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The increase of carbon footprint over the years is a serious cause of concern for mankind in recent times. As a consequence, carbon capture and sequestration has been given unprecedented focus. Chemical looping combustion (CLC) is one of the novel methods of carbon capture. A rotary reactor developed recently for CLC has been discussed extensively. The applicability of the chemical looping process in syngas production has been studied in this experiment. Ceria is used as the oxygen carrier material and YSZ (Yttria-Stabilized Zirconia) as the support material. Gas productions at different temperatures are studied to have a generic understanding of the reactions at different temperatures. Chemical looping reaction is observed to be a good method for syngas production, involving lesser steps than most conventional methods. Ceria is found to be a good oxygen carrier material. It is further noted that the quantity of syngas produced is higher as reactions are carried out at higher temperatures. Syngas produced using the chemical looping process allows for direct capture and sequestration of CO2, making the process in turn carbon neutral, sustainable and environment friendly.
The first comprehensive guide to chemical looping partial oxidation processes, covering key principles, techniques, and applications.
Chemical-looping (CL) is a novel and promising technology for several applications including oxy-combustion for carbon capture, hydrogen production and CO2 reuse. In this process, oxygen carriers are utilized to cyclically adsorb and release oxygen producing two separated exhaust streams with desirable products. A rotary reactor design with micro-channel structure was developed in the Reacting Gas Dynamics Lab (RGDL) at MIT, which exhibits superior performance over conversional designs. Preliminary simulation identified OC redox kinetics and material characteristics as keys to the success of CL technology. This thesis examines the fundamentals of the reduction and oxidation (redox) processes with the aim of achieving fast and reliable reaction kinetics for CL applications. Experiments are conducted in a button-cell fixed-bed reactor with an on-line mass spectrometer. The timeresolved kinetics are modeled with consideration of thermodynamics, surface chemistry, transport mechanism, and structural evolution. Our approach, combining well-controlled experiment and detailed kinetics modeling, enables a new methodology for identifying the rate-limiting mechanism, examining the defect electrochemistry, and designing alternative materials for chemical-looping technology. Redox study with nickel thin foils reveals that structural evolution is the determining factor. Nickel oxidation starts via nucleation of oxide grains, which overlap and annihilate the fast diffusion paths. The model shows that the reaction is limited by the decreasing ionic diffusivity. To achieve practical redox repeatability, NiO fine particles supported on YSZ nanopowder is tested, and superior kinetics and cyclic stability are observed. Fast oxygen exchange is achieved from 500 to 1000°C with sufficient utilization of the carrying capacity within 1 min. Improvement is attributed to the enhanced ionic diffusivity with YSZ. The use of ceria nanopowder exhibits an order of magnitude H2 production rate improvement as compared to the state-of-the-art. Ceria reduction is slow with a threshold temperature of 700°C. The model reveals that the charge transfer is the rate-determining step for H2 production. Improving H2 splitting requires: (i) reducing the defect formation enthalpy, and (ii) accelerating charge-transfer. The addition of Zr lowers the threshold temperature to 650°C with 60% improvement in the rates, resulting from 40% decrease in the defect formation enthalpy. Doping ceria with Pr 3+ further lowers the threshold temperature to 600°C while doubling the peak rate. The model reveals that the high concentration of surface defects achieved from either approach promotes adsorbate formation, thus accelerating the splitting steps. Similar conclusions are obtained for CO2 splitting. Using the derived kinetics, H2-syngas co-production with CH4 as fuel is examined. Two important stages are identified: the formation of the complete products on oxidized surface, and syngas on the reduced surface. CH4 reduction is found to be rate-limited by the slow fuel cracking reaction. To accelerate the kinetics, a novel perovskite-nickel composite OC is examined, in which nickel effectively catalyzes reduction, leading to an order of magnitude faster kinetics at 600-700°C. This project has clearly demonstrated that using novel materials, CL technology can provide an efficient solution to oxy-combustion based CO2 capture, and H2/syngas co-production. Specifically, the use of NiO/YSZ achieves fast kinetics, robust stability and sufficient OC utilization from 500 to 1000°C, enabling complete CO2 capture with minimum energy penalty. The ceria-, and perovskite-based OCs exhibit over an order-of-magnitude faster kinetics compared to the state-of-the-art, enabling improved H2 production/CO 2 reduction efficiency isothermally at 600-700°C. In-depth understanding gained on the redox fundamentals will shed light on the design and fabrication of new materials as well as optimization of the CL applications.
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.
This document is the final report for the project titled "Chemical Looping Gasification for Hydrogen Enhanced Syngas Production with In-Situ CO2 Capture" under award number FE0012136 for the performance period 10/01/2013 to 12/31/2014. This project investigates the novel Ohio State chemical looping gasification technology for high efficiency, cost efficiency coal gasification for IGCC and methanol production application. The project developed an optimized oxygen carrier composition, demonstrated the feasibility of the concept and completed cold-flow model studies. WorleyParsons completed a techno-economic analysis which showed that for a coal only feed with carbon capture, the OSU CLG technology reduced the methanol required selling price by 21%, lowered the capital costs by 28%, increased coal consumption efficiency by 14%. Further, using the Ohio State Chemical Looping Gasification technology resulted in a methanol required selling price which was lower than the reference non-capture case.
Energy Storage and Conversion Materials describes the application of inorganic materials in the storage and conversion of energy.
The gradual increase of population and the consequential rise in the energy demands in the recent years have led to the overwhelming use of fossil fuels. Hydrogen has recently gained substantial interest because of its outstanding features to be used as clean energy carrier and energy vector. Moreover, hydrogen appears to be an effective alternative to tackle the issues of energy security and greenhouse gas emissions given that it is widely recognized as a clean fuel with high energy capacity. Hydrogen can be produced by various techniques such as thermochemical, hydrothermal, electrochemical, electrolytic, biological and photocatalytic methods as well as hybrid systems. New Dimensions in Production and Utilization of Hydrogen emphasizes on the research, development and innovations in the production and utilization of hydrogen in the industrial biorefining, hydrotreating and hydrogenation technologies, fuel cells, aerospace sector, pharmaceuticals, metallurgy, as well as bio-oil upgrading. Moreover, the supply chain analysis, lifecycle assessment, techno-economic analysis, as well as strengths and threats of global hydrogen market are covered in the book. This book provides many significant insights and scientific findings of key technologies for hydrogen production, storage and emerging applications. The book serves as a reference material for chemical and biochemical engineers, mechanical engineers, physicists, chemists, biologists, biomedical scientists and scholars working in the field of sustainable energy and materials. Discusses the efficient usage of hydrogen as standalone fuel or feedstock in downstream processing Outlines key technologies for hydrogen production and their emerging applications Includes innovative approaches to the research and applications of hydrogen, including hydrotreating technologies, fuel cell vehicles and green fuel synthesis, the aerospace sector, pharmaceuticals, carbon dioxide hydrogenation, and bio-oils upgrading Serves as a reference for chemical, biochemical, and mechanical engineers, physicists, chemists, biologists, and biomedical scientists working in sustainable energy and materials
This book provides a review of worldwide developments in ammonia synthesis catalysts over the last 30 years. It focuses on the new generation of Fe1-xO based catalysts and ruthenium catalysts — both are major breakthroughs for fused iron catalysts. The basic theory for ammonia synthesis is systematically explained, covering topics such as the chemical components, crystal structure, preparation, reduction, performance evaluation, characterization of the catalysts, the mechanism and kinetics of ammonia synthesis reaction. Both theory and practice are combined in this presentation, with emphasis on the research methods, application and exploitation of catalysts.The comprehensive volume includes an assessment of the economic and engineering aspects of ammonia plants based on the performance of catalysts. Recent developments in photo-catalysis, electro-catalysis, biocatalysis and new uses of ammonia are also introduced in this book.The author, Professor Huazhang Liu, has been engaged in research and practice for more than 50 years in this field and was the inventor of the first Fe1-xO based catalysts in the world. He has done a lot of research on Fe3O4 based- and ruthenium based-catalysts, and has published more than 300 papers and obtained 21 patents during his career.
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.
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.