An investigation of the kinetics of CO2 uptake by a synthetic calcium based sorbent

This study examines the kinetics of carbonation by CO2 at temperatures of ca. 750 °C of a synthetic sorbent composed of 15 wt% mayenite (Ca12Al14O33) and CaO, designated HA-85-850, and draws comparisons with the carbonation of a calcined limestone. In-situ XRD has verified the inertness of mayenite, which neither interacts with the active CaO nor does it significantly alter the CaO carbonation–calcination equilibrium. An overlapping grain model was developed to predict the rate and extent of carbonation of HA-85-850 and limestone. In the model, the initial microstructure of the sorbent was defined by a discretised grain size distribution, assuming spherical grains. The initial input to the model – the size distribution of grains – was a fitted parameter, which was in good agreement with measurements made with mercury porosimetry and by the analysis of SEM images of sectioned particles. It was found that the randomly overlapping spherical grain assumption offered great simplicity to the model, despite its approximation to the actual porous structure within a particle. The model was able to predict the performance of the materials well and, particularly, was able to account for changes in rate and extent of reaction as the structure evolved after various numbers of cycles of calcination and carbonation.

Experimental investigation of turbine stator well rim seal, reingestion and interstage seal flows using gas concentration techniques and displacement measurements

Gas turbine engine performance requires effective and reliable internal cooling over the duty cycle of the engine. Life predictions for rotating components subject to the main gas path temperatures are vital. This demands increased precision in the specification of the internal air system flows which provide turbine stator well cooling and sealing. This in turn requires detailed knowledge of the flow rates through rim seals and interstage labyrinth seals. Knowledge of seal movement and clearances at operating temperatures is of great importance when prescribing these flows. A test facility has been developed at the University of Sussex, incorporating a two stage turbine rated at 400 kW with an individual stage pressure ratio of 1.7:1. The mechanical design of the test facility allows internal cooling geometry to be rapidly re-configured, while cooling flow rates of between 0.71 CW, ENT and 1.46 C W, ENT, may be set to allow ingress or egress dominated cavity flows. The main annulus and cavity conditions correspond to in cavity rotational Reynolds numbers of 1.71×106< Reφ <1.93×106. Displacement sensors have been used to establish hot running seal clearances over a range of stator well flow conditions, allowing realistic flow rates to be calculated. Additionally, gas seeding techniques have been developed, where stator well and main annulus flow interactions are evaluated by measuring changes in gas concentration. Experiments have been performed which allow rim seal and re-ingestion flows to be quantified. It will be shown that this work develops the measurement of stator well cooling flows and provides data suitable for the validation of improved thermo-mechanical and CFD codes, beneficial to the engine design process. Copyright © 2011 by Rolls-Royce plc.

Dynamic behaviour of gas jets in laser cutting

The efficiency and overall quality of a laser cutting operation is highly dependent on the assist gas parameters. The desire to cut thicker material has led to the observation of small process operating windows for thicker sections. The gas jet delivery and subsequent dynamical behaviour have significant effects on the cutting operation as the sample thickness increases. To date, few workers have examined the dynamical behaviour of the gas jet. This paper examines the characteristics of oxygen gas jets during CO2 laser cutting of steel. Particular emphasis is placed on the mass transfer effects that are operating within the kerf. Oxygen concentration levels within a model kerf are measured for various laser cutting set-ups. The results show a substantial reduction in oxygen concentration within the kerf. A system for oxygen concentration maintenance is described and cutting results from this system are compared with conventional techniques for cutting steels in the range 10 to 20mm thick. A theoretical analysis of turbulent mass transfer within a kerf is presented and compared with experiment.

A 5-step reduced mechanism for combustion of CO/H2/H2O/CH4/CO2 mixtures with low hydrogen/methane and high H2O content

In this study a 5-step reduced chemical kinetic mechanism involving nine species is developed for combustion of Blast Furnace Gas (BFG), a multi-component fuel containing CO/H2/CH4/CO2, typically with low hydrogen, methane and high water fractions, for conditions relevant for stationary gas-turbine combustion. This reduced mechanism is obtained from a 49-reaction skeletal mechanism which is a modified subset of GRI Mech 3.0. The skeletal and reduced mechanisms are validated for laminar flame speeds, ignition delay times and flame structure with available experimental data, and using computational results with a comprehensive set of elementary reactions. Overall, both the skeletal and reduced mechanisms show a very good agreement over a wide range of pressure, reactant temperature and fuel mixture composition. © 2012 The Combustion Institute..

A high performance oxygen storage material for chemical looping processes with CO2 capture

Chemical looping combustion (CLC) is a novel combustion technology that involves cyclic reduction and oxidation of oxygen storage materials to provide oxygen for the combustion of fuels to CO2 and H2O, whilst giving a pure stream of CO2 suitable for sequestration or utilisation. Here, we report a method for preparing of oxygen storage materials from layered double hydroxides (LDHs) precursors and demonstrate their applications in the CLC process. The LDHs precursor enables homogeneous mixing of elements at the molecular level, giving a high degree of dispersion and high-loading of active metal oxide in the support after calcination. Using a Cu-Al LDH precursor as a prototype, we demonstrate that rational design of oxygen storage materials by material chemistry significantly improved the reactivity and stability in the high temperature redox cycles. We discovered that the presence of sodium-containing species were effective in inhibiting the formation of copper aluminates (CuAl2O4 or CuAlO 2) and stabilising the copper phase in an amorphous support over multiple redox cycles. A representative nanostructured Cu-based oxygen storage material derived from the LDH precursor showed stable gaseous O2 release capacity (∼5 wt%), stable oxygen storage capacity (∼12 wt%), and stable reaction rates during reversible phase changes between CuO-Cu 2O-Cu at high temperatures (800-1000 °C). We anticipate that the strategy can be extended to manufacture a variety of metal oxide composites for applications in novel high temperature looping cycles for clean energy production and CO2 capture. © The Royal Society of Chemistry 2013.

Concentration dependence of the Er3+ visible and infrared luminescence in Y2-x Erx O3 thin films on Si

Y2-x Erx O3 thin films, with x varying between 0 and 0.72, have been successfully grown on crystalline silicon (c-Si) substrates by radio-frequency magnetron cosputtering of Y2 O 3 and Er2 O3 targets. As-deposited films are polycrystalline, showing the body-centered cubic structure of Y2 O3, and show only a slight lattice parameter contraction when x is increased, owing to the insertion of Er ions. All the films exhibit intense Er-related optical emission at room temperature both in the visible and infrared regions. By studying the optical properties for different excitation conditions and for different Er contents, all the mechanisms (i.e., cross relaxations, up-conversions, and energy transfers to impurities) responsible for the photoluminescence (PL) emission have been identified, and the existence of two different well-defined Er concentration regimes has been demonstrated. In the low concentration regime (x up to 0.05, Er-doped regime), the visible PL emission reaches its highest intensity, owing to the influence of up-conversions, thus giving the possibility of using Y2-x Er x O3 films as an up-converting layer in the rear of silicon solar cells. However, most of the excited Er ions populate the first two excited levels 4I11/2 and 4I13/2, and above a certain excitation flux a population inversion condition between the former and the latter is achieved, opening the route for the realization of amplifiers at 2.75 μm. Instead, in the high concentration regime (Er-compound regime), an increase in the nonradiative decay rates is observed, owing to the occurrence of cross relaxations or energy transfers to impurities. As a consequence, the PL emission at 1.54 μm becomes the most intense, thus determining possible applications for Y2-x Erx O 3 as an infrared emitting material. © 2009 American Institute of Physics.

The roles of energy and material efficiency in meeting steel industry CO2 targets.

Identifying strategies for reducing greenhouse gas emissions from steel production requires a comprehensive model of the sector but previous work has either failed to consider the whole supply chain or considered only a subset of possible abatement options. In this work, a global mass flow analysis is combined with process emissions intensities to allow forecasts of future steel sector emissions under all abatement options. Scenario analysis shows that global capacity for primary steel production is already near to a peak and that if sectoral emissions are to be reduced by 50% by 2050, the last required blast furnace will be built by 2020. Emissions reduction targets cannot be met by energy and emissions efficiency alone, but deploying material efficiency provides sufficient extra abatement potential.

Experimental investigation of dynamic response of acoustically forced turbulent premixed CH4/CO2/air flames

Increasing demand for energy and continuing increase in environmental as well as financial cost of use of fossil fuels drive the need for utilization of fuels from sustainable sources for power generation. Development of fuel-flexible combustion systems is vital in enabling the use of sustainable fuels. It is also important that these sustainable combustion systems meet the strict governmental emission legislations. Biogas is considered as one of the viable sustainable fuels that can be used to power modern gas turbines: However, the change in chemical, thermal and transport properties as well as change in Wobbe index due to the variation of the fuel constituents can have a significant effect on the performance of the combustor. It is known that the fuel properties have strong influence on the dynamic flame response; however there is a lack of detailed information regarding the effect of fuel compositions on the sensitivity of the flames subjected to flow perturbations. In this study, we describe an experimental effort investigating the response of premixed biogas-air turbulent flames with varying proportions of CH4 and CO2 to velocity perturbations. The flame was stabilized using a centrally placed conical bluff body. Acoustic perturbations were imposed to the flow using loud speakers. The flame dynamics and the local heat release rate of these acoustically excited biogas flames were studied using simultaneous measurements of OH and H2CO planar laser induced fluorescence. OH* chemiluminescence along with acoustic pressure measurements were also recorded to estimate the total flame heat release modulation and the velocity fluctuations. The measurements were carried out by keeping the theoretical laminar flame speed constant while varying the bulk velocity and the fuel composition. The results indicate that the flame sensitivity to perturbations increased with increased dilution of CH4 by CO2 at low amplitude forcing, while at high amplitude forcing conditions the magnitude of the flame response was independent of dilution.

Time resolved measurement of cold start hc concentration using the fast FID

Understanding mixture formation phenomena during the first few cycles of an engine cold start is extremely important for achieving the minimum engine-out emission levels at the time when the catalytic converter is not yet operational. Of special importance is the structure of the charge (film, droplets and vapour) which enters the cylinder during this time interval as well as its concentration profile. However, direct experimental studies of the fuel behaviour in the inlet port have so far been less than fully successful due to the brevity of the process and lack of a suitable experimental technique. We present measurements of the hydrocarbon (HC) concentration in the manifold and port of a production SI engine using the Fast Response Flame Ionisation Detector (FRFID). It has been widely reported in the past few years how the FRFID can be used to study the exhaust and in-cylinder HC concentrations with a time resolution of a few degrees of crank angle, and the device has contributed significantly to the understanding of unburned HC emissions. Using the FRFID in the inlet manifold is difficult because of the presence of liquid droplets, and the low and fluctuating pressure levels, which leads to significant changes in the response time of the instrument. However, using recently developed procedures to correct for the errors caused by these effects, the concentration at the sampling point can be reconstructed to align the FRFID signal with actual events in the engine. © 1996 Society of Automotive Engineers, Inc.

Updated correlation between aircraft smoke number and black carbon concentration

Aircraft emissions of black carbon (BC) contribute to anthropogenic climate forcing and degrade air quality. The smoke number (SN) is the current regulatory measure of aircraft particulate matter emissions and quantifies exhaust plume visibility. Several correlations between SN and the exhaust mass concentration of BC (CBC) have been developed, based on measurements relevant to older aircraft engines. These form the basis of the current standard method used to estimate aircraft BC emissions (First Order Approximation version 3 [FOA3]) for the purposes of environmental impact analyses. In this study, BC with a geometric mean diameter (GMD) of 20, 30, and 60 nm and filter diameters of 19 and 35 mm are used to investigate the effect of particle size and sampling variability on SN measurements. For BC with 20 and 30 nm GMD, corresponding to BC emitted by modern aircraft engines, a smaller SN results from a given CBC than is the case for BC with 60 nm GMD, which is more typical of older engines. An updated correlation between CBC and SNthat accounts for typical size of BC emitted by modern aircraft is proposed. An uncertainty of ±25% accounts for variation in GMD in the range 20-30 nm and for the range of filter diameters. The SN-CBC correlation currently used in FOA3 underestimates by a factor of 2.5-3 for SN <15, implying that current estimates of aircraft BC emissions derived from SN are underestimated by the same factor. Copyright © American Association for Aerosol Research.

Reversible CO2 absorption by the 6H perovskite Ba 4Sb2O9

A novel compound for carbon capture and storage (CCS) applications, the 6H perovskite Ba4Sb2O9, was found to be able to absorb CO2 through a chemical reaction at 873 K to form barium carbonate and BaSb2O6. This absorption was shown to be reversible through the regeneration of the original Ba4Sb 2O9 material upon heating above 1223 K accompanied by the release of CO2. A combined synchrotron X-ray diffraction, thermogravimetric, and microscopy study was carried out to characterize first the physical absorption properties and then to analyze the structural evolution and formation of phases in situ. Importantly, through subsequent carbonation and regeneration of the material over 100 times, it was shown that the combined absorption and regeneration reactions proceed without any significant reduction in the CO2 absorption capacity of the material. After 100 cycles the capacity of Ba4Sb2O9 was ∼0.1 g (CO 2)/g (sorbent), representing 73% of the total molar capacity. This is the first report of a perovskite-type material showing such good properties, opening the way for studies of new classes of inorganic oxide materials with stable and flexible chemical compositions and structures for applications in carbon capture. © 2013 American Chemical Society.