University, Diss., 2005--Potsdam.

Der Klimawandel und insbesondere die globale Erwärmung gehören aktuell zu den größten Herausforderungen an Politik und Wissenschaft. Steigende CO2-Emissionen sind hierbei maßgeblich für die Klimaerwärmung verantwortlich. Ein regulierender Faktor beim CO2-Austausch mit der Atmosphäre ist die Vegetation, welche als CO2-Senke aber auch als CO2-Quelle fungieren kann. Diese Funktionen können durch Analysen der Landbedeckungsänderung in Kombination mit Modellierungen der Kohlenstoffbilanz quantifiziert werden, was insbesondere von aktuellen und zukünftigen politischen Instrumenten wie CDM (Clean Development Mechanism) oder REDD (Reducing Emissions from Deforestation and Degradation) gefordert wird. Vor allem in Regionen mit starker Landbedeckungsänderung und hoher Bevölkerungsdichte sowie bei geringem Wissen über die Produktivität und CO2-Speicherpotentiale der Vegetation, bedarf es einer Erforschung und Quantifizierung der terrestrischen Kohlenstoffspeicher. Eine Region, für die dies in besonderem Maße zutrifft, ist Westafrika. Jüngste Studien haben gezeigt, dass sich einerseits die Folgen des Klimawandels und Umweltveränderungen sehr stark in Westafrika auswirken werden und andererseits Bevölkerungswachstum eine starke Änderung der Landbedeckung für die Nutzung als agrarische Fläche bewirkt hat. Folglich sind in dieser Region die terrestrischen Kohlenstoffspeicher durch Ausdehnung der Landwirtschaft und Waldrodung besonders gefährdet. Große Flächen agieren anstelle ihrer ursprünglichen Funktion als CO2-Senke bereits als CO2-Quelle. [...] / Global warming associated with climate change is one of the greatest challenges of today's world. One regulating factor of CO2 exchange with the atmosphere is the vegetation cover. Measurements of land cover changes in combination with modeling of the carbon balance can therefore contribute to determining temporal variations of CO2 sources and sinks, which is an essential necessity of existing and prospective political instruments like CDM (Clean Development Mechanism) or REDD (Reducing Emissions from Deforestation and Degradation). The need for quantifiable terrestrial carbon stocks is especially high for regions, where rates of land cover transformation and population density are high and knowledge on vegetation productivity is low. One region which is characterized by these criteria is West Africa. Therefore, carbon stocks in this region are seriously endangered by land cover change like the expansion of agriculture and forest logging. Large areas already act as carbon sources on a yearly basis instead of their previous function as carbon sink. Since only a few studies have analyzed the terrestrial carbon stocks in Africa and especially regional analysis in West Africa are missing, the following study focuses on regional scale modeling of the actual terrestrial carbon stocks. Additionally, the potential carbon stocks of unmanaged land cover and the potential for CO2 payments have been analyzed in this work. To quantify and assess carbon fluxes as well as the loss of carbon, net primary productivity of vegetation has been modeled, based on the plants characteristics to fix carbon from the atmosphere during photosynthesis. Modeling vegetation dynamics and net primary productivity has been realized by using MODIS 250m time series for semi-humid and semi-arid savanna ecosystems in West Africa. This study aimed to quantify CO2 exchanges of the Savanna regions in the Volta basin by applying and adapting the Regional Biomass Model (RBM). The RBM was developed by Jochen Richters (2005) at a resolution of 1000m for the Namibian Kaokoveld. In this study the model was optimized to the scale of 232m to consider the heterogeneous landscape in West Africa (RBM+). New input parameters with higher accuracies and resolution were generated instead of using the global standard products. The most important parameters for the modeling are FPAR and the fractional cover of herbaceous and woody vegetation. To enhance the MODIS FPAR product, linear interpolation and downscaling algorithms were applied. The main objective of the downscaling is a better representation of the finely scattered vegetation by the 232m resolution FPAR. The second optimized parameter, the fractional cover of herbaceous and woody vegetation was represented by the Vegetation Continuous Fields product (VCF) from MODIS in the originally version of the RBM. This global product reflects the vegetation structure of West Africa poorly, since few high resolution training data is available for this region, and the dynamic savanna vegetation can hardly be classified by not regionally adapted methods. Additionally, the data is only available with 500m resolution. Therefore, in this study a new product with 232m resolution was developed which represents the spatial heterogeneity well and, due to the regional adaptation, shows higher accuracies. The percentage cover of woody and herbaceous vegetation and bare soil on 232m MODIS data was calculated in a multi scale approach. Based on very high resolution data, represented by Quickbird and Ikonos with 0.6-4m resolution, and high resolution data from Landsat with 30m resolution, the percentage coverage was estimated for representative focus regions. These classifications were used as a training data set to determine the percentage coverage on the 232m scale with MODIS time series for the whole study region. Based on these optimized and adapted input parameters, the net primary productivity was modeled. Data from a meteorological station and an Eddy-Covariance-Flux allowed a detailed validation of the input parameters and of the model results. The model led to good results as it only overestimated the net primary productivity for the two analyzed years 2005 and 2006 by 8.8 and 2.0 %, respectively. The second aim of the study was an analysis of the potential for long term terrestrial carbon sinks. Classifications of the actual and of the potential land cover were calculated for this analysis. Considering the overall long time CO2 fixation behavior of trees, which depends on their age, longterm carbon stocks for 100 years were simulated. As carbon fixing could be paid by emission trading, which is in future depending on the political Post-Kyoto programs, potential alternative income was calculated with different price scenarios for the three countries. A comparison with the gross domestic products of these countries and with developing aid, showed the significance of CO2 trading in this region.

京都大学 / 0048 / 新制・課程博士 / 博士(工学) / 甲第18938号 / 工博第3980号 / 新制||工||1613(附属図書館) / 31889 / 京都大学大学院工学研究科都市社会工学専攻 / (主査)教授 松岡 俊文, 教授 後藤 仁志, 准教授 村田 澄彦 / 学位規則第4条第1項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DGAM

La séparation du CO2 d'un mélange de gaz par cristallisation d'hydrates de gaz est un procédé qui pourrait à terme présenter une alternative intéressante aux techniques conventionnelles de capture du CO2. L'objectif de cette thèse était d'évaluer le potentiel de ce procédé "hydrates" pour séparer le CO2 d'un mélange CO2-CH4 riche en CO2. Nous avons étudié en particulier la sélectivité de la séparation vis-à-vis du CO2 et la cinétique de cristallisation des hydrates, ainsi que l'effet d'additifs thermodynamiques et cinétiques (et de certaines de leurs combinaisons) sur ces deux paramètres pour différentes conditions opératoires (pression, température, concentrations). Les expériences de formation/décomposition d’hydrates ont été réalisées en mode "batch" dans un réacteur haute pression faisant partie d'un pilote expérimental conçu et construit entièrement pendant cette thèse. Un modèle semi-empirique a été également développé pour estimer le taux de conversion de l’eau en hydrate et la composition des différentes phases en présence (hydrates, liquide et vapeur) à l'équilibre. Les résultats obtenus montrent que l'association du sodium dodécyl sulfate (SDS), utilisé en tant que promoteur cinétique, avec du tétrahydrofurane (THF), utilisé en tant que promoteur thermodynamique, permet d'obtenir des résultats intéressants en terme de quantité d'hydrates formés et de cinétique de formation. La sélectivité de la séparation vis-à-vis du CO2 reste cependant trop faible (en moyenne quatre molécules de CO2 piégées dans la structure de l'hydrate pour une de CH4) pour envisager d’utiliser ce procédé "hydrates" à plus grande échelle afin de séparer le CO2 de ce type de mélange de gaz. / The separation of CO2 from a gas mixture by crystallization of gas hydrates is a process that could eventually provide an attractive alternative to the conventional techniques used for CO2 capture. The aim of this thesis was to evaluate the potential of this "hydrate" process to separate CO2 from a CO2-CH4 gas mixture, rich in CO2. We have studied in particular the selectivity of the separation toward CO2 and the hydrate crystallization kinetics. The effects of thermodynamic and kinetic additives (and some additive combinations) on these two parameters for different operating conditions (pressure, temperature, concentrations) were evaluated. Hydrate formation and dissociation experiments were performed in "batch mode” in a high pressure reactor, and with an experimental pilot rig designed and built entirely during this thesis. A semi-empirical model was also developed to estimate the water to hydrate conversion and the composition of the different phases (hydrates, liquid and vapor) at equilibrium. The results show that the combination of sodium dodecyl sulfate (SDS) used as a kinetic promoter, with tetrahydrofuran (THF) used as a thermodynamic promoter, provides interesting results in terms of both the amount of hydrates formed and the hydrate formation kinetics. The selectivity of the separation toward CO2 remains too low (an average of four CO2 molecules trapped in the hydrate structure for one of CH4) to consider using this "hydrate" process on a larger scale to separate CO2 from such a gas mixture.

This thesis analyses two strategies for decreasing anthropogenic carbon dioxide (CO2) emissions: to capture and store CO2, and to increase the use of biomass. First, two concepts for CO2 capture with low capture penalties are evaluated. The concepts are an integrated gasification combined cycle where the oxygen is supplied by a membrane reactor, and a hybrid cycle where the CO2 is captured at elevated pressure. Although the cycles have comparatively high efficiencies and low penalties, they illustrate the inevitable fact that capturing CO2 will always induce significant efficiency penalties. Other strategies are also needed if CO2 emissions are to be forcefully decreased. An alternative is increased use of biomass, which partially could be used for production of motor fuels (biofuels). This work examines arguments for directing biomass to the transport sector, analyses how biofuels (and also some other means) may be used to reduce CO2 emissions and increase security of motor fuel supply. The thesis also explores the possibility of reducing CO2 emissions by comparatively easy and cost-efficient CO2 capture from concentrated CO2 streams available in some types of biofuel plants. Many conclusions of the thesis could be associated with either of three meanings of the word sense: First, there is reason in biofuel production – since it e.g. reduces oil dependence. From a climate change mitigation perspective, however, motor fuel production is often a CO2-inefficient use of biomass, but the thesis explores how biofuels’ climate change mitigation effects may be increased by introducing low-cost CO2 capture. Second, the Swedish promotion of biofuels appears to have been governed more by a feeling for attaining other goals than striving for curbing climate change. Third, it seems to have been the prevalent opinion among politicians that the advantages of biofuels – among them their climate change mitigation benefits – are far greater than the disadvantages and that they should be promoted. Another conclusion of the thesis is that biofuels alone are not enough to drastically decrease transport CO2 emissions; a variety of measures are needed such as fuels from renewable electricity and improvements of vehicle fuel economy. / QC 20100823

To curb greenhouse gases and mitigate climate change is one of the biggest challenges human society face today. Carbon dioxide (CO2) has accumulated rapidly in the atmosphere as a consequence of burning of fossil fuels and deforestation. The aim of this study is to explore two methods to store carbon dioxide in geological formations and biological sinks. The aim is also to discuss the two mitigation options from a sustainable perspective and whether it can lead to a better environment and benefits for local and global societies. The research questions are: Which method to store carbon dioxide, geological or biological, is the most effective? Which method to store carbon dioxide, geological or biological, has the greatest potential to promote sustainable development for local communities? The method used is a comparative case study and presents four case studies that explore the potential for CO2 storage offshore in Norway and Brazil; and in tropical forests in Mexico and Brazil. The mitigation options are discussed from two different theoretical perspectives. The principle of the theory of ecological modernisation is that innovation and environmentally friendly technology can solve the environmental problems human societies face today, whereas the theory of common pool resources promotes local communities to govern limited resources in order to manage them sustainably. The findings suggest that ecological modernisation legitimize environmental destruction as carbon dioxide storage in geological formations (CCS) use the technology as a mean to extract more oil and gas; which results in a rebound-effect. Therefore, carbon dioxide capture in geological formations is not a realistic method unless it can prevent further emissions. Protected forest resources can be seen as biological insurance, which safeguard ecosystem services, biodiversity, and the forest potential to hold carbon. Carbon sequestration in tropical forest has the potential to store carbon dioxide given that the forests are protected and local communities have tenure rights, knowledge, and the means to protect the forest and manage them sustainably.

Im Rahmen dieser Arbeit werden Konzepte für Gasaufbereitung in Kombikraftwerken mit integrierter Wirbelschichtvergasung und CO2-Abtrennung untersucht (IGCC-CCS). Dabei stehen die Konvertierung von Kohlenmonoxid (CO-Shift) und die Einbindung dieses Prozeß-schrittes in ein IGCC-CCS-Kraftwerk im Mittelpunkt. Ziel der Arbeit ist die energetische und wirtschaftliche Bewertung von Konzepten zur CO2-Abtrennung für ein ab 2015 baubares, grundlastfähiges IGCC-CCS-Kraftwerk der 800-MW-Klasse. Dazu werden neben den bekannten konventionellen, mehrstufigen Konzepten der Rohgas- und Reingas-Shift weitere alternative Ansätze zur Steigerung des Anlagenwirkungsgrades sowie zur Senkung der spezifischen CO2-Emission verfolgt. Die Ergebnisse der mit Hilfe von ASPEN Plus und EBSILON Professional durchgeführten Prozesssimulationen werden im Vergleich zu Dampfkraftwerken neuester Bauart wirtschaftlich bewertet.

This article deals with main aspects of a novel technique for carbon dioxide capture and storage released by large combustion plants. Since this novel technique has become essential for reducing greenhouse gas emissions, it has been regulated by the European Union through the Directive number 2009/31. Therefore, acknowledging relevant legal aspects for regulation, suchas: mandatory, exploration permits, storage among others, the focus has been pointed out on responsibilities and guarantees regime. / El presente artículo desarrolla las principales aristas de la captura y almacenamiento del dióxido de carbono emanado de las grandes instalaciones de combustión, novedosa técnica que al tornarse imprescindible para la reducción de emisión de gases de efecto invernadero ha sido regulada porla Unión Europea (UE) a través de la directiva 2009/31. Así, tras reconocerlos aspectos jurídicos relevantes de su regulación —obligatoriedad, permisos de exploración y almacenamiento, entre otros— se incide en el régimen de responsabilidad y garantías.

Im Rahmen dieser Arbeit werden Konzepte für Gasaufbereitung in Kombikraftwerken mit integrierter Wirbelschichtvergasung und CO2-Abtrennung untersucht (IGCC-CCS). Dabei stehen die Konvertierung von Kohlenmonoxid (CO-Shift) und die Einbindung dieses Prozeß-schrittes in ein IGCC-CCS-Kraftwerk im Mittelpunkt. Ziel der Arbeit ist die energetische und wirtschaftliche Bewertung von Konzepten zur CO2-Abtrennung für ein ab 2015 baubares, grundlastfähiges IGCC-CCS-Kraftwerk der 800-MW-Klasse. Dazu werden neben den bekannten konventionellen, mehrstufigen Konzepten der Rohgas- und Reingas-Shift weitere alternative Ansätze zur Steigerung des Anlagenwirkungsgrades sowie zur Senkung der spezifischen CO2-Emission verfolgt. Die Ergebnisse der mit Hilfe von ASPEN Plus und EBSILON Professional durchgeführten Prozesssimulationen werden im Vergleich zu Dampfkraftwerken neuester Bauart wirtschaftlich bewertet.

Geophysical methods are essential for exploration and monitoring of subsurface formations, e.g. in carbon dioxide sequestration or enhanced geothermal energy. One of the keys to their successful application is the knowledge of how the measured physical quantities are related to the desired reservoir parameters. The work presented in this thesis shows that the presence of carbon dioxide (CO2) in pore space gives rise to multiple processes all of which contribute to the electrical rock conductivity variation. Basically, three mechanisms take place: (1) CO2 partially replaces the pore water, which is equivalent to a decrease in water saturation. (2) CO2 chemically interacts with the pore water by dissolution and dissociation. These processes change both the chemical composition and the pH of the pore filling fluid. (3) The low-pH environment can give rise to mineral dissolution and/or precipitation processes and changes the properties of the grain-water interface. Investigations on the pore water phase show that the reactive nature of CO2 in all physical states significantly acts on the electrical conductivity of saline pore waters. The physico-chemical interaction appears in different manifestations depending mainly on the pore water composition (salinity, ion types) but also on both temperature and pressure. The complex behaviour includes a low- and a high-salinity regime originating from the conductivity increasing effect of CO2 dissociation, which is opposed by the conductivity decreasing effect of reduced ion activity caused by the enhanced mutual impediment of all solutes. These results are fundamental since the properties of the water phase significantly act on all conduction mechanisms in porous media. In order to predict the variation of pore water conductivity, both a semi-analytical formulation and an empirical relationship for correcting the pore water conductivity, which depends on salinity, pressure and temperature, are derived. The central part of the laboratory experiments covers the spectral complex conductivity of water-bearing sand during exposure to and flow-through by CO2 at pressures up to 30MPa and temperatures up to 80°C. It is shown that the impact of CO2 on the real part of conductivity of a clean quartz sand is dominated by the low- and high-salinity regime of the pore water. The obtained data further show that chemical interaction causes a reduction of interface conductivity, which could be related to the low pH in the acidic environment. This effect is described by a correction term, which is a constant value as a first approximation. When the impact of CO2 is taken into account, a correct reconstruction of fluid saturation from electrical measurements is possible. In addition, changes of the inner surface area, which are related to mineral dissolution or precipitation processes, can be quantified. Both the knowledge gained from the laboratory experiments and a new workflow for the description and incorporation of geological geometry models enable realistic finite element simulations. Those were conducted for three different electromagnetic methods applied in the geological scenario of a fictitious carbon dioxide sequestration site. The results show that electromagnetic methods can play an important role in monitoring CO2 sequestration. Compared to other geophysical methods, electromagnetic techniques are generally very sensitive to pore fluids. The proper configuration of sources and receivers for a suitable electromagnetic method that generates the appropriate current systems is essential. Its reactive nature causes CO2 to interact with a water-bearing porous rock in a much more complex manner than non-reactive gases. Without knowledge of the specific interactions between CO2 and rock, a determination of saturation and, consequently, a successful monitoring are possible only to a limited extend. The presented work provides fundamental laboratory investigations for the understanding of the electrical properties of rocks when the reactive gas CO2 enters the rock-water system. All laboratory results are put in the context of potential monitoring applications. The transfer from petrophysical investigations to the planning of an operational monitoring design by means of close-to-reality 3D FE simulations is accomplished.