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

Vinyltrialkoxysilanes are grafted onto polyolefins via a radical mechanism; in a subsequent step, the pendant alkoxysilanes hydrolyze and condense upon exposure to water, resulting formation of crosslinks. Straight chain hydrocarbons were used as model compounds to investigate the regioselectivity of vinyltrimethoxysilane grafting. To stabilize the water-sensitive grafted products, the methoxy groups were substituted using phenyllithium. It was found that this reaction must be carried out for a minimum of three days to ensure full substitution. The grafted products were then separated on a weight basis using semi-preparative HPLC. Analysis of the di-grafted fraction using edited HSQC and HSQC-TOCSY NMR showed that radical propagation occurs via 1,4- and 1,5-intramolecular hydrogen shifts along the hydrocarbon backbone, resulting in multiple grafts per backbone. Post-combustion carbon capture targets CO₂ emissions from large point sources for capture and sequestration. A new class of potential carbon capture agents known as reversible ionic liquids (RevILs) has been synthesized and evaluated in terms of potential performance parameters (e.g. CO₂ capacity, viscosity, enthalpy of regeneration). These RevILs are silylated amines, which react with CO₂ to form a salt comprising an ammonium cation and a carbamate anion that is liquid at room temperature. Structural modifications of the basic silylamine skeleton result in drastic differences in the performance of the resulting RevIL. Systematic variation of the silylated amines allowed determination of a structure-property relationship, and continued iterations will allow development of an ideal candidate for scale-up. The properties and potential applications of gold nanoparticles (AuNP) are highly dependent on their size and shape. These properties are commonly controlled during liquid-phase synthesis through the use of capping agents, which must be removed following synthesis. Reverse micelles can also be used to control the morphology of AuNP during their synthesis. When RevILs are used in the formation of these reverse micelles, either as the disperse phase or as the surfactant, the built-in switch can be used to release the nanoparticles following their synthesis. This release on command could decrease the post-synthetic steps required to clean and purify AuNP prior to use. We have successfully synthesized AuNP using a number of different RevILs.

Fossil fuels constitute a significant fraction of the world’s energy demand. The burning of fossil fuels emits huge amounts of carbon dioxide into the atmosphere. Therefore, the limited availability of fossil fuel resources and the environmental impact of their use require a change to alternative energy sources or carriers (such as hydrogen) in the foreseeable future. The development of methods to mitigate carbon dioxide emission into the atmosphere is equally important. Hence, extensive research has been carried out on the development of cost-effective technologies for carbon dioxide capture and techniques to establish hydrogen economy. Hydrogen is a clean energy fuel with a very high specific energy content of about 120MJ/kg and an energy density of 10Wh/kg. However, its potential is limited by the lack of environment-friendly production methods and a suitable storage medium. Conventional hydrogen production methods such as Steam-methane-reformation and Coal-gasification were modified by the inclusion of NaOH. The modified methods are thermodynamically more favorable and can be regarded as near-zero emission production routes. Further, suitable catalysts were employed to accelerate the proposed NaOH-assisted reactions and a relation between reaction yield and catalyst size has been established. A 1:1:1 molar mixture of LiAlH4, NaNH2 and MgH2 were investigated as a potential hydrogen storage medium. The hydrogen desorption mechanism was explored using in-situ XRD and Raman Spectroscopy. Mesoporous metal oxides were assessed for CO2 capture at both power and non-power sectors. A 96.96% of mesoporous MgO (325 mesh size, surface area = 95.08 ± 1.5 m2/g) was converted to MgCO3 at 350°C and 10 bars CO2. But the absorption capacity of 1h ball milled zinc oxide was low, 0.198 gCO2 /gZnO at 75°C and 10 bars CO2. Interestingly, 57% mass conversion of Fe and Fe3O4 mixture to FeCO3 was observed at 200°C and 10 bars CO2. MgO, ZnO and Fe3O4 could be completely regenerated at 550°C, 250°C and 350°C respectively. Furthermore, the possible retrofit of MgO and a mixture of Fe and Fe3O4 to a 300 MWe coal-fired power plant and iron making industry were also evaluated.

Globally the combustion of fossil fuels has increased to a greater extent. Carbon dioxide (CO2) a major greenhouse gas isa by-product of such combustion practices. Increase in the quantity of CO2 emissions has resulted in serious environmental issues including global warming, ocean acidification, extreme weather, and much more leaving a direct impact on the human society. To reduce these emissions, we need a more efficient carbon dioxide capturing technology. Using advances in materials science and engineering we can develop newer technologies for the capture of carbon dioxide gas. Metal-organic frameworks (MOFs) constitute a class of three-dimensional porous materials. They have shown applicability in various fields including carbon dioxide capture. A vast variety of MOFs can be synthesized by selecting proper metal salts and organic-linkers to build up the MOF structure. This thesis focuses on the synthesis of MOFs through a sustainable process or green synthesis route. Most of the MOFs in this study have been synthesized at ambient temperature and pressure conditions with deionized water as the primary solvent. A total of eight MOFs were synthesized in this study using two organic-linkers namely, 1,2,4,5-tetrakis(4-carboxyphenyl)-benzene (H4TCPB) and 2,5-dihydroxy-1,4-benzoquinone (H2DHBQ). The metal-salts used were based on hafnium, zirconium, cerium, magnesium, iron and manganese. A number of qualitative and quantitative tests were carried out onthe MOF samples to ensure their quality of produce and performance. The primary focus was to test the materials for their capacity to uptake carbon dioxide (CO2) in a mixture of flue gases. The highest CO2 uptake capacity was recorded to be 3.02 mmol/g (at 293 K and 1 bar) by the H2DHBQ-magnesium based MOF. All the materials showed good results andwere proven to be reusable. All the synthesized MOFs were crystalline in nature, showed a single-phase microstructure and high surface area values. A supplementary study was conducted wherein the powdered MOFs were 3D printed by the Direct Ink Writing (DIW) technique using an alginate binder. The study was satisfactory because the MOFs after being 3D printed, managed to preserve their inherent properties and characteristics. The results were in par with that of their pristine MOF counterparts. / Den globala förbränningen av fossila bränslen har i allt större utsträckning ökat. Koldioxid (CO2) är en avde viktigast växthusgaserna och erhålls som biprodukt från många förbränningsmetoder. Den höga haltenkoldioxid i atmosfären har resulterat i allvarliga miljömässiga konsekvenser inklusive den globaluppvärmningen, försurning av haven, extremt väder och mycket mer som har en direkt påverkan på detmänskliga samhället. För att minska dessa utsläpp behöver vi en mer effektiv koldioxidinfångningsteknologi. Med hjälp av framsteg inom materialvetenskapen kan vi utveckla nyare tekniker för att fångakoldioxid.  Metallorganiska ramverk (MOFs) utgör en klass av tredimensionella porösa material. De har visat siganvändbara inom olika områden inklusive infångning av koldioxid. Många variation av MOF material kansyntetiseras från olika metallsalter och organiska ligander för att bygga upp MOF-strukturen. Dettaexamensarbete fokuserar på syntesen av metallorganiska ramverk via en grön syntesväg och en hållbarprocess. En stor del av MOF materialen som erhölls syntetiserades i rumstemperatur och vid normala tryckmed avjoniserat vatten som det primära lösningsmedlet. Åtta MOFs material syntetiserades i detta projekt med två olika organiska ligander, nämligen, 1,2,4,5-tetrakis(4-karboxifenyl)bensen (H4TCPB) och 2,5-dihydroxy-1,4-bensokinon (H2DHBQ). Metallsalternasom användes i synteserna baserades på hafnium(IV), zirkonium(IV), cerium(IV), magnesium(II), järn(II)och mangan(II). Ett antal kvalitativa och kvantitativa tester genomfördes på MOF:arna för att säkerställaderas kvalitet och prestanda. Det primära fokuset var att testa de olika materialen för deras förmåga att taupp koldioxid (CO2) i en blandning av olika gaser (så som kväve, N2). Den DHBQ-magnesium-baseradeMOF:en uppvisade den högsta CO2-upptagningsförmågan som var 3,02 mmol/g. Alla MOF material visadegoda resultat och visade sig även vara återanvändbara. Alla syntetiserade MOF:ar hade god kristallinitet,uppvisade en singulär fas samt hög ytarea. En kompletterande studie genomfördes där de syntetiserade MOFs materialen (i dess pulverform) 3Dprintades med hjälp av natriumalginat som bindemedel. Studien var lyckad eftersom MOF:arna erhöll entillämplig form/maktrostruktur samtidigt som materialen bevarade sina inneboende egenskaper efter 3Dprintningen.

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BECCS (Bioenergy Carbon Capture and Storage) is an important part of measures to achieve zero net emissions globally by 2050, as the technology can create carbon sinks. However, the technology is very energy-intensive and expensive, and affects the existing systems at implementation. The purpose of this study is to investigate the possibility of implementing BECCS at Karlstad Energy's biofuel-fired CHP-plant, Heden 3. The goal is, by simulation in CHEMCAD, to generate energy consumption key figures for two different separation technologies (MEA-MonoEthanolAmine and HPC-HotPotassiumCarbonate) with 90 % separation rate in three different operating cases. In addition, the systemic impact on Heden 3 will be determined by analyzing three different scenarios. In the first scenario fuel consumption is kept unchanged and steam to the carbon capture system is extracted before the turbine. In the second scenario fuel supply increases to meet the district heating needs of the existing system and steam to the carbon capture system is extracted before the turbine. In the third scenario fuel supply is kept unchanged and steam is extracted from the turbine. In addition, the study investigates various transport options for storage of carbon dioxide and finally calculate the total carbon sink Karlstad Energy can contribute to. The results show that production of electricity is reduced by 65-87 % after implementation of MEA and 151-238 % for HPC in the first scenario. Without heat utilization in the carbon capture system, heat production is reduced by 66-86 % with MEA and 54-76% for HPC. In the second scenario, a fuel supply increase by 134 % is required to meet the needs, which corresponds to more than twice the boiler capacity and results in a reduced production of electricity by 247 %. In the third scenario, production of electricity is reduced by 104 % at maximum load with HPC. The HPC system has high-quality heat to utilize, probably enough to meet the district heating needs without increasing the boiler power. But heat optimization opportunities need to be further explored in order to be able to express something to a greater extent. The MEA process does not offer the same opportunities for heat utilization. As the CHP-plant have heat as the main product, HPC would be a more suitable alternative despite the high load on the electricity production. The performance of the carbon dioxide plant seems to vary between different operating cases and it can be concluded that the variation is related to the flue gas composition rather than being load dependent. Transport of carbon dioxide by train has the lowest carbon dioxide emissions and requires the least number of cargoes for transport from Karlstad to storage in Norway. However, this is not relevant at present because of the lack of rail connection to the plant. Total carbon sink is approximately 127 000 tonnes per year if the boiler capacity is assumed to be unchanged. / BECCS (Bioenergy Carbon Capture and Storage) är en viktig del av åtgärder i målet om att nå nollnetto utsläpp år 2050 globalt, då tekniken kan skapa kolsänkor. Tekniken är dock mycket energikrävande och dyr, och påverkar de befintliga systemen vid implementering. Syftet med den här studien är att undersöka möjligheten att implementera BECCS på Karlstad Energis biobränsleeldade kraftvärmeverk, Heden 3. Målet är att, genom simulering i CHEMCAD, ta fram förbrukningsnyckeltal för två olika avskiljningstekniker (MEA-MonoEtanolAmin och HPC-HotPotassiumCarbonate) med 90 % avskiljningsgrad vid tre olika driftfall. Dessutom ska systempåverkan på Heden 3 fastställas genom analys av tre olika scenarier. I första scenariot hålls bränsleförbrukningen oförändrad och ånga till koldioxidavskiljningssystemet tappas av innan turbinen. I det andra scenariot ökar bränsletillförseln för att tillgodose fjärrvärmebehovet i det befintliga systemet och ånga till koldioxidavskiljningssystemet tappas av innan turbinen. I det tredje scenariot hålls bränsletillförseln oförändrad och ånga extraheras från turbinen. Därtill undersöks i studien olika transportmöjligheter till lagringsplats av koldioxiden och slutligen beräknas den totala kolsänkan Karlstad Energi kan bidra med. Resultaten visar att elproduktionen i det första scenariot reduceras med 65-87 % för MEA och för HPC 151-238 %. Utan värmeutnyttjande från koldioxidavskiljningssystemen reduceras värmeproduktionen med 66-86 % med MEA och 54-76 % med HPC. I det andra scenariot krävs att bränsletillförseln ökar med 134 % för att tillgodose behoven vilket motsvarar mer än dubbla panneffekten och innebär en reducerad elproduktion på 247 %. I det tredje scenariot reduceras elproduktionen med 104 % vid maximal last med HPC.  I HPC-systemet finns högvärdig värme att utnyttja, sannolikt tillräckligt mycket för att kunna uppfylla fjärrvärmebehovet utan att öka panneffekten. Men värmeoptimeringsmöjligheter behöver undersökas ytterligare för att kunna uttrycka något i större omfattning. I MEA-processen finns inte samma möjligheter till värmeutnyttjande. Eftersom kraftvärmeverket har värme som främsta produkt skulle således HPC vara ett lämpligare alternativ trots den höga belastningen på elproduktionen. Koldioxidanläggningens prestanda förefaller variera mellan olika driftfall och med en enklare undersökning kunde slutsatsen dras att variationen har ett samband med rökgassammansättningen snarare än att det är ett lastberoende. Transport av koldioxid med tåg har lägst koldioxidutsläpp och kräver minst antal laster för transport från Karlstad till lagring i Norge. Detta är dock inte aktuellt i dagsläget på grund av avsaknaden av räls in till verket. Den totala kolsänkan är cirka 127 000 ton per år om pannan antas köras oförändrat.

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.