%) - aluminium oxide (20 wt%) oxygen carrier. The net H2 production is higher by 28% and effective thermal efficiency is 10% more than that of autothermal reforming process for the best performing process configuration. A different process configuration is also shown to have higher syngas yield than the conventional two reactor chemical looping reforming system with iron oxide-magnesium aluminate as the oxygen carrier. Process simulations in ASPEN Plus software are performed under different heat transfer, pressure and co-injection conditions to understand the benefit offered by the improved process configuration. Finally, an improvement in H2 production and, subsequently, cold gas efficiency for a chemical looping combustion system is observed using a staged H2 separation approach in the oxidizer reactor. H2 separation module was simulated in ASPEN Plus software and several combinations of separation modules and oxidizer reactor were screened for highest H2 production. A maximum cold gas efficiency of about 79%, which is 7% and 1.5% higher than the steam methane reforming process (Department of Energy baseline case) and traditional chemical looping combustion system, respectively.
Covers the timely topic of fuel cells and hydrogen-based energy from its fundamentals to practical applications Serves as a resource for practicing researchers and as a text in graduate-level programs Tackles crucial aspects in light of the new directions in the energy industry, in particular how to integrate fuel processing into contemporary systems like nuclear and gas power plants Includes homework-style problems
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.
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.
This work details the technical, environmental and business aspects of current methanol production processes and presents recent developments concerning the use of methanol in transportation fuel and in agriculture. It is written by internationally renowned methanol experts from academia and industry.
The following study entails process simulations and techno-economic analysis based investigations of novel chemical looping partial oxidation processes. The moving bed reactor system analyzed in this dissertation provides chemical looping technologies several intrinsic advantages over conventional energy processing schemes. Chapter 2 focusses on optimizing the counter-current moving bed chemical looping system for H2 production from natural gas. The chemical looping process for H2 production from natural gas is optimized based on isothermal thermodynamic limits of an iron-based counter-current moving bed reactor system. The iso-thermal analysis is followed by a parametric sensitivity for energy balance for satisfying the auto-thermal heat balance. This is completed by computing temperature swings based on a net heat duty calculation for individual chemical looping reactors. Overall the chemical looping process is shown to have a cold gas efficiency of 77.6% (HHV basis) and an effective thermal efficiency of 75.1% (HHV basis), both of which are significantly higher than the baseline case. Chapter 3 discusses the Shale gas to Syngas process for integration into a Gas to Liquid fuel (GTL) plant. Following the methodology for an isothermal and an adiabatic analysis from Chapter 2, Chapter 3 identifies a suitable auto-thermal operating condition for the chemical looping reactors. The process simulation model is used to derive cost estimates based on standard engineering assumptions and completes a sensitivity analysis for several important economic parameters. The STS process is shown to require significantly lower natural gas feedstock than the conventional process baseline for producing the same amount of liquid fuels. The STS process lowers the capital cost investment for the syngas production section of a GTL plant by over 50% and if commercialized can be disruptive to liquid fuel production markets. Chapter 4 discusses the Coal to syngas (CTS) process for its technical and economic performance when integrated into a 10,000 tpd methanol plant. This chapter details the equipment sizing philosophy and cost methodology used in this dissertation for calculating economic performance of the novel processes developed. Further, sensitivity studies which analyze effect of economic parameters like the capital charge factor, natural gas price are considered to identify the critical technology parameters necessary to be de-risked for pilot scale and commercial scale operation of the CTS technology. The CTS process reduced the coal consumption by 14% for the same amount of methanol production. The CTS process also reduced the methanol required selling price by 21% over the corresponding baseline case with greater than 90% carbon capture. Chapter 5 discusses the two reducer chemical looping configurations and the fixed bed chemical looping configurations. The two reducer chemical looping configurations provide the flexibility for designing two different reducer reactors, each optimized to a specific fuel feedstock. The two reducer chemical looping configurations can improve over thermodynamic performance of a single reducer chemical looping configuration by providing the flexibility to get high solids conversion with high fuel conversions. The fixed bed operating strategy opens up ways to operate iron-based chemical looping system without solids circulation for high-efficiency production of syngas.
Advances in Synthesis Gas: Methods, Technologies and Applications: Syngas Products and Usage considers the applications and usages of syngas for producing different chemical materials such as hydrogen, methanol, ethanol, methane, ammonia, and more. In addition, power generation in fuel cells, or in combination with heat from syngas, as well as iron reduction with economic and environmental challenges for syngas utilization are described in detail. Introduces syngas characteristics and its properties Describes various methods and technologies for producing syngas Discusses syngas production from different roots and feedstocks
Provides a comprehensive review on the brand-new development of several multiphase reactor techniques applied in energy-related processes Explains the fundamentals of multiphase reactors as well as the sophisticated applications Helps the reader to understand the key problems and solutions of clean coal conversion techniques Details the emerging processes for novel refining technology, clean coal conversion techniques, low-cost hydrogen productions and CO2 capture and storage Introduces current energy-related processes and links the basic principles of emerging processes to the features of multiphase reactors providing an overview of energy conversion in combination with multiphase reactor engineering Includes case studies of novel reactors to illustrate the special features of these reactors