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Fuel quality issues in stationary fuel cell systems.

Description: Fuel cell systems are being deployed in stationary applications for the generation of electricity, heat, and hydrogen. These systems use a variety of fuel cell types, ranging from the low temperature polymer electrolyte fuel cell (PEFC) to the high temperature solid oxide fuel cell (SOFC). Depending on the application and location, these systems are being designed to operate on reformate or syngas produced from various fuels that include natural gas, biogas, coal gas, etc. All of these fuels contain species that can potentially damage the fuel cell anode or other unit operations and processes that precede the fuel cell stack. These detrimental effects include loss in performance or durability, and attenuating these effects requires additional components to reduce the impurity concentrations to tolerable levels, if not eliminate the impurity entirely. These impurity management components increase the complexity of the fuel cell system, and they add to the system's capital and operating costs (such as regeneration, replacement and disposal of spent material and maintenance). This project reviewed the public domain information available on the impurities encountered in stationary fuel cell systems, and the effects of the impurities on the fuel cells. A database has been set up that classifies the impurities, especially in renewable fuels, such as landfill gas and anaerobic digester gas. It documents the known deleterious effects on fuel cells, and the maximum allowable concentrations of select impurities suggested by manufacturers and researchers. The literature review helped to identify the impurity removal strategies that are available, and their effectiveness, capacity, and cost. A generic model of a stationary fuel-cell based power plant operating on digester and landfill gas has been developed; it includes a gas processing unit, followed by a fuel cell system. The model includes the key impurity removal steps to enable predictions of impurity breakthrough, component sizing, ...
Date: February 7, 2012
Creator: Papadias, D.; Ahmed, S. & Kumar, R. (Chemical Sciences and Engineering Division)
Partner: UNT Libraries Government Documents Department

Well-to-wheels analysis of fast pyrolysis pathways with the GREET model.

Description: The pyrolysis of biomass can help produce liquid transportation fuels with properties similar to those of petroleum gasoline and diesel fuel. Argonne National Laboratory conducted a life-cycle (i.e., well-to-wheels [WTW]) analysis of various pyrolysis pathways by expanding and employing the Greenhouse Gases, Regulated Emissions, and Energy Use in Transportation (GREET) model. The WTW energy use and greenhouse gas (GHG) emissions from the pyrolysis pathways were compared with those from the baseline petroleum gasoline and diesel pathways. Various pyrolysis pathway scenarios with a wide variety of possible hydrogen sources, liquid fuel yields, and co-product application and treatment methods were considered. At one extreme, when hydrogen is produced from natural gas and when bio-char is used for process energy needs, the pyrolysis-based liquid fuel yield is high (32% of the dry mass of biomass input). The reductions in WTW fossil energy use and GHG emissions relative to those that occur when baseline petroleum fuels are used, however, is modest, at 50% and 51%, respectively, on a per unit of fuel energy basis. At the other extreme, when hydrogen is produced internally via reforming of pyrolysis oil and when bio-char is sequestered in soil applications, the pyrolysis-based liquid fuel yield is low (15% of the dry mass of biomass input), but the reductions in WTW fossil energy use and GHG emissions are large, at 79% and 96%, respectively, relative to those that occur when baseline petroleum fuels are used. The petroleum energy use in all scenarios was restricted to biomass collection and transportation activities, which resulted in a reduction in WTW petroleum energy use of 92-95% relative to that found when baseline petroleum fuels are used. Internal hydrogen production (i.e., via reforming of pyrolysis oil) significantly reduces fossil fuel use and GHG emissions because the hydrogen from fuel gas or pyrolysis oil (renewable ...
Date: December 1, 2011
Creator: Han, J.; Elgowainy, A.; Palou-Rivera, I.; Dunn, J.B. & Wang, M.Q. (Energy Systems)
Partner: UNT Libraries Government Documents Department

A Distributed Electrochemistry Modeling Tool for Simulating SOFC Performance and Degradation

Description: This report presents a distributed electrochemistry (DEC) model capable of investigating the electrochemistry and local conditions with the SOFC MEA based on the local microstructure and multi-physics. The DEC model can calculate the global current-voltage (I-V) performance of the cell as determined by the spatially varying local conditions through the thickness of the electrodes and electrolyte. The simulation tool is able to investigate the electrochemical performance based on characteristics of the electrode microstructure, such as particle size, pore size, electrolyte and electrode phase volume fractions, and triple-phase-boundary length. It can also investigate performance as affected by fuel and oxidant gas flow distributions and other environmental/experimental conditions such as temperature and fuel gas composition. The long-term objective for the DEC modeling tool is to investigate factors that cause electrode degradation and the decay of SOFC performance which decrease longevity.
Date: October 13, 2011
Creator: Recknagle, Kurtis P.; Ryan, Emily M. & Khaleel, Mohammad A.
Partner: UNT Libraries Government Documents Department

High Purity Hydrogen Production with In-Situ Carbon Dioxide and Sulfur Capture in a Single Stage Reactor

Description: Enhancement in the production of high purity hydrogen (H{sub 2}) from fuel gas, obtained from coal gasification, is limited by thermodynamics of the water gas shift (WGS) reaction. However, this constraint can be overcome by conducting the WGS in the presence of a CO{sub 2}-acceptor. The continuous removal of CO{sub 2} from the reaction mixture helps to drive the equilibrium-limited WGS reaction forward. Since calcium oxide (CaO) exhibits high CO{sub 2} capture capacity as compared to other sorbents, it is an ideal candidate for such a technique. The Calcium Looping Process (CLP) developed at The Ohio State University (OSU) utilizes the above concept to enable high purity H{sub 2} production from synthesis gas (syngas) derived from coal gasification. The CLP integrates the WGS reaction with insitu CO{sub 2}, sulfur and halide removal at high temperatures while eliminating the need for a WGS catalyst, thus reducing the overall footprint of the hydrogen production process. The CLP comprises three reactors - the carbonator, where the thermodynamic constraint of the WGS reaction is overcome by the constant removal of CO{sub 2} product and high purity H{sub 2} is produced with contaminant removal; the calciner, where the calcium sorbent is regenerated and a sequestration-ready CO{sub 2} stream is produced; and the hydrator, where the calcined sorbent is reactivated to improve its recyclability. As a part of this project, the CLP was extensively investigated by performing experiments at lab-, bench- and subpilot-scale setups. A comprehensive techno-economic analysis was also conducted to determine the feasibility of the CLP at commercial scale. This report provides a detailed account of all the results obtained during the project period.
Date: July 31, 2011
Creator: Phalak, Nihar; Ramkumar, Shwetha; Connell, Daniel; Sun, Zhenchao; Yu, Fu-Chen; Deshpande, Niranjani et al.
Partner: UNT Libraries Government Documents Department

Poly(cyclohexadiene)-Based Polymer Electrolyte Membranes for Fuel Cell Applications

Description: The goal of this research project was to create and develop fuel cell membranes having high proton conductivity at high temperatures and high chemical and mechanical durability. Poly(1,3-cyclohexadiene) (PCHD) is of interest as an alternative polymer electrolyte membrane (PEM) material due to its ring-like structure which is expected to impart superior mechanical and thermal properties, and due to the fact that PCHD can readily be incorporated into a range of homopolymer and copolymer structures. PCHD can be aromatized, sulfonated, or fluorinated, allowing for tuning of key performance structure and properties. These factors include good proton transport, hydrophilicity, permeability (including fuel gas impermeability), good mechanical properties, morphology, thermal stability, crystallinity, and cost. The basic building block, 1,3-cyclohexadiene, is a hydrocarbon monomer that could be inexpensively produced on a commercial scale (pricing typical of other hydrocarbon monomers). Optimal material properties will result in novel low cost PEM membranes engineered for high conductivity at elevated temperatures and low relative humidities, as well as good performance and durability. The primary objectives of this project were: (1) To design, synthesize and characterize new non-Nafion PEM materials that conduct protons at low (25-50%) RH and at temperatures ranging from room temperature to 120 C; and (2) To achieve these objectives, a range of homopolymer and copolymer materials incorporating poly(cyclohexadiene) (PCHD) will be synthesized, derivatized, and characterized. These two objectives have been achieved. Sulfonated and crosslinked PCHD homopolymer membranes exhibit proton conductivities similar to Nafion in the mid-RH range, are superior to Nafion at higher RH, but are poorer than Nafion at RH < 50%. Thus to further improve proton conductivity, particularly at low RH, poly(ethylene glycol) (PEG) was incorporated into the membrane by blending and by copolymerization. Conductivity measurements at 120 C over RH ranging from 20 to 100% using the BekkTech protocol showed much improved ...
Date: March 7, 2011
Creator: Mays, Jimmy W.
Partner: UNT Libraries Government Documents Department

Effect of palladium dispersion on the capture of toxic components from fuel gas by palladium-alumina sorbents

Description: The dispersion and location of Pd in alumina-supported sorbents prepared by different methods was found to influence the performance of the sorbents in the removal of mercury, arsine, and hydrogen selenide from a simulated fuel gas. When Pd is well dispersed in the pores of the support, contact interaction with the support is maximized, Pd is less susceptible to poisoning by sulfur. and the sorbent has better long-term activity for adsorption of arsine and hydrogen selenide. but poorer adsorption capacity for Hg. As the contact interaction between Pd and the support is lessened the Pd becomes more susceptible to poisoning by sulfur. resulting in higher capacity for Hg, but poorer long-term performance for adsorption of arsenic and selenium.
Date: January 1, 2011
Creator: Baltrus, J.P.; Granite, E.J.; Rupp, E.C.; Stanko, D.C.; Howard, B. & Pennline, H.W.
Partner: UNT Libraries Government Documents Department

ADVANCED GASIFICATION MERCURY/TRACE METAL CONTROL WITH MONOLITH TRAPS

Description: Two Corning monoliths and a non-carbon-based material have been identified as potential additives for mercury capture in syngas at temperatures above 400°F and pressure of 600 psig. A new Corning monolith formulation, GR-F1-2189, described as an active sample appeared to be the best monolith tested to date. The Corning SR Liquid monolith concept continues to be a strong candidate for mercury capture. Both monolith types allowed mercury reduction to below 5-μg/m3 (~5 ppb), a current U.S. Department of Energy (DOE) goal for trace metal control. Preparation methods for formulating the SR Liquid monolith impacted the ability of the monolith to capture mercury. The Energy & Environmental Research Center (EERC)-prepared Noncarbon Sorbents 1 and 2 appeared to offer potential for sustained and significant reduction of mercury concentration in the simulated fuel gas. The Noncarbon Sorbent 1 allowed sustained mercury reduction to below 5-μg/m3 (~5 ppb). The non-carbon-based sorbent appeared to offer the potential for regeneration, that is, desorption of mercury by temperature swing (using nitrogen and steam at temperatures above where adsorption takes place). A Corning cordierite monolith treated with a Group IB metal offered limited potential as a mercury sorbent. However, a Corning carbon-based monolith containing prereduced metallic species similar to those found on the noncarbon sorbents did not exhibit significant or sustained mercury reduction. EERC sorbents prepared with Group IB and IIB selenide appeared to have some promise for mercury capture. Unfortunately, these sorbents also released Se, as was evidenced by the measurement of H2Se in the effluent gas. All sorbents tested with arsine or hydrogen selenide, including Corning monoliths and the Group IB and IIB metal-based materials, showed an ability to capture arsine or hydrogen selenide at 400°F and 600 psig. Based on current testing, the noncarbon metal-based sorbents appear to be the most effective arsine and hydrogen ...
Date: July 31, 2010
Creator: Musich, Mark A.; Swanson, Michael L.; Dunham, Grant E. & Stanislowski, Joshua J.
Partner: UNT Libraries Government Documents Department

Surface characterizatin of palladium-alumina sorbents for high-temperature capture of mercury and arsenic from fuel gas

Description: Coal gasification with subsequent cleanup of the resulting fuel gas is a way to reduce the impact of mercury and arsenic in the environment during power generation and on downstream catalytic processes in chemical production, The interactions of mercury and arsenic with PdlAl2D3 model thin film sorbents and PdlAh03 powders have been studied to determine the relative affinities of palladium for mercury and arsenic, and how they are affected by temperature and the presence of hydrogen sulfide in the fuel gas. The implications of the results on strategies for capturing the toxic metals using a sorbent bed are discussed.
Date: January 1, 2010
Creator: Baltrus, J.P.; Granite, E.J.; Pennline, H.W.; Stanko, D.; Hamilton, H.; Rowsell, L. et al.
Partner: UNT Libraries Government Documents Department

Subtask 4.2 - Coal Gasification Short Course

Description: Major utilities, independent power producers, and petroleum and chemical companies are intent on developing a fleet of gasification plants primarily because of high natural gas prices and the implementation of state carbon standards, with federal standards looming. Currently, many projects are being proposed to utilize gasification technologies to produce a synthesis gas or fuel gas stream for the production of hydrogen, liquid fuels, chemicals, and electricity. Financing these projects is challenging because of the complexity, diverse nature of gasification technologies, and the risk associated with certain applications of the technology. The Energy & Environmental Research Center has developed a gasification short course that is designed to provide technical personnel with a broad understanding of gasification technologies and issues, thus mitigating the real or perceived risk associated with the technology. Based on a review of research literature, tutorial presentations, and Web sites on gasification, a short course presentation was prepared. The presentation, consisting of about 500 PowerPoint slides, provides at least 7 hours of instruction tailored to an audience's interests and needs. The initial short course is scheduled to be presented September 9 and 10, 2009, in Grand Forks, North Dakota.
Date: June 30, 2009
Creator: Galbreath, Kevin
Partner: UNT Libraries Government Documents Department

Study of metallic materials for solid oxide fuel cell interconnect applications.

Description: Metallic interconnect acts as a gas separator and a gas distributor and therefore, it needs to function adequately in two widely different environments. The interconnect material will be exposed to air on one side and natural gas or coal-derived synthesis gas on the other side. The viable material for the interconnect application must be resistant not only to oxidation but also carburization in hydrocarbon containing low-oxygen environments. In addition, the scales that develop on the exposed surfaces must possess adequate electrical conductivity for them to function as current leads over long service life of the fuel cell. This report addresses five topics of interest for the development of metallic interconnects with adequate performance in fuel cells for long service life. The research conducted over the years and the conclusions reached were used to identify additional areas of research on materials for improved performance of components, especially metallic interconnects, in the complex fuel cell environments. This report details research conducted in the following areas: measurement of area specific electrical resistivity, corrosion performance in dual gas environments by experiments using alloy 446, long term corrosion performance of ferritic and austenitic alloys in hydrogen and methane-reformed synthesis fuel-gas environments, approaches to reduce the area resistance of metallic interconnect, and reduction of electrical resistivity of alumina scales on metallic interconnect. Based on the key requirements for metallic interconnects and the data developed on the corrosion behavior of candidate materials in meeting those requirements, several areas are recommended for further research to develop metallic interconnects with acceptable and reliable long-term performance in solid oxide fuel cells.
Date: April 24, 2009
Creator: Natesan, K. & Zeng, Z.
Partner: UNT Libraries Government Documents Department

Subtask 2.8 - Control of Trace Elements in Gasification Systems

Description: Detailed investigations were carried out to investigate the removal of mercury using a variety of substrates at elevated temperature under reducing conditions. Sorbents tested mainly comprised 6A, 7A, 1B, 2B, and metals from the periodic table. The new high-surface halogen-treated carbon sorbents performed exceptionally well on the bench scale at relatively high temperatures (400 C). The new sorbents could be incorporated into a gas cleanup technology for fuel gas, where the gas is cooled to medium temperatures. Other work in this task focused on halogen-containing sorbents prepared on a carbon support. Similar sorbents had been previously found to be superior for mercury in flue gas. All granular sorbents were conducted in fixed beds heated at 350 and 400 C with 10 vol% hydrogen in a nitrogen stream containing 34.8 {mu}g/m{sup 3} of Hg{sup 0}.
Date: March 28, 2009
Creator: Swanson, Michael
Partner: UNT Libraries Government Documents Department

Subtask 7.4 - Power River Basin Subbituminous Coal-Biomass Cogasification Testing in a Transport Reactor

Description: The U.S. Department of Energy (DOE) National Energy Technology Laboratory Office of Coal and Environmental Systems has as its mission to develop advanced gasification-based technologies for affordable, efficient, zero-emission power generation. These advanced power systems, which are expected to produce near-zero pollutants, are an integral part of DOE's Vision 21 Program. DOE has also been developing advanced gasification systems that lower the capital and operating costs of producing syngas for chemical production. A transport reactor has shown potential to be a low-cost syngas producer compared to other gasification systems since its high-throughput-per-unit cross-sectional area reduces capital costs. This work directly supports the Power Systems Development Facility utilizing the Kellogg Brown and Root transport reactor located at the Southern Company Services Wilsonville, Alabama, site. Over 3600 hours of operation on 17 different coals ranging from bituminous to lignite along with a petroleum coke has been completed to date in the pilot-scale transport reactor development unit (TRDU) at the Energy & Environmental Research Center (EERC). The EERC has established an extensive database on the operation of these various fuels in both air- and oxygen-blown modes utilizing a pilot-scale transport reactor gasifier. This database has been useful in determining the effectiveness of design changes on an advanced transport reactor gasifier and for determining the performance of various feedstocks in a transport reactor. The effects of different fuel types on both gasifier performance and the operation of the hot-gas filter system have been determined. It has been demonstrated that corrected fuel gas heating values ranging from 90 to 130 Btu/scf have been achieved in air-blown mode, while heating values up to 230 Btu/scf on a dry basis have been achieved in oxygen-blown mode. Carbon conversions up to 90% have also been obtained and are highly dependent on the oxygen-coal ratio. Higher-reactivity (low-rank) coals appear ...
Date: March 1, 2009
Creator: Swanson, Michael & Laudal, Daniel
Partner: UNT Libraries Government Documents Department

Production of Substitute Natural Gas from Coal

Description: The goal of this research program was to develop and demonstrate a novel gasification technology to produce substitute natural gas (SNG) from coal. The technology relies on a continuous sequential processing method that differs substantially from the historic methanation or hydro-gasification processing technologies. The thermo-chemistry relies on all the same reactions, but the processing sequences are different. The proposed concept is appropriate for western sub-bituminous coals, which tend to be composed of about half fixed carbon and about half volatile matter (dry ash-free basis). In the most general terms the process requires four steps (1) separating the fixed carbon from the volatile matter (pyrolysis); (2) converting the volatile fraction into syngas (reforming); (3) reacting the syngas with heated carbon to make methane-rich fuel gas (methanation and hydro-gasification); and (4) generating process heat by combusting residual char (combustion). A key feature of this technology is that no oxygen plant is needed for char combustion.
Date: January 31, 2009
Creator: Lucero, Andrew
Partner: UNT Libraries Government Documents Department

Fuel-Flexible Combustion System for Co-production Plant Applications

Description: Future high-efficiency, low-emission generation plants that produce electric power, transportation fuels, and/or chemicals from fossil fuel feed stocks require a new class of fuel-flexible combustors. In this program, a validated combustor approach was developed which enables single-digit NO{sub x} operation for a future generation plants with low-Btu off gas and allows the flexibility of process-independent backup with natural gas. This combustion technology overcomes the limitations of current syngas gas turbine combustion systems, which are designed on a site-by-site basis, and enable improved future co-generation plant designs. In this capacity, the fuel-flexible combustor enhances the efficiency and productivity of future co-production plants. In task 2, a summary of market requested fuel gas compositions was created and the syngas fuel space was characterized. Additionally, a technology matrix and chemical kinetic models were used to evaluate various combustion technologies and to select two combustor concepts. In task 4 systems analysis of a co-production plant in conjunction with chemical kinetic analysis was performed to determine the desired combustor operating conditions for the burner concepts. Task 5 discusses the experimental evaluation of three syngas capable combustor designs. The hybrid combustor, Prototype-1 utilized a diffusion flame approach for syngas fuels with a lean premixed swirl concept for natural gas fuels for both syngas and natural gas fuels at FA+e gas turbine conditions. The hybrid nozzle was sized to accommodate syngas fuels ranging from {approx}100 to 280 btu/scf and with a diffusion tip geometry optimized for Early Entry Co-generation Plant (EECP) fuel compositions. The swozzle concept utilized existing GE DLN design methodologies to eliminate flow separation and enhance fuel-air mixing. With changing business priorities, a fully premixed natural gas & syngas nozzle, Protoytpe-1N, was also developed later in the program. It did not have the diluent requirements of Prototype-1 and was demonstrated at targeted gas turbine conditions. ...
Date: December 31, 2008
Creator: Haynes, Joel; Brumberg, Justin; Iyer, Venkatraman; Janssen, Jonathan; Lacy, Ben; Mosbacher, Matt et al.
Partner: UNT Libraries Government Documents Department

Effect of Coal Contaminants on Solid Oxide Fuel System Performance and Service Life

Description: The U.S. Department of Energy's SECA program envisions the development of high-efficiency, low-emission, CO{sub 2} sequestration-ready, and fuel-flexible technology to produce electricity from fossil fuels. One such technology is the integrated gasification-solid oxide fuel cell (SOFC) that produces electricity from the gas stream of a coal gasifier. SOFCs have high fuel-to-electricity conversion efficiency, environmental compatibility (low NO{sub x} production), and modularity. Naturally occurring coal has many impurities and some of these impurities end in the fuel gas stream either as a vapor or in the form of fine particulate matter. Establishing the tolerance limits of SOFCs for contaminants in the coal-derived gas will allow proper design of the fuel feed system that will not catastrophically damage the SOFC or allow long-term cumulative degradation. The anodes of Ni-cermet-based SOFCs are vulnerable to degradation in the presence of contaminants that are expected to be present in a coal-derived fuel gas stream. Whereas the effects of some contaminants such as H{sub 2}S, NH{sub 3} and HCl have been studied, the effects of other contaminants such as As, P, and Hg have not been ascertained. The primary objective of this study was to determine the sensitivity of the performance of solid oxide fuel cells to trace level contaminants present in a coal-derived gas stream in the temperature range 700 to 900 C. The results were used to assess catastrophic damage risk and long-term cumulative effects of the trace contaminants on the lifetime expectancy of SOFC systems fed with coal-derived gas streams.
Date: September 30, 2008
Creator: Krishnan, Gopala; Jayaweera, P.; Bao, J.; Perez, J.; Lau, K. H.; Hornbostel, M. et al.
Partner: UNT Libraries Government Documents Department

Advanced High-Temperature, High-Pressure Transport Reactor Gasification

Description: The U.S. Department of Energy (DOE) National Energy Technology Laboratory Office of Coal and Environmental Systems has as its mission to develop advanced gasification-based technologies for affordable, efficient, zero-emission power generation. These advanced power systems, which are expected to produce near-zero pollutants, are an integral part of DOE's Vision 21 Program. DOE has also been developing advanced gasification systems that lower the capital and operating costs of producing syngas for chemical production. A transport reactor has shown potential to be a low-cost syngas producer compared to other gasification systems since its high-throughput-per-unit cross-sectional area reduces capital costs. This work directly supports the Power Systems Development Facility utilizing the KBR transport reactor located at the Southern Company Services Wilsonville, Alabama, site. Over 2800 hours of operation on 11 different coals ranging from bituminous to lignite along with a petroleum coke has been completed to date in the pilot-scale transport reactor development unit (TRDU) at the Energy & Environmental Research Center (EERC). The EERC has established an extensive database on the operation of these various fuels in both air-blown and oxygen-blown modes utilizing a pilot-scale transport reactor gasifier. This database has been useful in determining the effectiveness of design changes on an advanced transport reactor gasifier and for determining the performance of various feedstocks in a transport reactor. The effects of different fuel types on both gasifier performance and the operation of the hot-gas filter system have been determined. It has been demonstrated that corrected fuel gas heating values ranging from 90 to 130 Btu/scf have been achieved in air-blown mode, while heating values up to 230 Btu/scf on a dry basis have been achieved in oxygen-blown mode. Carbon conversions up to 95% have also been obtained and are highly dependent on the oxygen-coal ratio. Higher-reactivity (low-rank) coals appear to perform better ...
Date: March 31, 2008
Creator: Swanson, Michael & Laudal, Daniel
Partner: UNT Libraries Government Documents Department

Ultra Low NOx Catalytic Combustion for IGCC Power Plants

Description: In order to meet DOE's goals of developing low-emissions coal-based power systems, PCI has further developed and adapted it's Rich-Catalytic Lean-burn (RCL{reg_sign}) catalytic reactor to a combustion system operating on syngas as a fuel. The technology offers ultra-low emissions without the cost of exhaust after-treatment, with high efficiency (avoidance of after-treatment losses and reduced diluent requirements), and with catalytically stabilized combustion which extends the lower Btu limit for syngas operation. Tests were performed in PCI's sub-scale high-pressure (10 atm) test rig, using a two-stage (catalytic then gas-phase) combustion process for syngas fuel. In this process, the first stage consists of a fuel-rich mixture reacting on a catalyst with final and excess combustion air used to cool the catalyst. The second stage is a gas-phase combustor, where the air used for cooling the catalyst mixes with the catalytic reactor effluent to provide for final gas-phase burnout and dilution to fuel-lean combustion products. During testing, operating with a simulated Tampa Electric's Polk Power Station syngas, the NOx emissions program goal of less than 0.03 lbs/MMBtu (6 ppm at 15% O{sub 2}) was met. NOx emissions were generally near 0.01 lbs/MMBtu (2 ppm at 15% O{sub 2}) (PCI's target) over a range on engine firing temperatures. In addition, low emissions were shown for alternative fuels including high hydrogen content refinery fuel gas and low BTU content Blast Furnace Gas (BFG). For the refinery fuel gas increased resistance to combustor flashback was achieved through preferential consumption of hydrogen in the catalytic bed. In the case of BFG, stable combustion for fuels as low as 88 BTU/ft{sup 3} was established and maintained without the need for using co-firing. This was achieved based on the upstream catalytic reaction delivering a hotter (and thus more reactive) product to the flame zone. The PCI catalytic reactor was also ...
Date: March 31, 2008
Creator: Etemad, Shahrokh; Baird, Benjamin; Alavandi, Sandeep & Pfefferle, William
Partner: UNT Libraries Government Documents Department

Surface characterization of Pd/Al2O3 sorbents for mercury capture from fuel gas

Description: The surface composition of a series of Pd/alumina sorbents has been characterized to better understand the factors influencing their ability to adsorb mercury from fuel gas. Both a temperature effect and a dispersion effect were found. Maximum adsorption of Hg occurred at the -lowest temperature tested, 204°C, and decreased with increasing temperatures. Maximum adsorption of Hg on a per-atom basis of Pd is observed at low loadings of Pd ( < 8.5% Pd) due to better dispersion of Pd at those loadings; a change in its partitioning occurs at higher loadings. The presence of H2S 'in the fuel gas acts to promote the adsorption of Hg through its association with Hg in the Pd lattice.
Date: January 1, 2008
Creator: Baltrus, J.P.; Granite, E.J.; Stanko, D.C. & Pennline, H.W.
Partner: UNT Libraries Government Documents Department

Post-Combustion and Pre-Combustion CO2 Capture Solid Sorbents

Description: Combustion of fossil fuels is one of the major sources of the greenhouse gas CO2. Pressure swing adsorption/sorption (PSA/PSS) and temperature swing adsorption/sorption (TSA/TSS) are some of the potential techniques that could be utilized for removal of CO2 from fuel gas streams. It is very important to develop sorbents to remove CO2 from fuel gas streams that are applicable for a wide range of temperatures. NETL researchers have developed novel CO2 capture sorbents for low, moderate, and high temperature applications. A novel liquid impregnated solid sorbent was developed for CO2 removal in the temperature range of ambient to 60 °C. The sorbent is regenerable at 60 – 80 °C. The sorbent formulations were prepared to be suitable for various reactor configurations (i.e., fixed and fluidized bed). Minimum fluidization gas velocities were also determined. Multi-cycle tests conducted in an atmospheric bench scale reactor with simulated flue gas indicated that the sorbent retains its CO2 sorption capacity with a CO2 removal efficiency of approximately 99% and was unaffected by presence of water vapor. The sorbent was subsequently commercially prepared by Süd Chemie to determine the viability of the sorbent for mass production. Subsequent testing showed that the commercially-synthesized sorbent possesses the same properties as the lab-synthesized equivalent. An innovative solid sorbent containing mixture of alkali earth and alkali compounds was developed for CO2 removal at 200 – 315°C from high pressure gas streams suitable for IGCC systems. The sorbent showed very high capacity for CO2 removal from a gas streams containing 28% CO2 at 200 °C and at 20 atm during a lab scale reactor test. This sorbent can be regenerated at 20 atm and at 375 °C utilizing a gas stream containing steam. High pressure enhanced the CO2 sorption process. Bench scale testing showed consistent capacities and regenerability. A unique high ...
Date: November 1, 2007
Creator: Siriwardane, R.V.; Stevens, R.W. & Robinson, Clark
Partner: UNT Libraries Government Documents Department

Carbon Dioxide Capture and Separation Techniques for Gasification-based Power Generation Point Sources

Description: The capture/separation step for carbon dioxide (CO2) from large-point sources is a critical one with respect to the technical feasibility and cost of the overall carbon sequestration scenario. For large-point sources, such as those found in power generation, the carbon dioxide capture techniques being investigated by the in-house research area of the National Energy Technology Laboratory possess the potential for improved efficiency and reduced costs as compared to more conventional technologies. The investigated techniques can have wide applications, but the research has focused on capture/separation of carbon dioxide from flue gas (post-combustion from fossil fuel-fired combustors) and from fuel gas (precombustion, such as integrated gasification combined cycle or IGCC). With respect to fuel gas applications, novel concepts are being developed in wet scrubbing with physical absorption; chemical absorption with solid sorbents; and separation by membranes. In one concept, a wet scrubbing technique is being investigated that uses a physical solvent process to remove CO2 from fuel gas of an IGCC system at elevated temperature and pressure. The need to define an ideal solvent has led to the study of the solubility and mass transfer properties of various solvents. Pertaining to another separation technology, fabrication techniques and mechanistic studies for membranes separating CO2 from the fuel gas produced by coal gasification are also being performed. Membranes that consist of CO2-philic ionic liquids encapsulated into a polymeric substrate have been investigated for permeability and selectivity. Finally, dry, regenerable processes based on sorbents are additional techniques for CO2 capture from fuel gas. An overview of these novel techniques is presented along with a research progress status of technologies related to membranes and physical solvents.
Date: June 1, 2007
Creator: Pennline, H. W.; Luebke, D. R.; Jones, K. L.; Morsi, B. I.; Heintz, Y. J. & Ilconich, J. B.
Partner: UNT Libraries Government Documents Department

Optical Fiber Chemical Sensor with Sol-Gel Derived Refractive Material as Transducer for High Temperature Gas Sensing in Clean Coal Technology

Description: The chemistry of sol-gel derived silica and refractive metal oxide has been systematically studied. Sol-gel processes have been developed for preparing porous silica and semiconductor metal oxide materials. Micelle/reversed micelle techniques have been developed for preparing nanometer sized semiconductor metal oxides and noble metal particles. Techniques for doping metal ions, metal oxides and nanosized metal particles into porous sol-gel material have also been developed. Optical properties of sol-gel derived materials in ambient and high temperature gases have been studied by using fiber optic spectroscopic techniques, such as fiber optic ultraviolet/visible absorption spectrometry, fiber optic near infrared absorption spectrometry and fiber optic fluorescence spectrometry. Fiber optic spectrometric techniques have been developed for investigating the optical properties of these sol-gel derived materials prepared as porous optical fibers or as coatings on the surface of silica optical fibers. Optical and electron microscopic techniques have been used to observe the microstructure, such as pore size, pore shape, sensing agent distribution, of sol-gel derived material, as well as the size and morphology of nanometer metal particle doped in sol-gel derived porous silica, the nature of coating of sol-gel derived materials on silica optical fiber surface. In addition, the chemical reactions of metal ion, nanostructured semiconductor metal oxides and nanometer sized metal particles with gas components at room temperature and high temperatures have also been investigated with fiber optic spectrometric methods. Three classes of fiber optic sensors have been developed based on the thorough investigation of sol-gel chemistry and sol-gel derived materials. The first group of fiber optic sensors uses porous silica optical fibers doped with metal ions or metal oxide as transducers for sensing trace NH{sub 3} and H{sub 2}S in high temperature gas samples. The second group of fiber optic sensors uses sol-gel derived porous silica materials doped with nanometer particles of noble metals ...
Date: December 31, 2006
Creator: Tao, Shiquan
Partner: UNT Libraries Government Documents Department

Systems Analyses of Advanced Brayton Cycles For High Efficiency Zero Emission Plants

Description: Table 1 shows that the systems efficiency, coal (HHV) to power, is 35%. Table 2 summarizes the auxiliary power consumption within the plant. Thermoflex was used to simulate the power block and Aspen Plus the balance of plant. The overall block flow diagram is presented in Figure A1.3-1 and the key unit process flow diagrams are shown in subsequent figures. Stream data are given in Table A1.3-1. Equipment function specifications are provided in Tables A1.3-2 through 17. The overall plant scheme consists of a cryogenic air separation unit supplying 95% purity O{sub 2} to GE type high pressure (HP) total quench gasifiers. The raw gas after scrubbing is treated in a sour shift unit to react the CO with H{sub 2}O to form H{sub 2} and CO{sub 2}. The gas is further treated to remove Hg in a sulfided activated carbon bed. The syngas is desulfurized and decarbonized in a Selexol acid gas removal unit and the decarbonized syngas after humidification and preheat is fired in GE 7H type steam cooled gas turbines. Intermediate pressure (IP) N{sub 2} from the ASU is also supplied to the combustors of the gas turbines as additional diluent for NOx control. A portion of the air required by the ASU is extracted from the gas turbines. The plant consists of the following major process units: (1) Air Separation Unit (ASU); (2) Gasification Unit; (3) CO Shift/Low Temperature Gas Cooling (LTGC) Unit; (4) Acid Gas Removal Unit (AGR) Unit; (5) Fuel Gas Humidification Unit; (6) Carbon Dioxide Compression/Dehydration Unit; (7) Claus Sulfur Recovery/Tail Gas Treating Unit (SRU/TGTU); and (8) Power Block.
Date: November 1, 2006
Creator: Rao, A. D.; Francuz, J.; Liao, H.; Verma, A. & Samuelsen, G. S.
Partner: UNT Libraries Government Documents Department

Enhanced Hydrogen Production Integrated with CO2 Separation in a Single-Stage

Description: Enhancement in the production of high purity hydrogen from fuel gas, obtained from coal gasification, is limited by thermodynamics of the Water Gas Shift Reaction. However, this constraint can be overcome by concurrent water-gas shift (WGS) and carbonation reactions to enhance H{sub 2} production by incessantly driving the equilibrium-limited WGS reaction forward and in-situ removing the CO2 product from the gas mixture. The spent sorbent is then regenerated by calcining it to produce a pure stream of CO{sub 2} and CaO which can be reused. However while performing the cyclic carbonation and calcination it was observed that the CO{sub 2} released during the in-situ calcination causes the deactivation of the iron oxide WGS catalyst. Detailed understanding of the iron oxide phase diagram helped in developing a catalyst pretreatment procedure using a H{sub 2}/H{sub 2}O system to convert the deactivated catalyst back to its active magnetite (Fe{sub 3}O{sub 4}) form. The water gas shift reaction was studied at different temperatures, different steam to carbon monoxide ratios (S/C) 3:1, 2:1, 1:1 and different total pressures ranging from 0-300 psig. The combined water gas shift and carbonation reaction was investigated at temperatures ranging from 600-700C, S/C ratio of 3:1 to 1:1 and at different pressures of 0-300 psig and the calcium looping process was found to produce high purity hydrogen with in-situ CO{sub 2} capture.
Date: September 30, 2006
Creator: Iyer, Mahesh; Ramkumar, Shwetha & Fan, Liang-Shih
Partner: UNT Libraries Government Documents Department

Synthesis and Characterization of CO- and H2S-Tolerant Electrocatalysts for PEM Fuel Cell

Description: The present state-of-art Proton Exchange Membrane Fuel Cell (PEMFC) technology is based on platinum (Pt) as a catalyst for both the fuel (anode) and air (cathode) electrodes. This catalyst is highly active but susceptible to poisoning by CO, which may be present in the H{sub 2}-fuel used or may be introduced during the fuel processing. Presence of trace amount of CO and H{sub 2}S in the H{sub 2}-fuel poisons the anode irreversibly and decreases the performance of the PEMFCs. In an effort to reduce the Pt-loading and improve the PEMFC performance, we propose to synthesize a number of Pt-based binary, ternary, and quaternary electrocatalysts using Ru, Mo, Ir, Ni, and Co as a substitute for Pt. By fine-tuning the metal loadings and compositions of candidate electrocatalysts, we plan to minimize the cost and optimize the catalyst activity and performance in PEMFC. The feasibility of the novel electrocatalysts will be demonstrated in the proposed effort with gas phase CO and H{sub 2}S concentrations typical of those found in reformed fuel gas with coal/natural gas/methanol feedstocks. In this work binary, ternary, and quaternary platinum-based electrocatalysts were synthesized for the purpose of lowering the cost and increasing the CO tolerance of the membrane electrode assembly (MEA) in the fuel cell. The metals Ru, Mo, W, Ir, Co and Se were alloyed with platinum on a carbon support using a modified reduction method. These catalysts were fabricated into MEAs and evaluated for electrical performance and CO tolerance with polarization experiments. The quaternary system Pt/Ru/Mo/Ir system is the most CO tolerant in the PEMFC and has a low total metal loading of 0.4 mg/cm{sup 2} in the electrode of the cell.
Date: September 30, 2006
Creator: Ilias, Shamsuddin
Partner: UNT Libraries Government Documents Department