An investigation of the kinetics of CO 2 uptake by a synthetic calcium based sorbent

This study examines the kinetics of carbonation by CO 2 at temperatures of ca. 750°C of a synthetic sorbent composed of 15wt% mayenite (Ca 12Al 14O 33) 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. © 2011 Elsevier Ltd.

Assessing the potential of yield improvements, through process scrap reduction, for energy and CO2 abatement in the steel and aluminium sectors

Targets to cut 2050 CO2 emissions in the steel and aluminium sectors by 50%, whilst demand is expected to double, cannot be met by energy efficiency measures alone, so options that reduce total demand for liquid metal production must also be considered. Such reductions could occur through reduced demand for final goods (for instance by life extension), reduced demand for material use in each product (for instance by lightweight design) or reduced demand for material to make existing products. The last option, improving the yield of manufacturing processes from liquid metal to final product, is attractive in being invisible to the final customer, but has had little attention to date. Accordingly this paper aims to provide an estimate of the potential to make existing products with less liquid metal production. Yield ratios have been measured for five case study products, through a series of detailed factory visits, along each supply chain. The results of these studies, presented on graphs of cumulative energy against yield, demonstrate how the embodied energy in final products may be up to 15 times greater than the energy required to make liquid metal, due to yield losses. A top-down evaluation of the global flows of steel and aluminium showed that 26% of liquid steel and 41% of liquid aluminium produced does not make it into final products, but is diverted as process scrap and recycled. Reducing scrap substitutes production by recycling and could reduce total energy use by 17% and 6% and total CO 2 emissions by 16% and 7% for the steel and aluminium industries respectively, using forming and fabrication energy values from the case studies. The abatement potential of process scrap elimination is similar in magnitude to worldwide implementation of best available standards of energy efficiency and demonstrates how decreasing the recycled content may sometimes result in emission reductions. Evidence from the case studies suggests that whilst most companies are aware of their own yield ratios, few, if any, are fully aware of cumulative losses along their whole supply chain. Addressing yield losses requires this awareness to motivate collaborative approaches to improvement. © 2011 Elsevier B.V. All rights reserved.

Embodied Energy and Gas Emissions of Retaining Wall Structures

The embodied energy (EE) and gas emissions of four design alternatives for an embankment retaining wall system are analyzed for a hypothetical highway construction project. The airborne emissions considered are carbon dioxide (CO 2), methane (CH 4), nitrous oxide (N 2O), sulphur oxides (SO X), and nitrogen oxides (NO X). The process stages considered in this study are the initial materials production, transportation of construction machineries and materials, machinery operation during installation, and machinery depreciations. The objectives are (1) to determine whether there are statistically significant differences among the structural alternatives; (2) to understand the relative proportions of impacts for the process stages within each design; (3) to contextualize the impacts to other aspects in life by comparing the computed EE values to household energy consumption and car emission values; and (4) to examine the validity of the adopted EE as an environmental impact indicator through comparison with the amount of gas emissions. For the project considered in this study, the calculated results indicate that propped steel sheet pile wall and minipile wall systems have less embodied energy and gas emissions than cantilever steel tubular wall and secant concrete pile wall systems. The difference in CO 2 emission for the retaining wall of 100 m length between the most and least environmentally preferable wall design is equivalent to an average 2.0 L family car being driven for 6.2 million miles (or 62 cars with a mileage of 10,000 miles/year for 10 years). The impacts in construction are generally notable and careful consideration and optimization of designs will reduce such impacts. The use of recycled steel or steel pile as reinforcement bar is effective in reducing the environmental impact. The embodied energy value of a given design is correlated to the amount of gas emissions. © 2011 American Society of Civil Engineers.

Development of a tool for rapidly assessing the implementation difficulty and emissions benefits of innovations

Consumer goods manufacturers aiming to reduce the environmental impact associated with their products commonly pursue incremental change strategies, but more radical approaches may be required if we are to address the challenges of sustainable consumption. One strategy to realize step change reductions is to prepare a portfolio of innovations providing different levels of impact reduction in exchange for different levels of organizational resource commitment. In this research a tool is developed to support this strategy, starting with the assumption that through brainstorming or other eco-innovation approaches, a long-list of candidate innovations has been created. The tool assesses the potential greenhouse gas benefit of an innovative option against the difficulty of its implementation. A simple greenhouse gas benefit assessment method based on streamlined LCA was used to analyze impact reduction potential, and a novel measure of implementation difficulty was developed. The predictions of implementation difficulty were compared against expert opinion, and showed similar results indicating the measure can be used sensibly to predict implementation difficulty. The assessment of the environmental gain versus implementation difficulty is visualized in a matrix, showing the trade-offs of several options. The tool is deliberately simple with scalar measures of CO 2 emissions benefits and implementation difficulty so tool users must remain aware of other potential environmental burdens besides greenhouse gases (e.g. water, waste). In addition, although relative life cycle emissions benefits of an option may be low, the absolute impact of an option can be high and there may be other co-benefits, which could justify higher levels of implementation difficulty. Different types of consumer products (e.g. household, personal care, foods) have been evaluated using the tool. Initial trials of the tool within Unilever demonstrate that the tool facilitates rapid evaluation of low-carbon innovations. © 2011 Elsevier Ltd. All rights reserved.

The development of a hot rolling process for variable cross-section I-beams

To meet targeted reductions in CO 2 emissions by 2050, demand for metal must be cut, for example through the use of lightweight technologies. However, the efficient production of weight optimized components often requires new, more flexible forming processes. In this paper, a novel hot rolling process is presented for forming I-beams with variable cross-section, which are lighter than prismatic alternatives. First, the new process concept is presented and described. A detailed computational and experimental analysis is then conducted into the capabilities of the process. Results show that the process is capable of producing defect free I-beams with variations in web depth of 30-50%. A full analysis of the process then indicates the likely failure modes, and identifies a safe operating window. Finally, the implications of these results for producing lightweight beams are discussed. © 2012 Elsevier B.V. All rights reserved.

Effects of preferential transport in turbulent bluff-body-stabilized lean premixed CH 4/air flames

Preferential species diffusion is known to have important effects on local flame structure in turbulent premixed flames, and differential diffusion of heat and mass can have significant effects on both local flame structure and global flame parameters, such as turbulent flame speed. However, models for turbulent premixed combustion normally assume that atomic mass fractions are conserved from reactants to fully burnt products. Experiments reported here indicate that this basic assumption may be incorrect for an important class of turbulent flames. Measurements of major species and temperature in the near field of turbulent, bluff-body stabilized, lean premixed methane-air flames (Le=0.98) reveal significant departures from expected conditional mean compositional structure in the combustion products as well as within the flame. Net increases exceeding 10% in the equivalence ratio and the carbon-to-hydrogen atom ratio are observed across the turbulent flame brush. Corresponding measurements across an unstrained laminar flame at similar equivalence ratio are in close agreement with calculations performed using Chemkin with the GRI 3.0 mechanism and multi-component transport, confirming accuracy of experimental techniques. Results suggest that the large effects observed in the turbulent bluff-body burner are cause by preferential transport of H 2 and H 2O through the preheat zone ahead of CO 2 and CO, followed by convective transport downstream and away from the local flame brush. This preferential transport effect increases with increasing velocity of reactants past the bluff body and is apparently amplified by the presence of a strong recirculation zone where excess CO 2 is accumulated. © 2011 The Combustion Institute.

The structure of turbulent stratified and premixed methane/air flames I: Non-swirling flows

A series of flames in a turbulent methane/air stratified swirl burner is presented. The degree of stratification and swirl are systematically varied to generate a matrix of experimental conditions, allowing their separate and combined effects to be investigated. Non-swirling flows are considered in the present paper, and the effects of swirl are considered in a companion paper (Part II). A mean equivalence ratio of φ=0.75 is used, with φ for the highest level of stratification spanning 0.375-1.125. The burner features a central bluff-body to aid flame stabilization, and the influence of the induced recirculation zone is also considered. The current work focuses on non-swirling flows where two-component particle image velocimetry (PIV) measurements are sufficient to characterize the main features of the flow field. Scalar data obtained from Rayleigh/Raman/CO laser induced fluorescence (CO-LIF) line measurements at 103μm resolution allow the behavior of key combustion species-CH 4, CO 2, CO, H 2, H 2O and O 2-to be probed within the instantaneous flame front. Simultaneous cross-planar OH-PLIF is used to determine the orientation of the instantaneous flame normal in the scalar measurement window, allowing gradients in temperature and progress variable to be angle corrected to their three dimensional values. The relationship between curvature and flame thickness is investigated using the OH-PLIF images, as well as the effect of stratification on curvature.The main findings are that the behavior of the key combustion species in temperature space is well captured on the mean by laminar flame calculations regardless of the level of stratification. H 2 and CO are significant exceptions, both appearing at elevated levels in the stratified flames. Values for surface density function and by extension thermal scalar dissipation rate are found to be substantially lower than laminar values, as the thickening of the flame due to turbulence dominates the effect of increased strain. These findings hold for both premixed and stratified flames. The current series of flames is proposed as an interesting if challenging set of test cases for existing and emerging turbulent flame models, and data are available on request. © 2012 The Combustion Institute.

The structure of turbulent stratified and premixed methane/air flames II: Swirling flows

Experimental results are presented from a series of turbulent methane/air stratified flames stabilized on a swirl burner. Nine operating conditions are considered, systematically varying the level of stratification and swirl while maintaining a lean global mean equivalence ratio of φ̄=0.75. Scalar data are obtained from Rayleigh/Raman/CO laser induced fluorescence (CO-LIF) line measurements at 103μm resolution, allowing the behavior of the major combustion species-CH 4, CO 2, CO, H 2, H 2O and O 2-to be probed within the instantaneous flame front. The corresponding three-dimensional surface density function and thermal scalar dissipation rate are investigated, along with geometric characteristics of the flame such as curvature and flame thickness. Hydrogen and carbon monoxide levels within the flame brush are raised by stratification, indicating models with laminar premixed flame chemistry may not be suitable for stratified flames. However, flame surface density, scalar dissipation and curvature all appear insensitive to the degree of stratification in the flames surveyed. © 2012 The Combustion Institute.

The effect of addition of ZrO2 to Fe2O3 for hydrogen production by chemical looping

In this paper, a synthetic mixture of ZrO2 and Fe 2O3 was prepared by coprecipitation for use in chemical looping and hydrogen production. Cycling experiments in a fluidized bed showed that a material composed of 30 mol % ZrO2 and 70 mol % Fe 2O3 was capable of producing hydrogen with a consistent yield of 90 mol % of the stoichiometric amount over 20 cycles of reduction and oxidation at 1123 K. Here, the iron oxide was subjected to cycles consisting of nearly 100% reduction to Fe followed by reoxidation (with steam or CO 2 and then air) to Fe2O3. There was no contamination by CO of the hydrogen produced, at a lower detection limit of 500 ppm, when the conversion of Fe3O4 to Fe was kept below 90 mol %. A preliminary investigation of the reaction kinetics confirmed that the ZrO2 support does not inhibit rates of reaction compared with those observed with iron oxide alone. © 2012 American Chemical Society.

Comparative analysis of carbonization drivers in China's megacities

This study investigates the key drivers affecting emission increases in terms of population growth, economic growth, industrial transformation, and energy use in six Chinese megacities: Beijing, Shanghai, Tianjin, Chongqing, Guangzhou, and Hong Kong. The six cities represent the most-developed regions in China and they have similar per capita carbon dioxide (CO 2) emissions as many developed countries. There is an urgent need to quantify the magnitude of each factor in driving the emissions changes in those cities so that a potential bottom-up climate mitigation policy design at the city and sectoral levels can be initiated. We adopt index decomposition analysis and present the results in both additive and multiplicative approaches to reveal the absolute and relative levels of each factor in driving emission changes during 1985-2007. Among all cities, economic effect and energy intensity effect have always been the two dominant factors contributing to the changes in carbon emissions. This study reveals that there are large variations in the ways driving forces contribute to emission levels in different cities and industrial sectors. © 2012 by Yale University.

Preliminary evaluation of a nuclear scenario involving innovative gas cooled reactors

In order to guarantee a sustainable supply of future energy demand without compromising the environment, some actions for a substantial reduction of CO 2 emissions are nowadays deeply analysed. One of them is the improvement of the nuclear energy use. In this framework, innovative gas-cooled reactors (both thermal and fast) seem to be very attractive from the electricity production point of view and for the potential industrial use along the high temperature processes (e.g., H 2 production by steam reforming or I-S process). This work focuses on a preliminary (and conservative) evaluation of possible advantages that a symbiotic cycle (EPR-PBMR-GCFR) could entail, with special regard to the reduction of the HLW inventory and the optimization of the exploitation of the fuel resources. The comparison between the symbiotic cycle chosen and the reference one (once-through scenario, i.e., EPR-SNF directly disposed) shows a reduction of the time needed to reach a fixed reference level from ∼170000 years to ∼1550 years (comparable with typical human times and for this reason more acceptable by the public opinion). In addition, this cycle enables to have a more efficient use of resources involved: the total electric energy produced becomes equal to ∼630 TWh/year (instead of only ∼530 TWh/year using only EPR) without consuming additional raw materials. © 2009 Barbara Vezzoni et al.

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.

Characterization of light and heavy hydrated magnesium carbonates using thermal analysis

Upon heating, hydrated magnesium carbonates (HMCs) undergo a continuous sequence of decomposition reactions. This study aims to investigate the thermal decomposition of various commercially produced HMCs classified as light and heavy, highlight their differences, and provide an insight into their compositions in accordance with the results obtained from thermal analysis and microstructure studies. An understanding of the chemical compositions and microstructures, and a better knowledge of the reactions that take place during the decomposition of HMCs were achieved through the use of SEM, XRD, and TG/differential thermal analysis (DTA). The quantification of their CO 2 contents was provided by TG and dissolving the samples in HCl acid. Results show that variations exist within the microstructure and decomposition patterns of the two groups of HMCs, which do not exactly fit into the fixed stoichiometry of the known HMCs in the MgO-CO2-H2O system. The occurrence of an exothermic DTA peak was only observed for the heavy HMCs, which was attributed to their high CO2 contents and the relatively delayed decomposition pattern. © 2013 Akadémiai Kiadó, Budapest, Hungary.