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Laboratory Investigations in Support of Carbon Dioxide-in-Water Emulsions Stabilized by Fine Particles for Ocean and Geologic Sequestration of Carbon Dioxide

Description: Since the submission of our last Semi-annual Report, dated September 2006, the research objectives of this Co-operative Agreement shifted toward geologic sequestration of carbon dioxide. In the period September 2006-February 2007, experiments were conducted in a High-Pressure Batch Reactor (HPBR) for creating emulsions of liquid carbon dioxide (/CO{sub 2})-in-water stabilized by fine particles for geologic sequestration of CO{sub 2}. Also, emulsions were created in water of a binary mixture of liquid carbon dioxide and liquid hydrogen sulfide (/H{sub 2}S), called Acid Gas (AG). This leads to the possibility of safe disposal of AG in deep geologic formations, such as saline aquifers. The stabilizing particles included pulverized limestone (CaCO{sub 3}), unprocessed flyash, collected by an electrostatic precipitator at a local coal-fired power plant, and pulverized siderite (FeCO{sub 3}). Particle size ranged from submicron to a few micrometers. The first important finding is that /CO{sub 2} and /H{sub 2}S freely mix as a binary liquid without phase separation. The next finding is that the mixture of /CO{sub 2} and /H{sub 2}S can be emulsified in water using fine particles as emulsifying agents. Such emulsions are stable over prolonged periods, so it should not be a problem to inject an emulsion into subterranean formations. The advantage of injecting an emulsion into subterranean formations is that it is denser than the pure liquid, therefore it is likely to disperse in the bottom of the geologic formation, rather than buoying upward (called fingering). In such a fashion, the risk of the liquids escaping from the formation, and possibly re-emerging into the atmosphere, is minimized. This is especially important for H{sub 2}S, because it is a highly toxic gas. Furthermore, the emulsion may interact with the surrounding minerals, causing mineral trapping. This may lead to longer sequestration periods than injecting the pure liquids alone.
Date: January 8, 2007
Creator: Golomb, Dan; Ryan, David & Barry, Eugene
Partner: UNT Libraries Government Documents Department

Laboratory Investigations in Support of Carbon Dioxide-in-Water Emulsions Stabilized by Fine Particles for Ocean and Geologic Sequestration of Carbon Dioxide

Description: This semi-annual progress report includes our latest research on deep ocean sequestration of CO{sub 2}-in-Water (C/W) emulsions stabilized by pulverized limestone (CaCO{sub 3}). We describe a practical system that could be employed for the release of a dense C/W emulsion. The heart of the system is a Kenics-type static mixer. The testing and evaluation of a static mixer in the NETL High-Pressure Water Tunnel Facility was described in the previous semi-annual report. The release system could be deployed from a floating platform over the open ocean, or at the end of an off-shore pipe laying on the continental slope. Because the emulsion is much denser than ambient seawater, modeling shows that upon release the plume will sink much deeper from the injection point, increasing the sequestration time for CO{sub 2}. When released in the open ocean, a plume containing the output of a 500 MW{sub el} coal-fired power plant will typically sink hundreds of meters below the injection point. When released from a pipe on the continental shelf, the plume will sink about twice as much because of the limited entrainment of ambient seawater when the plume flows along the sloping seabed. Furthermore, the plume is slightly alkaline, not acidic. The disadvantage is that the creation of the emulsion requires significant amounts of pulverized limestone, on the order of 0.5-0.75 weight ratio of limestone to CO{sub 2}. While pulverized limestone with particle size appropriate for creating C/W emulsions can be purchased for $38 per ton, it is shown in this report that it may be more economic to purchase raw limestone from quarries and pulverize it in situ using grinding mills. In this case the major cost elements are the capital and operating costs of the grinding mills, resulting in a total cost of about $11 per ton of pulverized ...
Date: July 8, 2006
Creator: Golomb, Dan; Barry, Eugene & Ryan, David
Partner: UNT Libraries Government Documents Department

LABORATORY INVESTIGATIONS IN SUPPORT OF CARBON DIOXIDE-LIMESTONE SEQUESTRATION IN THE OCEAN

Description: In the second half of the second contractual year the construction of the High Pressure Flow Reactor (HPFR) was completed, tested, and satisfactory results have been obtained. The major component of the HPFR is a Kenics-type static mixer in which two fluids are thoroughly mixed. In our case the two fluids are liquid or supercritical CO{sub 2} and a slurry of pulverized limestone (CaCO{sub 3}) in pure or artificial seawater. The outflow from the static mixer is an emulsion consisting of CO{sub 2} droplets coated with a sheath of CaCO{sub 3} particles dispersed in water. The coated CO{sub 2} droplets are called globules, and the emulsion is called globulsion. By adjusting the proportions of the two fluids, carbon dioxide and water, the length and pressure drop across the static mixer, globules with a fairly uniform distribution of diameters can be obtained. By using different particle sizes of CaCO{sub 3}, globules can be obtained that are lighter or heavier than water, thus floating or sinking in a water column. The globulsion ensuing from the static mixer flows into a high pressure cell with windows, where the properties of the globules can be observed, such as their diameter and settling velocity. Using the Stokes' equation, the specific gravity of the globules can be determined. Also, a second generation High Pressure Batch Reactor (HPBR) was constructed. This reactor allows better mixing of the ingredients, more accurate temperature and pressure control, better illumination and video camera observations. In this reactor we established that CO{sub 2}-in-water globulsions can be formed stabilized by other particles than pulverized limestone. So far, we used flyash obtained from a local coal-fired power plant, and a pulverized magnesium silicate mineral, lizardite, Mg{sub 3}Si{sub 2}O{sub 5}(OH){sub 4}, obtained from DOE's Albany Research Laboratory. In the reporting period we conducted joint experiments ...
Date: September 1, 2004
Creator: Golomb, Dan; Barry, Eugene; Ryan, David; Lawton, Carl; Swett, Peter; Hannon, John et al.
Partner: UNT Libraries Government Documents Department

LABORATORY INVESTIGATIONS IN SUPPORT OF CARBON DIOXIDE-LIMESTONE SEQUESTRATION IN THE OCEAN

Description: This semi-annual progress reports includes further findings on CO{sub 2}-in-Water (C/W) emulsions stabilized by fine particles. In previous reports we described C/W emulsions using pulverized limestone (CaCO{sub 3}), flyash, and a pulverized magnesium silicate mineral, lizardite, Mg{sub 3}Si{sub 2}O{sub 5}(OH){sub 4}, which has a similar composition as the more abundant mineral, serpentine. All these materials formed stable emulsions consisting of droplets of liquid or supercritical CO{sub 2} coated with a sheath of particles dispersed in water. During this semi-annual period we experimented with pulverized beach sand (10-20 {micro}m particle diameter). Pulverized sand produced an emulsion similar to the previously used materials. The globules are heavier than water, thus they accumulate at the bottom of the water column. Energy Dispersive X-ray (EDX) analysis revealed that the sand particles consisted mainly of SiO{sub 2}. Sand is one of the most abundant materials on earth, so the economic and energy penalties of using it for ocean sequestration consist mainly of the cost of transporting the sand to the user, the capital and operating costs of the pulverizer, and the energy expenditure for mining, shipping and grinding the sand. Most likely, sand powder would be innocuous to marine organisms if released together with CO{sub 2} in the deep ocean. We examined the effects of methanol (MeOH) and monoethanolamine (MEA) on emulsion formation. These solvents are currently used for pre- and post-combustion capture of CO{sub 2}. A fraction of the solvents may be captured together with CO{sub 2}. A volume fraction of 5% of these solvents in a mix of CO{sub 2}/CaCO{sub 3}/H{sub 2}O had no apparent effect on emulsion formation. Previously we have shown that a 3.5% by weight of common salt (NaCl) in water, simulating seawater, also had no appreciable effect on emulsion formation. We investigated the formation of inverted emulsions, where water ...
Date: April 1, 2005
Creator: Golomb, Dan; Barry, Eugene; Ryan, David; Lawton, Carl; Swett, Peter; Duan, Huishan et al.
Partner: UNT Libraries Government Documents Department

Laboratory Investigations in Support of Carbon Dioxide-Limestone Sequestration in the Ocean

Description: This semi-annual progress reports includes further findings on CO{sub 2}-in-Water emulsions stabilized by fine particles of limestone (CaCO{sub 3}). Specifically, here we report on the tests performed in the DOE National Energy Technology Laboratory High Pressure Water Tunnel Facility (HPWTF) using a Kenics-type static mixer for the formation of a CO{sub 2}-H{sub 2}O emulsion stabilized by fine particles of CaCO{sub 3}. The tested static mixer has an ID of 0.5 cm, length 23.5 cm, number of baffles 27. Under pressure, a slurry of CaCO{sub 3} particles (mean particle size 6 {micro}m) in reverse osmosis (RO) water and liquid CO{sub 2} were co-injected into the mixer. From the mixer, the resulting emulsion flowed into the HPWTF, which was filled with RO water kept at 6.8 MPa pressure and 4, 8 or 12 C. The emulsion plume was photographed by three video cameras through spy windows mounted on the wall of the HPWTF. The mixer produced an emulsion consisting of tiny CO{sub 2} droplets sheathed with a layer of CaCO{sub 3} particles dispersed in water. The sheathed droplets are called globules. The globules diameter was measured to be in the 300-500 {micro}m range. The globules were sinking in the HPWTF, indicating that they are heavier than the ambient water. The tests in the HPWTF confirmed that the Kenics-type static mixer is an efficient device for forming a CO{sub 2}-H{sub 2}O emulsion stabilized by fine particles of CaCO{sub 3}. The static mixer may prove to be a practical device for sequestering large quantities of CO{sub 2} in the deep ocean in the form of a CO{sub 2}-H{sub 2}O-CaCO{sub 3} emulsion. The static mixer can be mounted at the end of pipelines feeding the mixer. The static mixer has no moving parts. The pressure drop across the mixer that is necessary to sustain good ...
Date: April 1, 2006
Creator: Golomb, Dan; Barry, Eugene; Ryan, David; Pennell, Stephen; Swett, Peter; Duan, Huishan et al.
Partner: UNT Libraries Government Documents Department

Laboratory Investigations in Support of Carbon Dioxide-Limestone Sequestration in the Ocean

Description: This semi-annual progress reports includes further findings on CO{sub 2}-in-Water (C/W) emulsions stabilized by fine particles. In previous semi-annual reports we described the formation of stable C/W emulsions using pulverized limestone (CaCO{sub 3}), flyash, beach sand, shale and lizardite, a rock rich in magnesium silicate. For the creation of these emulsions we used a High-Pressure Batch Reactor (HPBR) equipped with view windows for illumination and video camera recording. For deep ocean sequestration, a C/W emulsion using pulverized limestone may be the most suitable. (a) Limestone (mainly CaCO{sub 3}) is cheap and plentiful; (b) limestone is innocuous for marine organisms (in fact, it is the natural ingredient of shells and corals); (c) it buffers the carbonic acid that forms when CO{sub 2} dissolves in water. For large-scale sequestration of a CO{sub 2}/H{sub 2}O/CaCO{sub 3} emulsion a device is needed that mixes the ingredients, liquid carbon dioxide, seawater, and a slurry of pulverized limestone in seawater continuously, rather than incrementally as in a batch reactor. A practical mixing device is a Kenics-type static mixer. The static mixer has no moving parts, and the shear force for mixing is provided by the hydrostatic pressure of liquid CO{sub 2} and CaCO{sub 3} slurry in the delivery pipes from the shore to the disposal depth. This semi-annual progress report is dedicated to the description of the static mixer and the results that have been obtained using a bench-scale static mixer for the continuous formation of a CO{sub 2}/H{sub 2}O/CaCO{sub 3} emulsion. The static mixer has an ID of 0.63 cm, length 23.5 cm, number of baffles 27. Under pressure, a slurry of CaCO{sub 3} in artificial seawater (3.5% by weight NaCl) and liquid CO{sub 2} are co-injected into the mixer. From the mixer, the resulting emulsion flows into a Jerguson cell with two oblong windows ...
Date: November 1, 2005
Creator: Golomb, Dan; Barry, Eugene; Ryan, David; Lawton, Carl; Pennell, Stephen; Swett, Peter et al.
Partner: UNT Libraries Government Documents Department

Laboratory Investigations in Support of Dioxide-Limestone Sequestration in the Ocean

Description: Research under this Project has proven that liquid carbon dioxide can be emulsified in water by using very fine particles as emulsion stabilizers. Hydrophilic particles stabilize a CO{sub 2}-in-H{sub 2}O (C/W) emulsion; hydrophobic particles stabilize a H{sub 2}O-in-CO{sub 2} (W/C) emulsion. The C/W emulsion consists of tiny CO{sub 2} droplets coated with hydrophilic particles dispersed in water. The W/C emulsion consists of tiny H{sub 2}O droplets coated with hydrophobic particles dispersed in liquid carbon dioxide. The coated droplets are called globules. The emulsions could be used for deep ocean sequestration of CO{sub 2}. Liquid CO{sub 2} is sparsely soluble in water, and is less dense than seawater. If neat, liquid CO{sub 2} were injected in the deep ocean, it is likely that the dispersed CO{sub 2} droplets would buoy upward and flash into vapor before the droplets dissolve in seawater. The resulting vapor bubbles would re-emerge into the atmosphere. On the other hand, the emulsion is denser than seawater, hence the emulsion plume would sink toward greater depth from the injection point. For ocean sequestration a C/W emulsion appears to be most practical using limestone (CaCO{sub 3}) particles of a few to ten ?m diameter as stabilizing agents. A mix of one volume of liquid CO{sub 2} with two volumes of H{sub 2}O, plus 0.5 weight of pulverized limestone per weight of liquid CO{sub 2} forms a stable emulsion with density 1087 kg m{sup -3}. Ambient seawater at 500 m depth has a density of approximately 1026 kg m{sup -3}, so the emulsion plume would sink by gravity while entraining ambient seawater till density equilibrium is reached. Limestone is abundant world-wide, and is relatively cheap. Furthermore, upon disintegration of the emulsion the CaCO{sub 3} particles would partially buffer the carbonic acid that forms when CO{sub 2} dissolves in seawater, alleviating ...
Date: September 30, 2008
Creator: Golomb, Dan; Barry, Eugene; Ryan, David; Pennell, Stephen; Lawton, Carl; Swett, Peter et al.
Partner: UNT Libraries Government Documents Department