Pathways towards large-scale implementation of CO2 capture and storage: A case study for the Netherlands

We sketch four possible pathways how carbon dioxide capture and storage (CCS) (r)evolution may occur in the Netherlands, after which the implications in terms of CO₂ stored and avoided, costs and infrastructural requirements are quantified. CCS may play a significant role in decarbonising the Dutch energy and industrial sector, which currently emits nearly 100 Mt CO₂/year. We found that 15 Mt CO₂ could be avoided annually by 2020, provided some of the larger gas fields that become available the coming decade could be used for CO₂ storage. Halfway this century, the mitigation potential of CCS in the power sector, industry and transport fuel production is estimated at maximally 80–110 Mt CO₂/year, of which 60–80 Mt CO₂/year may be avoided at costs between 15 and 40 €/t CO₂, including transport and storage. Avoiding 30–60 Mt CO₂/year by means of CCS is considered realistic given the storage potential represented by Dutch gas fields, although it requires planning to assure that domestic storage capacity could be used for CO₂ storage. In an aggressive climate policy, avoiding another 50 Mt CO₂/year may be possible provided that nearly all capture opportunities that occur are taken. Storing such large amounts of CO₂ would only be possible if the Groningen gas field or large reservoirs in the British or Norwegian part of the North Sea will become available.     

CCS scenarios optimization by spatial multi-criteria analysis: Application to multiple source sink matching in Hebei province

A method, based on spatial analysis of the different criteria to be taken into consideration for building scenarios of CO₂ capture and storage (CCS), has been developed and applied to real case studies in the Hebei province. Totally 88 point sources (42 from power sector, 9 from iron and steel, 18 from cement, 16 from ammonia, and 3 from oil refinery) are estimated and their total emission amounts to 231.7 MtCO₂/year with power, iron and steel, cement, ammonia and oil refinery sharing 59.13%, 25.03%, 11.44%, 3.5%, and 0.91%, respectively. Storage opportunities can be found in Hebei province, characterised by a strong tectonic subsidence during the Tertiary, with several kilometres of accumulated clastic sediments. Carbon storage potential for 25 hydrocarbon fields selected from the Huabei complex is estimated as 215 MtCO₂ with optimistic assumption that all recovered hydrocarbon could be replaced by an equivalent volume of CO₂ at reservoir conditions. Storage potential for aquifers in the Miocene Guantao formation is estimated as 747 MtCO₂ if closed aquifer assumed or 371 MtCO₂ if open aquifer and single highly permeable horizon assumed. Due to poor knowledge on deep hydrogeology and to pressure increase in aquifer, injecting very high rates requested by the major CO₂ sources (>10 MtCO₂/year) is the main challenge, therefore piezometry and discharge must be carefully controlled. A source sink matching model using ArcGIS software is designed to find the least-cost pathway and to estimate transport route and cost accounting for the additional costs of pipeline construction due to landform and land use. Source sink matching results show that only 15–25% of the emissions estimated for the 88 sources can be sequestrated into the hydrocarbon fields and the aquifers if assuming sinks should be able to accommodate at least 15 years of the emissions of a given source.     

Geological storage of CO2 in saline aquifers—A review of the experience from existing storage operations

The experience from CO₂ injection at pilot projects (Frio, Ketzin, Nagaoka, US Regional Partnerships) and existing commercial operations (Sleipner, Snøhvit, In Salah, acid-gas injection) demonstrates that CO₂ geological storage in saline aquifers is technologically feasible. Monitoring and verification technologies have been tested and demonstrated to detect and track the CO₂ plume in different subsurface geological environments. By the end of 2008, approximately 20 Mt of CO₂ had been successfully injected into saline aquifers by existing operations. Currently, the highest injection rate and total storage volume for a single storage operation are approximately 1 Mt CO₂/year and 25 Mt, respectively. If carbon capture and storage (CCS) is to be an effective option for decreasing greenhouse gas emissions, commercial-scale storage operations will require orders of magnitude larger storage capacity than accessed by the existing sites. As a result, new demonstration projects will need to develop and test injection strategies that consider multiple injection wells and the optimisation of the usage of storage space. To accelerate large-scale CCS deployment, demonstration projects should be selected that can be readily employed for commercial use; i.e. projects that fully integrate the capture, transport and storage processes at an industrial emissions source.     

Methodology for CO2 chain analysis

The paper presents a methodology for CO₂ chain analysis with particular focus on the impact of technology development on the total system economy. The methodology includes the whole CO₂ chain; CO₂ source, CO₂ capture, transport and storage in aquifers or in oil reservoirs for enhanced oil recovery. It aims at supporting the identification of feasible solutions and assisting the selection of the most cost-effective options for carbon capture and storage. To demonstrate the applicability of the methodology a case study has been carried out to illustrate the possible impact of technology improvements and market development. The case study confirms that the CO₂-quota price to a large extent influence the project economy and dominates over potential technology improvements. To be economic feasible, the studied chains injecting the CO₂ in oil reservoirs for increased oil production require a CO₂-quota price in the range of 20–27 €/tonne CO₂, depending on the technology breakthrough. For the chains based on CO₂ storage in saline aquifers, the corresponding CO₂-quota price varies up to about 40 €/tonne CO₂.     

Modeling the impacts of climate policy on the deployment of carbon dioxide capture and geologic storage across electric power regions in the United States

This paper summarizes the results of a first-of-its-kind holistic, integrated economic analysis of the potential role of carbon dioxide (CO₂) capture and storage (CCS) technologies across the regional segments of the United States (U.S.) electric power sector, over the time frame 2005–2045, in response to two hypothetical emissions control policies analyzed against two potential energy supply futures that include updated and substantially higher projected prices for natural gas. This paper's detailed analysis is made possible by combining two specialized models developed at Battelle: the Battelle CO₂-GIS to determine the regional capacity and cost of CO₂ transport and geologic storage; and the Battelle Carbon Management Electricity Model, an electric system optimal capacity expansion and dispatch model, to examine the investment and operation of electric power technologies with CCS against the background of other options. A key feature of this paper's analysis is an attempt to explicitly model the inherent heterogeneities that exist in both the nation's current and future electricity generation infrastructure and in its candidate deep geologic CO₂ storage formations. Overall, between 180 and 580 gigawatts (GW) of coal-fired integrated gasification combined cycle with CCS (IGCC + CCS) capacity is built by 2045 in these four scenarios, requiring between 12 and 41 gigatonnes of CO₂ (GtCO₂) storage in regional deep geologic reservoirs across the U.S. Nearly all of this CO₂ is from new IGCC + CCS systems, which start to deploy after 2025. Relatively little IGCC + CCS capacity is built before that time, primarily under unique niche opportunities. For the most part, CO₂ emissions prices will likely need to be sustained at over $20/tonne CO₂ before CCS begins to deploy on a large scale within the electric power sector. Within these broad national trends, a highly nuanced picture of CCS deployment across the U.S. emerges. Across the four scenarios studied here, power plant builders and operators within some North American Electric Reliability Council (NERC) regions do not employ any CCS while other regions build more than 100 GW of CCS-enabled generation capacity. One region sees as much as 50% of its geologic CO₂ storage reservoirs’ total theoretical capacity consumed by 2045, while most of the regions still have more than 90% of their potential storage capacity available to meet storage needs in the second half of the century and beyond. A detailed presentation of the results for power plant builds and operation in two key regions: ECAR in the Midwest and ERCOT in Texas, provides further insight into the diverse set of economic decisions that generate the national and aggregate regional results.     

Carbon dioxide storage capacity in uneconomic coal beds in Alberta,Canada: Methodology,potential and site identification

Methodology is presented for a first-order regional-scale estimation of CO₂ storage capacity in coals under sub-critical conditions, which is subsequently applied to Cretaceous-Tertiary coal beds in Alberta, Canada. Regions suitable for CO₂ storage have been defined on the basis of groundwater depth and CO₂ phase at in situ conditions. The theoretical CO₂ storage capacity was estimated on the basis of CO₂ adsorption isotherms measured on coal samples, and it varies between ∼20 kt CO₂/km² and 1260 kt CO₂/km², for a total of approximately 20 Gt CO₂. This represents the theoretical storage capacity limit that would be attained if there would be no other gases present in the coals or they would be 100% replaced by CO₂, and if all the coals will be accessed by CO₂. A recovery factor of less than 100% and a completion factor less than 50% reduce the theoretical storage capacity to an effective storage capacity of only 6.4 Gt CO₂. Not all the effective CO₂ storage capacity will be utilized because it is uneconomic to build the necessary infrastructure for areas with low storage capacity per unit surface. Assuming that the economic threshold to develop the necessary infrastructure is 200 kt CO₂/km², then the CO₂ storage capacity in coal beds in Alberta is greatly reduced further to a practical capacity of only ∼800 Mt CO₂.     

The potential for increased atmospheric CO2 emissions and accelerated consumption of deep geologic CO2 storage resources resulting from the large-scale deployment of a CCS-enabled unconventional fossil fuels industry in the U.S.

Desires to enhance the energy security of the United States have spurred renewed interest in the development of abundant domestic heavy hydrocarbon resources including oil shale and coal to produce unconventional liquid fuels to supplement conventional oil supplies. However, the production processes for these unconventional fossil fuels create large quantities of carbon dioxide (CO₂) and this remains one of the key arguments against such development. Carbon dioxide capture and storage (CCS) technologies could reduce these emissions and preliminary analysis of regional CO₂ storage capacity in locations where such facilities might be sited within the U.S. indicates that there appears to be sufficient storage capacity, primarily in deep saline formations, to accommodate the CO₂ from these industries. Nevertheless, even assuming wide-scale availability of cost-effective CO₂ capture and geologic storage resources, the emergence of a domestic U.S. oil shale or coal-to-liquids (CTL) industry would be responsible for significant increases in CO₂ emissions to the atmosphere. The authors present modeling results of two future hypothetical climate policy scenarios that indicate that the oil shale production facilities required to produce 3 MMB/d from the Eocene Green River Formation of the western U.S. using an in situ retorting process would result in net emissions to the atmosphere of between 3000 and 7000 MtCO₂, in addition to storing potentially 900–5000 MtCO₂ in regional deep geologic formations via CCS in the period up to 2050. A similarly sized, but geographically more dispersed domestic CTL industry could result in 4000–5000 MtCO₂ emitted to the atmosphere in addition to potentially 21,000–22,000 MtCO₂ stored in regional deep geologic formations over the same period. While this analysis shows that there is likely adequate CO₂ storage capacity in the regions where these technologies are likely to deploy, the reliance by these industries on large-scale CCS could result in an accelerated rate of utilization of the nation's CO₂ storage resource, leaving less high-quality storage capacity for other carbon-producing industries including electric power generation.     

Training carbon management engineers: Removing a major hurdle for geologic CO2 storage by increasing educational capacity

Implementing geologic storage of CO₂ at a material scale (ca. 1 Gt C/year) will require an industry comparable in size to the current oil and gas industry and a workforce trained in subsurface engineering. Since the same technologies that apply to hydrocarbon production apply to the subsurface storage of CO₂, petroleum engineering (PE) graduates will be valuable candidates to work in the carbon storage industry. We expect however that the demand for PEs from the oil and gas industry will increase, and that already strained educational capacity will not be sufficient to supply both industries. Thus we advocate building new targeted educational infrastructure. We present a model curriculum based on an existing accredited multidisciplinary degree program. This program combines the fundamentals of petroleum engineering with the subsurface architecture emphasis of geology and the environmental perspective of hydrogeology. We indicate key elements of this program that could be integrated with other, more traditional undergraduate engineering majors that also deal with the subsurface.     

Intermediate storage of carbon dioxide in geological formations: A technical perspective

Enhanced oil recovery (EOR) through CO₂ flooding has been practiced on a commercial basis for the last 35 years and continues today at several sites, currently injecting in total over 30 million tons of CO₂ annually. This practice is currently exclusively for economic gain, but can potentially contribute to the reduction of emissions of greenhouse gases provided it is implemented on a large scale. Optimal operations in distributing CO₂ to CO₂-EOR or enhanced gas recovery (EGR) projects (referred to here collectively as CO₂-EHR) on a large scale and long time span imply that intermediate storage of CO₂ in geological formations may be a key component. Intermediate storage is defined as the storage of CO₂ in geological media for a limited time span such that the CO₂ can be sufficiently reproduced for later use in CO₂-EHR. This paper investigates the technical aspects, key individual parameters and possibilities of intermediate storage of CO₂ in geological formations aiming at large scale implementation of carbon dioxide capture and storage (CCS) for deep emission reduction. The main parameters are thus the depth of injection and density, CO₂ flow and transport processes, storage mechanisms, reservoir heterogeneity, the presence of impurities, the type of the reservoirs and the duration of intermediate storage. Structural traps with no flow of formation water combined with proper injection planning such as gas-phase injection favour intermediate storage in deep saline aquifers. In depleted oil and gas fields, high permeability, homogeneous reservoirs with structural traps (e.g. anticlinal structures) are good candidates for intermediate CO₂ storage. Intuitively, depleted natural gas reservoirs can be potential candidates for intermediate storage of carbon dioxide due to similarity in storage characteristics.     

The value of post-combustion carbon dioxide capture and storage technologies in a world with uncertain greenhouse gas emissions constraints

By analyzing how the largest CO₂ emitting electricity-generating region in the United States, the East Central Area Reliability Coordination Agreement (ECAR), responds to hypothetical constraints on greenhouse gas emissions, the authors demonstrate that there is an enduring role for post-combustion CO₂ capture technologies. The utilization of pulverized coal generation with carbon dioxide capture and storage (PC + CCS) technologies is particularly significant in a world where there is uncertainty about the future evolution of climate policy and in particular uncertainty about the rate at which the climate policy will become more stringent. The paper's analysis shows that within this one large, heavily coal-dominated electricity-generating region, as much as 20–40 GW of PC + CCS could be operating before the middle of this century. Depending upon the state of PC + CCS technology development and the evolution of future climate policy, the analysis shows that these CCS systems could be mated to either pre-existing PC units or PC units that are currently under construction, announced and planned units, as well as PC units that could continue to be built for a number of decades even in the face of a climate policy. In nearly all the cases analyzed here, these PC + CCS generation units are in addition to a much larger deployment of CCS-enabled coal-fueled integrated gasification combined cycle (IGCC) power plants. The analysis presented here shows that the combined deployment of PC + CCS and IGCC + CCS units within this one region of the U.S. could result in the potential capture and storage of between 3.2 and 4.9 Gt of CO₂ before the middle of this century in the region's deep geologic storage formations.     

Simultaneous CO2 injection and water production to optimise aquifer storage capacity

The estimates for geological CO₂ storage capacity worldwide vary, but it is generally believed that the capacity in saline aquifers will be sufficient for the amounts of CO₂ that will need to be stored. The effort required to select and qualify a geological storage site for safe storage will, however, be significant and storage capacity may be a limited resource regionally. Both from a economic and resource management perspective it is therefore important that potential storage sites are exploited to their full potential.In static capacity estimates, where the maximum stored amount of CO₂ is given as a fraction of the formation pore volume, typically arrive at efficiency factors in the range of a few per cents. Recent work has shown that when the dynamic behaviour of the injected CO₂ is taken into account, the efficiency factor will be reduced because of the increase in pore pressure in the region around the injection well(s). The increase in pore pressure will propagate much further than the CO₂. The EU directive on geological CO₂ storage specifically addresses the restriction that will apply when different storage sites are interacting due to pressure communication. Consequently, the pore pressure increase at the boundary of the storage license area will be an important limiting factor for the amount of CO₂ that can be injected.One obvious method to control the pore pressure is to produce water from the aquifer at some distance from the CO₂ injection wells. This paper discusses results from simulations of CO₂ injection in two aquifers on the Norwegian Continental Shelf; the Johansen aquifer and the southern part of the Utsira aquifer. These aquifers are candidates for injection of CO₂ shipped out via pipeline from the Norwegian West Coast. The injected amounts of CO₂ over a period of 50 years are 0.518 Gtonne for the Johansen aquifer and 1.04 Gtonne for the Utsira aquifer.Several design options for the injection operations are investigated: Injection of CO₂ without water production; injection into several wells to distribute the injected fluids and reduce the local pressure increase around each injection well; and injection with simultaneous production of water from one or more wells. The boundaries of the aquifer formations are assumed closed in all simulations. The possible consequences of other types of boundary conditions (semi-closed or open) are briefly discussed.     

CO2 capture from power plants: Part I. A parametric study of the technical performance based on monoethanolamine

Capture and storage of CO₂ from fossil fuel fired power plants is drawing increasing interest as a potential method for the control of greenhouse gas emissions. An optimization and technical parameter study for a CO₂ capture process from flue gas of a 600 MWe bituminous coal fired power plant, based on absorption/desorption process with MEA solutions, using ASPEN Plus with the RADFRAC subroutine, was performed. This optimization aimed to reduce the energy requirement for solvent regeneration, by investigating the effects of CO₂ removal percentage, MEA concentration, lean solvent loading, stripper operating pressure and lean solvent temperature.Major energy savings can be realized by optimizing the lean solvent loading, the amine solvent concentration as well as the stripper operating pressure. A minimum thermal energy requirement was found at a lean MEA loading of 0.3, using a 40 wt.% MEA solution and a stripper operating pressure of 210 kPa, resulting in a thermal energy requirement of 3.0 GJ/ton CO₂, which is 23% lower than the base case of 3.9 GJ/ton CO₂. Although the solvent process conditions might not be realisable for MEA due to constraints imposed by corrosion and solvent degradation, the results show that a parametric study will point towards possibilities for process optimisation.     

Seismic detection of CO2 leakage along monitoring wellbores

A pilot carbon dioxide (CO₂) sequestration experiment was carried out in the Michigan Basin in which ～10,000 tonnes of supercritical CO₂ was injected into the Bass Island Dolomite (BILD) at 1050 m depth. A passive seismic monitoring (PSM) network was operated before, during and after the ～17-day injection period. The seismic monitoring network consisted of two arrays of eight, three-component sensors, deployed in two monitoring wells at only a few hundred meters from the injection point. 225 microseismic events were detected by the arrays. Of these, only one event was clearly an injection-induced microearthquake. It occurred during injection, approximately 100 m above the BILD formation. No events, down to the magnitude ?3 detection limit, occurred within the BILD formation during the injection. The observed seismic waveforms associated with the other 224 events were quite unusual in that they appear to contain dominantly compressional (P) but no (or extremely weak) shear (S) waves, indicating that they are not associated with shear slip on faults. The microseismic events were unusual in two other ways. First, almost all of the events occurred prior to the start of injection into the BILD formation. Second, hypocenters of the 94 locatable events cluster around the wells where the sensor arrays were deployed, not the injection well. While the temporal evolution of these events shows no correlation with the BILD injection, they do correlate with CO₂ injection for enhanced oil recovery (EOR) into the 1670 m deep Coral Reef formation that had been going on for ～2.5 years prior to the pilot injection experiment into the BILD formation. We conclude that the unusual microseismic events reflect degassing processes associated with leakage up and around the monitoring wells from the EOR-related CO₂ injection into the Coral Reef formation, ～700 m below the depth of the monitoring arrays. This conclusion is also supported by the observation that as soon as injection into the Coral Reef formation resumed at the conclusion of the BILD demonstration experiment, seismic events (essentially identical to the events associated with the Coral Reef injection prior to the BILD experiment) again started to occur close to a monitoring arrays. Taken together, these observations point to vertical migration around the casings of the monitoring wellbores. Detection of these unusual microseismic events was somewhat fortuitous in that the arrays were deployed at the depth where the CO₂ undergoes a strong volume increase during transition from a supercritical state to a gas. Given the large number of pre-existing wellbores that exist in depleted oil and gas reservoirs that might be considered for CO₂ sequestration projects, passive seismic monitoring systems could be deployed at appropriate depths to systematically detect and monitor leakage along them.     

CO2 capture from hot stove gas in steel making process

The capture of CO₂ from a hot stove gas in steel making process containing 30 vol% CO₂ by chemical absorption in a rotating packed bed (RPB) was studied. The RPB had an inner diameter of 7.6 cm, an outer diameter of 16 cm, and a height of 2 cm. The aqueous solutions containing 30 wt% of single and mixed monoethanolamine (MEA), 2-(2-aminoethylamino)ethanol (AEEA), and piperazine (PZ) were used. The CO₂ capture efficiency was found to increase with increasing temperature in a range of 303–333 K. It was also found to be more dependent on gas and liquid flow rates but less dependent on rotating speed when the speed was higher than 700 rpm. The obtained results indicated that the mixed alkanolamine solutions containing PZ were more effective than the single alkanolamine solutions. This was attributed to the highest reaction rate of PZ with CO₂. A higher portion of PZ in the mixture was more favorable to CO₂ capture. The highest gas flow rates allowed to achieve a desired CO₂ capture efficiency and the correspondent height of transfer unit (HTU) were determined at different aqueous solution flow rates. Because all the 30 wt% single and mixed alkanolamine solutions could result in a HTU less than 5.0 cm at a liquid flow rate of 100 mL/min, chemical absorption in a RPB instead of a packed bed adsorber is therefore suggested to capture CO₂ from the flue gases in steel making processes.     

Maintaining a neutral water balance in a 450 MWe NGCC-CCS power system with post-combustion carbon dioxide capture aimed at offshore operation

A post-combustion CO₂ capture process intended for offshore operations has been designed and optimised for integration with a natural gas-fired power plant on board a floating structure developed by the Norway-based company Sevan Marine ASA—designated Sevan GTW (gas-to-wire). The concept is constrained by the structure of the floater carrying a SIEMENS modular power system rated at 450 MW_e, with a capture rate of 90% and CO₂ compression (1.47 Mtpa) for pipeline pressure at 12 MPa. A net efficiency of 45% (based on a lower heating value) is estimated for the system with CO₂ capture, thus suggesting that the post-combustion CO₂ capture system is accountable for a fuel penalty of nine percentage points.The rationale behind the technology selection is the urgency of replacing the dispersed aero-derivative gas turbines which power the offshore oil and gas production units in Norwegian waters with near-zero emission power.As (inherently) fresh water usually constitutes a limiting factor in sea operations, efforts are made to obtain a neutral water balance to obtain an optimal design. This is primarily achieved by controlling the cleaned flue gas temperature at the top of the absorber column.     

A comparison of on-site nutrient and energy recycling technologies in algal oil production

Research on biofuel production pathways from algae continues because among other potential advantages they avoid key consequential effects of terrestrial oil crops, such as competition for cropland. However, the economics, energetic balance, and climate change emissions from algal biofuels pathways do not always show great potential, due in part to high fertilizer demand. Nutrient recycling from algal biomass residue is likely to be essential for reducing the environmental impacts and cost associated with algae-derived fuels. After a review of available technologies, anaerobic digestion (AD) and hydrothermal liquefaction (HTL) were selected and compared on their nutrient recycling and energy recovery potential for lipid-extracted algal biomass using the microalgae strain Scenedesmus dimorphus. For 1 kg (dry weight) of algae cultivated in an open raceway pond, 40.7 g N and 3.8 g P can be recycled through AD, while 26.0 g N and 6.8 g P can be recycled through HTL. In terms of energy production, 2.49 MJ heat and 2.61 MJ electricity are generated from AD biogas combustion to meet production system demands, while 3.30 MJ heat and 0.95 MJ electricity from HTL products are generated and used within the production system.Assuming recycled nutrient products from AD or HTL technologies displace demand for synthetic fertilizers, and energy products displace natural gas and electricity, the life cycle greenhouse gas reduction achieved by adding AD to the simulated algal oil production system is between 622 and 808 g carbon dioxide equivalent (CO₂e)/kg biomass depending on substitution assumptions, while the life cycle GHG reduction achieved by HTL is between 513 and 535 g CO₂e/kg biomass depending on substitution assumptions. Based on the effectiveness of nutrient recycling and energy recovery, as well as technology maturity, AD appears to perform better than HTL as a nutrient and energy recycling technology in algae oil production systems.     

Large-scale impact of CO2 storage in deep saline aquifers: A sensitivity study on pressure response in stratified systems

Large volumes of CO₂ captured from carbon emitters (such as coal-fired power plants) may be stored in deep saline aquifers as a means of mitigating climate change. Storing these additional fluids may cause pressure changes and displacement of native brines, affecting subsurface volumes that can be significantly larger than the CO₂ plume itself. This study aimed at determining the three-dimensional region of influence during/after injection of CO₂ and evaluating the possible implications for shallow groundwater resources, with particular focus on the effects of interlayer communication through low-permeability seals. To address these issues quantitatively, we conducted numerical simulations that provide a basic understanding of the large-scale flow and pressure conditions in response to industrial-scale CO₂ injection into a laterally open saline aquifer. The model domain included an idealized multilayered groundwater system, with a sequence of aquifers and aquitards (sealing units) extending from the deep saline storage formation to the uppermost freshwater aquifer. Both the local CO₂-brine flow around the single injection site and the single-phase water flow (with salinity changes) in the region away from the CO₂ plume were simulated. Our simulation results indicate considerable pressure buildup in the storage formation more than 100 km away from the injection zone, whereas the lateral distance migration of brine is rather small. In the vertical direction, the pressure perturbation from CO₂ storage may reach shallow groundwater resources only if the deep storage formation communicates with the shallow aquifers through sealing units of relatively high permeabilities (higher than 10^?18 m²). Vertical brine migration through a sequence of layers into shallow groundwater bodies is extremely unlikely. Overall, large-scale pressure changes appear to be of more concern to groundwater resources than changes in water quality caused by the migration of displaced saline water.     

Capture of carbon dioxide from flue or fuel gas mixtures by clathrate crystallization in a silica gel column

A column of silica gel was employed to contact water with flue gas (CO₂/N₂) mixture to assess if CO₂ can be separated by hydrate crystallization. Three different silica gels were used. One with a pore size of 30 nm (particle size 40–75 μm) and two with a pore size of 100 nm and particle sizes of 40–75 and 75–200 μm respectively. The observed trends indicate that larger pores and particle size increase the gas consumption, CO₂ recovery, separation factor and water conversion to hydrate. Thus, the gel (gel #3) with the larger particle size and larger pore size was chosen to carry out experiments with concentrated CO₂ mixtures and for experiments in the presence of tetrahydrofuran (THF), which itself is a hydrate forming substance. Addition of THF reduces the operating pressure in the crystallizer but it also reduces the gas uptake. Gel #3 was also used in experiments with a fuel gas (CO₂/H₂) mixture in order to recover CO₂ and H₂. It was found that the gel column performs as well as a stirred reactor in separating the gas components from both flue gas and fuel gas mixtures. However, the crystallization rate and hydrate yield are considerably enhanced in the former. Finally the need for stirring is eliminated with the gel column which is enormously beneficial economically.     

Experimental investigation of wellbore integrity and CO2–brine flow along the casing–cement microannulus

Wellbore integrity is one of the key performance criteria in the geological storage of CO₂. It is significant in any proposed storage site but may be critical to the suitability of depleted oil and gas reservoirs that may have 10’s to 1000’s of abandoned wells. Much previous work has focused on Portland cement which is the primary material used to seal wellbore systems. This work has emphasized the potential dissolution of Portland cement. However, an increasing number of field studies (e.g., Carey et al., 2007), experimental studies (e.g., Kutchko et al., 2006) and theoretical considerations indicate that the most significant leakage mechanism is likely to be flow of CO₂ along the casing–cement microannulus, cement–cement fractures, or the cement–caprock interface.In this study, we investigate the casing–cement microannulus through core-flood experiments. The experiments were conducted on a synthetic wellbore system consisting of a 5-cm diameter sample of cement that was cured with an embedded rectangular length of steel casing that had grooves to accommodate fluid flow. The experiments were conducted at 40 $°$ C and 14 MPa pore pressure for 394 h. During the experiment, 6.2 l of a 50:50 mixture of supercritical CO₂ and 30,000 ppm NaCl-rich brine flowed through 10-cm of limestone before flowing through the 6-cm length cement–casing wellbore system. Approximately 59,000 pore volumes of fluid moved through the casing–cement grooves. Scanning electron microscopy revealed that the CO₂–brine mixture impacted both the casing and the cement. The Portland cement was carbonated to depths of 50–250 $\mu$m by a diffusion-dominated process. There was very little evidence for mass loss or erosion of the Portland cement. By contrast, the steel casing reacted to form abundant precipitates of mixed calcium and iron carbonate that lined the channels and in one case almost completely filled a channel. The depth of steel corroded was estimated at 25– $30\mu$m and was similar in value to results obtained with a simplified corrosion model.The experimental results were applied to field observations of carbonated wellbore cement by Carey et al. (2007) and Crow et al. (2009) to show that carbonation of the field samples was not accompanied by significant CO₂–brine flow at the casing–cement interface. The sensitivity of standard-grade steel casing to corrosion suggests that relatively straight-forward wireline logging of external casing corrosion could be used as a useful indicator of flow behind casing. These experiments also reinforce other studies that indicate rates of Portland cement deterioration are slow, even in the high-flux CO₂–brine experiments reported here.