Life cycle analysis is carried out for 11 predicted configurations of pyrolysis biochar systems to determine greenhouse gas balance, using an original spreadsheet model. System parameters reflect deployment in Scotland, and results demonstrate that all major crop and forestry feedstocks offer greater GHG abatement than other bioenergy technologies, regardless of system configuration. Sensitivity analysis determines the relative importance of uncertain variables in the model and optimistic to pessimistic scenarios are used for system operation. Slow pyrolysis is compared to fast pyrolysis and biomass co-firing for GHG abatement and electricity production, using various scenarios for availability of indigenous Scottish feedstocks.

In an effort to reduce atmospheric carbon dioxide (CO2) emissions and mitigate climate change, it has been proposed to sequester supercritical CO2 in underground saline aquifers. Geological storage of CO2 involves different trapping mechanisms which are not yet fully understood. In order to improve the understanding of the effect of chemical reaction on the flow and transport of CO2, these storage mechanisms are modelled experimentally and numerically in this work. In particular, the destabilising interaction between the fluid hydrodynamics and a density-increasing second-order chemical reaction is considered. It is shown that after nondimensional scaling, the flow in a given physicochemical system is governed by two dimensionless groups, Da/Ra2, which measures the timescale for convection compared to those for reaction and diffusion, and CBo', which reflects the excess of the environmental reactant species relative to the diffusing solute. The destabilising reactive scenario is modelled experimentally under standard laboratory conditions using an immiscible two-layer system with acetic acid acting as the solute. A novel colorimetric technique is developed to infer the concentrations of chemical species from the pH of the solution making it possible to measure the flux of solute into the aqueous domain. The validity of this experimental system as a suitable analogue for the dissolution of CO2 is tested against previous work and the destabilising effect of reaction is investigated by adding ammonia to the lower aqueous layer. The system is also modelled numerically and it is shown that the aqueous phase reaction between acetic acid and ammonia can be considered to be instantaneous, meaning that Da/Ra2 tends to infinity and the flow is therefore governed only by the initial dimensionless concentration of reactant in the aqueous phase. The results from the experiments and numerical simulations are in good agreement, showing that an increase in the initial concentration of reactant increases the destabilising effect of reaction, accelerates the onset of convection and enhances the rate of dissolution of solute. The numerical model is then applied to a real world aquifer in the Sleipner gas field and it is demonstrated how the storage capacity of a potential CO2 reservoir could be enhanced by chemical reaction.

Implementing effective and environmentally responsible carbon capture technologies is one of the principle challenges of this century. Successful implementation requires a host of engineering advancements, but also a fundamental understanding of the underlying physics, chemistry, and materials science at play in these highly complex systems. A large body of scholarship examines both current technologies as well as future strategies, but to date little exploration of the surface behavior of these systems has been examined. As these carbon capture systems involve uptake of gaseous CO2 to either aqueous or solid substrates, understanding the chemistry and physics governing the boundary between the two reactant phases is critical. Yet probing the unique chemistry and physics of these interfacial systems is very difficult. This dissertation addresses this knowledge gap by examining the surface chemistry of monoethanolamine and CO2. Monoethanolamine is a simple organic amine currently used in small scale CO2 scrubbing, and acts as an industrial benchmark for CO2 capture efficiency. The studies presented throughout this dissertation employ surface selective techniques, including vibrational sum frequency spectroscopy, surface tensiometry, and computation methodologies, in order to determine the behavior governing aqueous amine interfaces. The adsorption behavior and surface orientation of aqueous monoethanolamine is examined first. The results show monoethanolamine is present at the surface, highly ordered, and solvated. Perturbations to this amine surface from gaseous CO2 and SO2, as well as from liquid HCl, are examined in the remainder of the dissertation. Reactions between the amine and acids are shown to cause immediate changes to the interface, but the interface then remains largely unaffected as further reaction evolves. The studies presented herein provide a needed exploration of the interfacial picture of these highly reactive systems, with implications for future carbon capture materials and design.

The rapid electrification through natural gas in Mexico; the interest of the country to mitigate the effects of climate change; and the opportunity for rolling out Enhanced Oil Recovery at national level requires an important R&D effort to develop nationally relevant CCS technology in natural gas combined cycle power plants. Post-combustion carbon dioxide capture at gas-fired power plants is identified and proposed as an effective way to reduce CO2 emissions generated by the electricity sector in Mexico. In particular, gas-fired power plants with carbon dioxide capture and the sequential combustion of supplementary natural gas in the heat recovery steam generator can favourably increase the production of carbon dioxide, compared to a conventional configuration. This could be attractive in places with favourable conditions for enhanced oil recovery and where affordable natural gas prices will continue to exist, such as Mexico and North America. Sequential combustion makes use of the excess oxygen in gas turbine exhaust gas to generate additional CO2, but, unlike in conventional supplementary firing, allows keeping gas temperatures in the heat recovery steam generator below 820°C, avoiding a step change in capital costs. It marginally decreases relative energy requirements for solvent regeneration and amine degradation. Power plant models integrated with capture and compression process models of Sequential Supplementary Firing Combined Cycle (SSFCC) gas-fired units show that the efficiency penalty is 8.2% points LHV compared to a conventional natural gas combined cycle power plant with capture. The marginal thermal efficiency of natural gas firing in the heat recovery steam generator can increase with supercritical steam generation to reduce the efficiency penalty to 5.7% points LHV. Although the efficiency is lower than the conventional configuration, the increment in the power output of the combined steam cycle leads a reduction of the number of gas turbines, at a similar power output to that of a conventional natural gas combined cycle. This has a positive impact on the number of absorbers and the capital costs of the post-combustion capture plant by reducing the total volume of flue gas by half on a normalised basis. The relative reduction of overall capital costs is, respectively, 9.1% and 15.3% for the supercritical and the subcritical combined cycle configurations with capture compared to a conventional configuration. The total revenue requirement, a metric combining levelised cost of electricity and revenue from EOR, shows that, at gas prices of 2$/MMBTU and for CO2 selling price from 0 to 50 $/tonneCO2, subcritical and supercritical sequential supplementary firing presents favourably at 47.3-26 $/MWh and 44.6-25 $/MWh, respectively, compared with a conventional NGCC at 49.5-31.7 $/MWh. When operated at part-load, these configurations show greater operational flexibility by utilising the additional degree of freedom associated with the combustion of natural gas in the HRSG to change power output according to electricity demand and to ensure continuity of CO2 supply when exposed to variation in electricity prices. The optimisation of steady state part-load performance shows that reducing output by adjusting supplementary fuel keeps the gas turbine operating at full load and maximum efficiency when the net power plant output is reduced from 100% to 50%. For both subcritical and supercritical combined cycles, the thermal efficiency at part-load is optimised, in terms of efficiency, with sliding pressure operation of the heat recovery steam generator. Fixed pressure operation is proposed as an alternative for supercritical combined cycles to minimise capital costs and provide fast response rates with acceptable performance levels.

Geological carbon dioxide (CO2) storage in the United Kingdom (UK) will likely be entirely offshore, which may lead to the production and disposal into the sea of reservoir waters to increase storage capacity, or through CO2-Enhanced Oil Recovery (CO2-EOR). These produced waters have the potential to contain significant concentrations of trace metals that could be of harm to the environment. Batch experiments with CO2, warm brines, and reservoir sandstones were undertaken for this thesis to determine concentrations of 8 trace metals (arsenic, cadmium, chromium, copper, mercury, nickel, lead, zinc) which could be leached during CO2 storage in 4 UK North Sea hydrocarbon reservoirs. A sequential extraction procedure (SEP) was also used to determine the potential mobility of these metals under CO2 storage from mineral phases making up the reservoir samples. The results broadly showed that mobilised trace metal concentrations were low (parts per billion, ppb) in the batch experiments, with the exceptions of nickel and zinc. These metals were associated with carbonate and some feldspar dissolution, with other metals apparently desorbed from mineral surfaces, probably clays. The results of the SEP, however, were a poor predictor of actual mobility with respect to the batch experiments, although useful in determining the distribution of trace metals within the defined mineral phases (water soluble, ion exchangeable, carbonate, oxide, sulphide, silicate). In addition, fieldwork was carried out at Green River, Utah, to collect 10 CO2-driven spring water samples and 5 local aquifer rock samples. This area was used as a natural analogue for CO2-mobilised trace metals from sandstone aquifers. Trace metal concentrations in spring waters were very low (ppb) and batch experiments using Utah rock samples, spring water collected from Crystal Geyser, and CO2 confirmed very low mobility of these metals. The SEP was repeated for the Utah reservoir rocks, but again was not a reliable predictor for actual mobility, other than to confirm that overall bulk concentrations of trace metals was low. Comparison of trace metal concentrations from the batch experiments with data from UK North Sea oil and gas produced waters shows that overall, concentrations mobilised in batch experiments are within the range of concentrations across all North Sea fields reporting their data. However, on a field-by-field basis, some CO2 mobilised concentrations exceeded those currently produced by oil and gas activities. Furthermore, average batch experiment trace metal loads are higher than average oil and gas produced waters, and in some cases exceed international guidelines. Therefore, while the majority of trace metals have low mobility and therefore low environmental impact, this should be assessed on a case-by-case basis. Regular monitoring of dissolved constituents in produced waters carried should also be carried out, particularly in the initial stages of CO2 storage operations, with remedial action taken as required to reduce the environmental impact of offshore carbon capture and storage.

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No description available.

Global warming is becoming ever increasing concern in our society. As such the likelihood of a carbon tax in the US is becoming increasingly likely. A carbon tax will be expensive enough that coal-based power plants will either have to install carbon capture technology or close. The two front runner technologies for carbon capture are amine scrubbing, and oxyfuel combustion. The downside is that both of these technologies increase power generation cost in a new plant by about 80% and have up to a 30% parasitic load, which reduces the cycle efficiency, that is, the power production per unit fuel consumed, by the same 30%. Retrofitting existing plants by either of these technologies is even more expensive and inefficient since it requires major modifications or replacement of the existing plant in addition to the new capture technology. Sustainable Energy Solutions (SES) has developed a carbon capture technology named cryogenic carbon capture (CCC). CCC is a process by which the flue gas cools to the point that CO2 desublimates. This process is more efficient, cheaper, and has about half of the parasitic load of other technologies, approaching the theoretical minimum in CO2 separation within heat exchanger and compressor efficiencies. This thesis conceptually describes, experimentally characterizes, and theoretically models one desublimating heat exchanger as an integral part of the CCC process. A spray tower conceptually developed by SES and theoretically and experimentally explored in previous work at lab scale is developed at bench scale in this work with accompanying major modifications to the theoretical model. It sprays a cold contact liquid to cool warm gas (relative to the contact liquid) that travels up the tower. Nominal operating temperatures are around -120 to -130 °C for 90% and 99% capture, respectively. Once the flue gas cools enough, CO2 desublimates on the liquid droplet surfaces and forms a slurry with the contact liquid. This spray tower can achieve arbitrarily high CO2 capture efficiency, depending on the temperature of the exiting gas and other operational variables. The experimental data outlined here varied these operational parameters over broad ranges to achieve capture efficiencies of 55% to greater than 95%, providing a robust data set for model comparison. The operational parameters explored include liquid temperature, liquid flow rate, gas flow rate, and droplet size. These data validated a transport and design model that predicts capture for future scale-up and design of the project. The data and model indicate expected behaviors with most of these variables and a dependence on internal droplet temperature profiles that may be higher than expected. This project significantly advanced the experimental database and the model capabilities that describe the spray tower.

Carbon capture, utilization and storage (CCUS) in confined saline aquifers in sedimentary formations has the potential to reduce the impact of fossil fuel combustion on climate change by storing CO2 in geologic formations in perpetuity. At PT conditions relevant to CCUS, CO2 is less dense than the pre-existing brine in the formation, and the more buoyant CO2 will migrate to the top of the formation where it will be in contact with cap rock. A typical cap rock is clay-rich shale, and interactions between shales and CO2 are poorly understood at PT conditions appropriate for CCUS in saline formations. In this study, the interaction of CO2 with clay minerals in the cap rock overlying a saline formation has been examined, using Na-rich montmorillonite as an analog for clay-rich shale. Attenuated Total Reflectance -- Fourier Transform Infrared Spectroscopy (ATR -FTIR) was used to identify potential crystallographic sites (AlAlOH, AlMgOH and interlayer space) where CO2 could interact with montmorillonite at 35"C and 50"C and from 0-1200 psi.  Analysis of the data indicates that CO2 that is preferentially incorporated into the interlayer space, with dehydrated montmorillonite capable of incorporating more CO2 than hydrated montmorillonite. No evidence of chemical interactions between CO2 and montmorillonite were identified, and no spectroscopic evidence for carbonate mineral formation was observed.  Further work is needed to determine if reservoir seal quality is more likely to be degraded or enhanced by CO2 - montmorillonite interactions. / Master of Science

The Paris Agreement aims to limit global warming to 1.5 degrees Celsius, and Sweden has set a goal toreach net-zero emissions by 2045. Carbon Capture and Storage (CCS) is one method that can reducecarbon dioxide emissions. The industry and transportation sectors are the biggest sources of emissionsin Sweden, requiring technological developments and increased investment to reduce their carbondioxide (CO2) emissions. The Geological Survey of Sweden (SGU) is responsible for controls,supervision, operation, and construction of activities connected with carbon dioxide (CO2) storage. SGUbelieves that the storage conditions in Sweden are poor. Sedimentary, basaltic and ultramafic rock ispreferable for CO2 storage, but finding the right sort of bedrock at the right depth and with the rightvolumes and porosity is the challenge. Hence it is in question to collaborate with nations in the northern sea, in order to transport and storageCO2 which would lessen the burden of needing to build new infrastructure. There are a few upcomingCarbon Capture and Utilisation (CCU) projects in Sweden but from the industry’s point of view, thepriority seems to be mostly on Bio-CCS. However, there is still interest for CCS technology in industrialproduction such as steel or cement and also Direct Air Capture (DAC) in the near future. Due to thehigh cost of CCS, funding through the Swedish Energy Agency and EU is vital in order to make iteconomically viable. Other Cost reducing solutions such as relocation on old oil and gas fields orarranging CCS hubs are possible. In summary, this study concludes that CCS is not currently a feasible technique in order to reduce CO2 from the atmosphere, given the current state and costs for it. If the technology becomes more energyefficient and when financial means are in place, the future is bright for CCS. It is extremely relevantthat this technology continues to develop into a better, cheaper and faster way to capture CO2 and reduceemissions of the effective greenhouse gases. / Parisavtalet syftar till att begränsa den globala uppvärmningen till 1,5 grader Celsius och Sverige harockså satt som mål att nå nettonollutsläpp till år 2045. Ett sätt att nå dessa mål kan vara med teknikenför Carbon Capture and Storage (CCS) som är en metod för att minska koldioxidhalten i atmosfären.Den här rapporten syftar till att undersöka med hjälp av litteraturstudier och intervjuer hur genomförbarCCS är som teknik för att minska koldioxidutsläppen samt hur man även kan minska på den befintligamängden koldioxid som redan finns i luften. Huvudfokuset är att undersöka hur CCS fungerar och vilkakostnader som är involverade. Eftersom koldioxid (CO2) är en av de växthusgaser som bidrar mest tillden globala uppvärmningen är det viktigt att vidta åtgärder för att minska den. Det är inte bara utsläppenav CO2 som måste minska utan även mängden CO2 som redan finns i atmosfären. Forskning kring CCSär därför viktig för att hitta nya sätt att effektivisera metoden och göra den mer genomförbar. Naturvårdsverket ger ut en årlig rapport som utvärderar landets framsteg mot att nå sina miljömål,inklusive “Begränsad klimatpåverkan”. Rapporten konstaterar att även om EU och Sverige har minskatutsläppen ökar de fortfarande globalt sett. Industri- och transportsektorn identifieras som de störstautsläppskällorna i Sverige. Den svenska förordningen om CCS regleras av miljöbalken som testar kollagringi geologiska formationer som en miljöfarlig verksamhet och den separerade CO2 ses som avfall.Sverige har ännu inte någon kommersiell CCS-anläggning men regeringen har föreslagit att svenskaindustrier bör införa CCS för att minska dessa utsläpp. Både Sverige och EU har investerat i att utvecklateknik för att minska användningen av fossila bränslen och underlätta för användningen av CCS. CCS processen består av tre huvudsteg: avskiljning och separering av CO2, transport samt lagring elleråteranvändning. Alla typer av nuvarande CCS-metoder kräver en stor mängd energi och de flesta avdem separerar CO2 från industriella förbränningar. Direct Air Capture (DAC) är en annaninfångningsteknik som är mer flexibel när det gäller placering, men också dyrare än de andra teknikerna.Transporten av den infångade CO2 kan ske med lastbil, tåg, fartyg eller rör. De mest genomförbaraalternativen är dock rörledningar och via fartyg på grund av deras transportkapacitet. Rörledningarkräver en välutvecklad infrastruktur, vilket gör dem kostsamma, men de är det mest genomförbaraalternativet för att separera CO2 från landbaserade anläggningar och transportera dem till närliggandelagringsplatser. Geologisk lagring av CO2 kan göras både på land och till havs. Injektion till dengeologiska formationen vid lagringsplatser sker via borrhål. CO2 förvätskas och ersätter denursprungliga vätskan i bergmaterialets porer i berggrunden och reagerar så småningom med berget ochbildar nya mineraler i berggrunden. Sveriges Geologiska Undersökning (SGU) ansvarar för kontroller, tillsyn, drift och uppförande avverksamheter kopplade till CO2-lagring. Geologin i Sverige lämpar sig dock generellt sett inte förlagring av CO2, förutom för vissa sydliga områden. Nordsjön har en del gynnsamma förutsättningar förCO2-lagring och det finns även potentiella geologiska formationer i södra Östersjön. Sedimentära,basaltiska eller ultramafiska bergarter är att föredra för geologisk CO2-lagring. Den största utmaningenär att hitta rätt sorts berggrund på rätt djup och med rätt volym och porositet. Den största svårigheten med CCS är den höga kostnaden, vilket bidrar till att hämma den utbreddaanvändningen. Kostnaden för CCS inkluderar olika faktorer som infångningsmetod, transportmedel,lagringsplats och övervakning över lagringen. Bland dessa är infångningen den dyraste fasen avtekniken, följt av lagring, transport och övervakning. Kostnaderna för varje fas har analyserats över2olika intervaller med hänsyn till lägre, medelstora och högre kostnader men även beroende på regiondå kostnaden kan variera beroende på ländernas förutsättningar. Infångningsfasen av CCS har betydande kostnadsvariationer beroende på vilken metod som används,renheten hos den infångade CO2 samt den energi som krävs för avskiljningsprocesserna.Högkoncentrerade CO2-strömmar har lägre bearbetningskostnader än lågkoncentrerade. DAC är förnärvarande den dyraste infångningsmetoden. Transportkostnader för CO2 inkluderar kostnaderrelaterade till infrastruktur, drift, underhåll, konstruktion och markanvändning. Kostnaden för transportmed rör beror på faktorer som diameter, avstånd och flödeshastighet. Högre flödeshastigheter genomrörledningar kan minska transportkostnaderna. Lagringskostnader för CO2 omfattar utgifter förborrning, infrastruktur, projektledning, licensiering och platsval. Geologisk lagring på land är förnärvarande mer kostnadseffektivt på grund av de utmaningar och högre kostnader som är förknippademed geologisk lagring till havs. Övervakningskostnader är till exempel screening och utvärdering avlagringsplatser samt uppgifter som datainsamling, platsrankning, brunnsinstallation och seismiskautvärderingar. Att minska energitillgången för infångning, förbättra val av lösningsmedel vid separationsfasen,återanvända och utveckla befintlig infrastruktur är exempel som kan hjälpa till att sänka kostnadernaför CCS-processen och främja en bredare användning. Ett annat förslag för att öka den ekonomiskalönsamheten är genom att implementera CCS nav eller kluster. Dessa CCS nav eller kluster ger företagmöjligheten att samordna infrastrukturen för sina CCS-anläggningar. Detta kan lindra den ekonomiskabördan att bygga upp egen kostsam infrastruktur. Nedlagda olje- och gasfält kan återbrukas för CCS- anläggningar då efterfrågan av fossila bränslenminskar. Istället för att riva ner verksamheterna för fossilt bränsle, exploatera ny mark och borra nyahål kan olje- och gasfälten i exempelvis norra haven återbrukas för CCS- anläggningar. Danmark är ettav de första länderna som har tagit initiativet att omvandla oljeanläggningar till koldioxidlagringanläggningar. Det är möjligt att söka om ekonomiskt stöd från Energimyndigheten eller EU för att få stöd till främstBio-CCS projekt men även andra. Detta är i syfte för att underlätta en fri marknad för tekniker somimplementerar koldioxidinfångst. Ambitionen med detta stödsystem är för att realisera en infångst av10 miljoner CO2 via Bio-CCS och minst 2 miljoner CO2/år för andra CCS tekniker. Genom omvändauktion får det företag som kan erbjuda infångad CO2/ton med Bio-CCS teknik för lägst pris, ta del avstödsystemet. EU har även initiativ att finansiera CCS-projekt genom CETPartnership eller EU:sinnovationsfond vars syfte är att stödja forskning och innovation inom CCS. Sammanfattningsvis kom denna studie fram till att CCS inte är genomförbart idag som en teknik för attminska CO2 från atmosfären med hänsyn till nuläget och kostnaderna för att implementera. Om teknikenenergi effektiviseras och när ekonomiska medel finns på plats är framtiden ljus för CCS. Det är oerhörtrelevant att denna teknik fortsätter att utvecklas till ett bättre, billigare och snabbare sätt att fånga uppCO2 och minska utsläppen av de effektiva växthusgaserna. Regeringen och industrin måste därförsamarbeta bättre för att underlätta regelverk som främjar och möjliggör samarbete inom CCS-branschendå många myndigheter lyfter fram att CCS är en nödvändig teknik för framtiden för att uppnå klimatneutralitet.