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Thesis (Ph. D.)--Ohio State University, 2005. / Title from first page of PDF file. Document formatted into pages; contains xx, 176 p.; also includes graphics (some col.). Includes bibliographical references (p. 169-176). Available online via OhioLINK's ETD Center

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Thesis (Ph.D.)--University of Nebraska-Lincoln, 2006. / Title from title screen (site viewed April 26, 2007). PDF text: vii, 158 p. : ill. UMI publication number: AAT 3221294. Includes bibliographical references. Also available in microfilm and microfiche formats.

To decrease carbon dioxide emissions into the atmosphere for climate change mitigation it is necessary to modify existing practices in processes where greenhouse gases are emitted. Due to the extremely large volumes of carbon dioxide produced globally, it is generally accepted that although carbon dioxide conversion and utilisation will contribute in the long term, in the short to medium term it will be necessary to capture and store carbon dioxide emissions to progress towards a low carbon future. Current industrial capture processes incur large energy and thus economic penalties. Storage in geological formations requires robust confidence in storage security to be publically accepted. Therefore the objective of this work was to study carbon dioxide capture and storage in processes directly confronting these two major challenges. Carbon dioxide adsorption on oxide materials for advanced carbon capture processes with lower energetic and economic penalties was investigated. Water was shown to play a crucial role in determining the presence of reactive sites, the speciation of carbonates formed and increased sorbent utilisation. A high surface area oxide with specifically exposed facets was prepared and the impact of these facets on carbon dioxide uptake performance was assessed. Volumetric gas adsorption and isotherm modelling supported the presence of two distinct adsorption sites. To enhance confidence in storage security it is necessary to understand storage processes that result in stable products. An apparatus capable of obtaining geological storage conditions was developed and carbonate formation and surface hydration at high pressure was investigated. By locating individual reactive cations on the surface of silica, silicate mineral analogues were prepared. It was shown that carbonate speciation was dependent on the reactive cation and the presence or absence of water.

Kyoto University (京都大学) / 0048 / 新制・課程博士 / 博士(工学) / 甲第17131号 / 工博第3621号 / 新制||工||1550(附属図書館) / 29870 / 京都大学大学院工学研究科社会基盤工学専攻 / (主査）教授 松岡 俊文, 教授 大津 宏康, 准教授 水戸 義忠 / 学位規則第4条第1項該当

The most widely advocated method of carbon capture and storage involves the injection of CO2 into underground geological formations. Key to the development of this geological sequestration technology is the existence of suitable high-integrity geological sites for the safe, long-term storage of CO2. Unlike depleted oil and gas reservoirs which are historically proven to be well-defined, formations with saline brines may not have a similar proven sealing capacity. In the main, complex geochemical reactions occur in the supercritical CO2 / brine / host rock environment which can cause significant changes in the porosity, permeability and injectivity of the formation. Depending of the nature of the processes, the effects of the underground injection of CO2 may (1) yield increased storage capacity of the target horizon, or (2) lead to increased potential for leakage beyond the confining layers of the saline formation, or (3) impede the injection exercise as a whole. It is conceivable that accelerated, localized mineral carbonation could be induced at strategic places between the CO2 plume and fault zones or facies changes present in deep saline formations, in order to prevent the migration of CO2 outside the confined layers of the reservoir. The South African electricity producer, Eskom, generated 36.01 million tons of coal- combustion fly ash in 2010. About 5.6% were reused for the production of cement. The remaining 33.89 million tons were safely disposed of and managed on Eskom ash dumps and dams which are located adjacent to their corresponding power stations. South Africa has a long history regarding the development of new applications for this material and is very active in the development of ash technologies. Concurrently, the power industry is also a major carbon dioxide (CO2 ) emitter, with Eskom’s emissions approximating 225 million tons for 2010. In this study, the author introduces a theoretical concept whereby fly ash in a slurry form could be injected at strategic sites of deep saline formations. The purpose of this injection strategy is to prevent the migration of injected anthropogenic CO2 plumes beyond the confining layers of the formations, via induced in situ localized, accelerated mineral carbonation. The proposed application falls within the carbon capture and storage (CCS) initiative by geological sequestration and aims at improving the integrity of deep saline formations which may be at risk of leakage upon injection of CO2. The use of coal-combustion fly ash in industrial mineral carbonation and the research involving its applications in carbon capture and storage (CCS) has internationally gained increased attention. However, the work involving fly ash in industrial mineral carbonation has only focused on the sequestration of sub-critical CO2. This work demonstrates for the first time that fly ash can react with supercritical CO2 under varying pressure and temperature conditions. The experiments were conducted following an assumed geothermal gradient for deep saline reservoirs, as described by Viljoen, 2010, i.e. 44°C/80bar and 50°C/100bar. Ultra-pure water was used as a solvent. The duration of experiments ranged from 60 minutes to 7 days. Under these T/ P conditions, carbonates in the form of calcite (CaCO3 ) were only detected at completion of the 7 days experiment. Further investigation was undertaken at 90°C/90bar for 2 hours using synthetic brine as a solvent, in order to mimic the composition of deep saline formations. This work yielded both aragonite and calcite, which formed as sheets at the base and on the walls of the batch reactor. The carbonated sheet fragments were examined using scanning electron microscopy (SEM) and were found to have an approximate thickness of 16 μm. A thinner layer of white precipitate on the walls of the reactor was composed of aragonite and calcite and contained an amorphous phase of carbonate of ca. 1% by volume. The mineralogical composition of these carbonated sheets was confirmed using XRD, which demonstrated the presence of aragonite (23%), calcite (3%) and fly ash minerals (e.g. mullite, quartz). It also contained an XRD-amorphous phase of about 37%. These sheets were thus enriched in calcium and carbon but also other elements were found to be present (Al, Si, Na, Mg and Cl) as shown by SEM. It is, however, unclear whether these elements identified in the spectrum are part of the sheet or are rather indicative of an effect of analytical volume created by the SEM electron beam being larger than the thickness of the sheet. Small amounts of S were also detected. Fly ash particles as well as a small number of needle-shaped gypsum crystals were visibly embedded in the sheet (SEM). Copyright / Dissertation (MSc)--University of Pretoria, 2012. / Geology / unrestricted

<p>Increasing CO₂ concentrations in the Earth's atmosphere have led to global warming with climate change effects. Future RCP scenarios per the IPCC suggest that local solutions to limit emissions are necessary but may not suffice to combat the anthropogenic CO₂ problem. Climate intervention has been given increasing consideration. A climate intervention approach of removing CO₂ from the atmosphere through dry ice deposition and storage in Antarctica is considered. While the technology needs continued development, understanding the meteorological response to significant carbon dioxide removal (CDR) in Antarctica takes precedence. Various Antarctica CDR scenarios are simulated through the fully-coupled general circulation model CESM 2.1.1. Modern simulations (15 years) with prognostic CO₂ include 1) anthropogenic emissions (control), 2) no emissions, 3) emissions with ~4.5 ppmv sequestration annually (half sequestration), and 4) emissions with ~9 ppmv sequestration annually (full sequestration). Full sequestration attempts to remove enough CO₂ to achieve pre-industrial concentration by the end of the simulation. Experiments 1) and 3) were continued until mid-21st century (50 years total) with SSP1-2.6 conditions and emissions to examine the CDR impact on the atmosphere under the Paris Treaty Agreement scenario (which limits Earth's warming to 1.5^oC-2^oC above pre-industrial values). </p> <p> Modern simulations show sequestration scenarios have more of an impact on 2m-air temperature and little effect on precipitation patterns in 15 years. SSP1-2.6 simulations show that an additional 1^oC of warming can be inhibited by continuing sequestration and limiting emissions. Further, sequestration shows counteraction to warming in many of the locations that are predicted to warm per the RCP 2.6 scenario in the IPCC (2013), as well as counteraction to the predicted IPCC precipitation changes. These results are obtained from one simulation of each experiment, and it is recognized that ensemble runs in line with IPCC predictions are necessary to examine all possible predictions to CDR. Future considerations include sea level rise, carbon cycle response, convective parameters, and relocation of sequestration.<a></a></p>

This study was designed to understand the possible impact of carbon dioxide on different reservoir rocks in south-central Mississippi. Eight samples, including six from the Heidelberg field (Mississippi), were exposed to carbon dioxide under simulated subsurface conditions of elevated temperature and pressure and then analyzed using thin section petrography, scanning electron microscopy, X-ray diffraction, and focused ion beam-SEM. Three of the eight samples showed dissolution in calcite and corrosion in smectite. SEM and EDS analysis of treated sample 5 (Se-5/shaly-sandtsone) and sample 8 (S-8/dolomitic-limestone) revealed newly precipitated lath- and fibrous-like crystals composed of sulfur (S), oxygen (O), and calcium (Ca), thus interpreted as gypsum. Three-dimensional analysis using FIB of dolomitic limestone samples (Smackover Formation) revealed that gypsum crystals fill fracture porosity. This study significantly contributes to the understanding of carbon dioxide impact on reservoir rock and promotes better management of natural gas resources.

The objective of this study was to develop a protocol to test the reactivity of glauconite, a Fe/Mg bearing aluminosilicate mineral, in carbon storage. A selected glauconite-rich sample from the Cambrian Riley Formation of Central Texas was used containing glauconite 38 wt%, quartz 58 wt%, and calcite 4 wt%. Ten experiments were conducted using two techniques where total pressure was: 1) controlled by delivering CO2 to a high-pressure apparatus; 2) kept at saturated vapor level in autoclaves. The treated glauconite samples were analyzed with Scanning Electron Microscopy (SEM), Energy Dispersive Spectroscopy (SEM), and X-ray Diffraction techniques (XRD). Although the reaction between glauconite and CO2 was not visible, calcite crystallized in solution when its pH exceeded the value of 6.88. The research provides a foundation to develop further investigations of rock reactions under CO2 saturated conditions.