Publications Database - List of capture publications

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    June, 2005

Vol 1 Chapter 10: Creative Chemical Approaches for Carbon Dioxide Removal from Flue Gas

Dag Eimer, Merethe Sjøvoll, Nils Eldrup, Richard H. Heyn, Olav Juliussen, Malcolm McLarney and Ole Swang

Carbon dioxide capture costs need to be reduced more than marginally. This work was initiated because of the realisation that new and radically different ways of dealing with carbon dioxide capture from exhaust gas must be searched for in parallel with research on already established paths. Perceived limitations for improvements in these established paths is a driver for such research. Another is the sheer amount of exhaust gas that is thought to need treatment in the future. The target set for the present project was to produce ideas with potential for reducing carbon dioxide capture costs by at least 50% relative to a defined reference case.

Carbon Dioxide Capture for Storage in Deep Geologic Formations – Results from the CO₂ Capture Project Capture and Separation of Carbon Dioxide from Combustion Sources - Volume 1
Edited by: David C. Thomas, Senior Technical Advisor, Advanced Resources International Inc, USA

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    June, 2005

Vol 1 Chapter 11: Pre-Combustion Decarbonisation Technology Summary

Henrik Andersen

Abstract: The CO₂ Capture Project (CCP) was formed in late 2000 and after a review and evaluation phase began actual technical development work near the end of 2001. Most of the technology providers had only 2 years to complete their work. Even then, significant progress and advances in several key areas were made. New insights on adoption of existing technology in the CCP industrial scenarios were achieved. The key results from the pre-combustion technology development projects are:

• Four new advanced technologies were developed to “proof-of-concept” with significant advancement in efficiency, cost and CO₂ capture compared to the best available capture technology.
• The four technologies showed cost reduction potential in the range from 30 to 60%, with the Hydrogen Membrane Reformer demonstrating the highest potential.
• Three of the new advanced technologies were developed for different CCP scenarios. The designs were checked, integrated, and cost estimated by an independent contractor (Fluor) in order to assure design quality and consistency when comparing with the baseline technology, thus enhancing credibility of the conclusions.
• Significant advancements were made in hydrogen membrane materials covering a wide temperature range.
• Further development is needed to advance the most promising technologies, however, it is expected that new technologies can be developed and demonstrated in 2010–2015 with costs in the range of $15–40 MM.
• Pre-combustion technology can be developed to meet stringent requirements on NOx, CO, and SOx formation. The lowest NOx formation was predicted to be 5 ppm vol. from a combined cycle gas turbine. For open-cycle gas turbines, the NOx formation was reduced by 50%. CO and SOx formation were virtually zero.
• Pre-combustion technology can be designed as stand-alone facilities for both retrofit and new build applications giving a wide application range and benefits with respect to integration in existing complex facilities, e.g. refineries.
• Pre-combustion technology can be used for other applications, e.g. gas-to-liquids (GTL), ammonia, hydrogen and syngas production, thus increasing the economic potential of the technology and return of investment.
• Significant improvement in energy and CO₂ capture efficiency was obtained for several technologies, resulting in an efficiency penalty for combined cycle gas turbines of less than 5% with nearly 100% CO₂ capture.
• A 15% improvement of gas turbine heat rate can be obtained when switching from natural gas to hydrogenrich fuel, making the pre-combustion technology a strong candidate for the large numbers of open-cycle gas turbines in operation in the US.
• Demonstrated very low CO₂ avoided costs for the Canadian scenario—CO₂ capture from petroleum coke fired IGCC—approximately $10–15 per ton.
• Existing pre-combustion technology can be considered proven for a wide range of CO₂ capture applications including the CCP scenarios.

Carbon Dioxide Capture for Storage in Deep Geologic Formations – Results from the CO₂ Capture Project Capture and Separation of Carbon Dioxide from Combustion Sources - Volume 1
Edited by: David C. Thomas, Senior Technical Advisor, Advanced Resources International Inc, USA

(338 Kb)      View   Download

    June, 2005

Vol 1 Chapter 12: Generation of Hydrogen Fuels for a Thermal Power Plant with Integrated CO₂-Capture Using a CaO–CaCO3 Cycle

Julien Meyer, Rolf Jarle Aaberg and Bjørg Andresen

Abstract: A new integrated reforming reaction for hydrogen production is simulated. Hydrogen gas is produced from natural gas and water in a modified reforming reaction where CO₂ reacts with a metal oxide (MetO, e.g. CaO) to form a metal carbonate (MetCO3, e.g. CaCO3). The carbonate is decomposed thermally in a separate reaction and the metal oxide is recycled back to the reformer. This provides an efficient means of separation of the carbon dioxide from the reformer. The exothermic carbonation reaction provides most of the energy necessary to drive the hydrogen-producing reaction to completion. The CO₂ removal process has been designed and simulated to test the generation of hydrogen fuels for a thermal power plant. Although, the concept originally was intended for integration with processes with high-temperature waste heat, the thermodynamic analysis shows that the process can be used for hydrogen production for a combined cycle power plant and steam boilers as well.

Carbon Dioxide Capture for Storage in Deep Geologic Formations – Results from the CO₂ Capture Project Capture and Separation of Carbon Dioxide from Combustion Sources - Volume 1
Edited by: David C. Thomas, Senior Technical Advisor, Advanced Resources International Inc, USA

(702 Kb)      View   Download

    June, 2005

Vol 1 Chapter 15: Development of a Hydrogen Mixed Conducting Membrane Based CO₂ Capture Process

Bent Vigeland and Knut Ingvar Aasen

Abstract: The aim of this CCP sub-project has been to develop dense hydrogen mixed conducting ceramic membranes (HMCM) with sufficient H₂ transport rates and stability under normal methane steam reforming conditions, and further develop a techno economically viable precombustion de-carbonization (PCDC) power generating process applying said materials. In the novel natural gas to hydrogen process a two step membrane reformer system replaces the traditionally hydrogen production train. The membrane reformer concept combines steam methane reforming and HMCM. Hydrogen generated in the steam methane reformer sections is transported through the membrane and is in a first step reacted with air extracted from a gas turbine to generate a nitrogen and steam containing sweep gas. This sweep gas is used to recover most of the hydrogen in a membrane reformer step two generating a high pressure (15– 20 bar) hydrogen fuel containing about 40% H₂, 40% N₂ and 20% H₂O. The hydrogen fuel mixture is then combusted with air in the gas turbine. The low hydrogen concentration in the fuel is a major advantage since this will depress formation of nitric oxides in the combustion chamber to 15 ppmv or below. The residual synthesis gas containing mainly CO₂, H₂O and CO is further converted to CO₂ and H₂O in a residual gas oxidation section. CO₂ can then be captured simply by condensation of the water vapor. A large number of candidate membrane materials have been synthesized and characterized followed by hydrogen permeability measurements in atmospheric laboratory tests at both SINTEF and University of Oslo (UiO). Based on the measurements and theoretical evaluations, a main candidate materials system, was selected. Theoretical analyses indicate that the membranes will be stable above 700 8C under process conditions. Supported membrane tubes have been fabricated and tested by Hydro in a pressurized hydrogen flux test rig under relevant process conditions. The measured H₂ flux in the test rig compares favorably with model predictions. Based on cost estimate from Fluor the CCP CEM team did a cost analysis to evaluate the potential for this technology compared with, e.g. theNorwegian baseline technology. This indicates that the hydrogenmembrane reformer process has the potential to reduce the cost of CO₂ capture in a CCGT power plant with at least 50%.

Carbon Dioxide Capture for Storage in Deep Geologic Formations – Results from the CO₂ Capture Project Capture and Separation of Carbon Dioxide from Combustion Sources - Volume 1
Edited by: David C. Thomas, Senior Technical Advisor, Advanced Resources International Inc, USA

(472 Kb)      View   Download

    June, 2005

Vol 1 Chapter 19: Grace: Development of Pd-Zeolite Composite Membranes for Hydrogen Production by Membrane Reactor

M. Mene´ndez, M.P. Pina, M.A. Urbiztondo, L. Casado, M. Boutonnet, S. Rojas and S. Nassos

Abstract: Pd–zeolite composite membranes have been prepared over the external surface of macroporous a-alumna tubular supports by secondary growth of zeolite layers followed by Pd modification. Pd nanoparticles (few nanometers in size) filtration and/or impregnation þ in situ reduction of an organic Pd precursor have been explored as deposition techniques devoted to enhance the H₂ separation performance of the non-defect free A-type zeolite membranes. The Pd deposition aims toward the partial blockage of the non-selective intercrystalline pathways, which may account for a significant fraction of the total permeation flux. The Pd–zeolite composite substrates have been characterized by XRD, SEM and EDX. The study of the permeation properties of these substrates for single (N₂) and binary mixtures (H₂–CO₂) before and after Pd modification, reveals some improvements in terms of H₂ separation performance. The impregnation þ in situ reduction of palladium acetylacetonate solution (Pd(acac)2) carried out over KA zeolite membranes previously seeded with Pd nanoparticles appears as the most adequate among the tested methods. Separation factors for H₂-CO₂ binary mixtures up to 145 have been achieved, although further optimization is required to improve the H₂ permeation fluxes (around 1028 mol H2/m2 s Pa).

Carbon Dioxide Capture for Storage in Deep Geologic Formations – Results from the CO₂ Capture Project Capture and Separation of Carbon Dioxide from Combustion Sources - Volume 1
Edited by: David C. Thomas, Senior Technical Advisor, Advanced Resources International Inc, USA

(686 Kb)      View   Download

    June, 2005

Vol 1 Chapter 20: Grace: Development of Silica Membranes for Gas Separation at Higher Temperatures

Henk Kruidhof, Mieke W.J. Luiten, Nieck E. Benes and Henny J.M. Bouwmeester

Abstract: Using a polymeric gel solution route, tubular micro-porous silica membranes showing high hydrogen permeance and high gas selectivities have been prepared. Silica membranes have been coated on top of steam-stable g-Al2O3 intermediate membranes inside a high-quality tubular support. Tube ends were coated with glass giving a gastight changeover between support and membranes. Single dead-end gas permeance measurements performed at temperatures >300℃ and 4 bar pressure difference showed hydrogen fluxes >1.1026 mol m22 s21 Pa21 while H₂/CO₂ perm selectivity under these conditions was found to be 80-100. H₂/CO₂ selectivity increases up to 200 with decreasing pressure down to 1 bar. Membranes were shown to be thermally stable for at least 2000 h at temperatures between 200 and 400℃. Preliminary water-gas-shift experiments were performed at temperatures above 250℃ and showed higher than equilibrium CO conversion.

Carbon Dioxide Capture for Storage in Deep Geologic Formations - Results from the CO₂ Capture Project Capture and Separation of Carbon Dioxide from Combustion Sources - Volume 1
Edited by: David C. Thomas, Senior Technical Advisor, Advanced Resources International Inc, USA

(205 Kb)      View   Download

    June, 2005

Vol 1 Chapter 21: Grace: Development of Supported Palladium Alloy Membranes

Hallgeir Klette, Henrik Raeder, Yngve Larring and Rune Bredesen

Abstract: The present study reports development and testing of flat and tubular supported palladium alloy membrane modules at SINTEF. Membranes with thickness in the range of 1 mm have been prepared by a two-stage magnetron sputter process using a single crystal silicon wafer as intermediate support and a wire mesh or porous material as final support. Testing of the hydrogen flux through the tubular membranes at 300℃ has shown that permeance values of about 3 x 1026 mol/(m₂ s Pa) can be attained. For a flat membrane, peak permeance values of about 6.8 x 1026 mol/(m₂ s Pa) was attained at 300℃. The membranes are able to separate hydrogen gas from nitrogen gas with 100% selectivity within the detection limits of the equipment. Tubular membrane supports that have been reinforced by a steel insert have been tested up to 14 bar transmembrane pressure. Although the selectivity drops at high pressure, the tests show that the membrane film does not disintegrate at high pressure even at 300℃. Some of the membranes described have been shipped to ITM-CNR in Italy for catalytic reactor testing as a part of the GRACE program.

Carbon Dioxide Capture for Storage in Deep Geologic Formations - Results from the CO₂ Capture Project Capture and Separation of Carbon Dioxide from Combustion Sources - Volume 1
Edited by: David C. Thomas, Senior Technical Advisor, Advanced Resources International Inc, USA

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    June, 2005

Vol 1 Chapter 22: Grace: Experimental Evaluation of Hydrogen Production by Membrane Reaction

Giuseppe Barbieri and Paola Bernardo

Abstract: Water gas shift reaction, widely used for upgrading H₂ containing streams, was analyzed in a membrane reactor (MR) using tubular Pd/Ag, silica and zeolite-A supported Pd membranes supplied by SINTEF (Norway), the University of Twente (The Netherlands) and the University of Zaragoza (Spain), respectively. MR experiments were carried out investigating the effect of temperature (200-338℃), reaction pressure (up to 550 kPa), partial pressure difference, sweep factor (0–7.5) and space velocity (472–2308 h21) on CO conversion and identifying rate determining step (kinetics or thermodynamics). H₂O/CO feed molar ratio was around the stoichiometric value. However, three different streams were fed to the MR: an equimolecular H₂O/CO stream; an “ATR exit þ Extra Steam” stream (20% CO, 20% H₂O, 10% CO₂, 50% H₂); and the outlet stream (partially converted) of a traditional reactor (TR) placed before the MR. TR experiments were also performed at a high SV (15,050 h21). A commercial, Haldor-Topsoe low temperature Cu–Zn oxides-based catalyst (LK821-2) was employed in both MR and TR. TR equilibrium conversion (TR-EC) was considered as reference because it is the upper limit for typical reactors. This constraint can be overcome by MR as a consequence of H₂ removal by means of a selective membrane. CO conversion measured in MR experiments, using the SINTEF and Twente University membranes, significantly overcome the thermodynamic limit for TR, depending also on the operating conditions, mainly temperature, pressure and feed composition. In some cases a total conversion was obtained. Also, the use of a TR before the MR allows the TR-EC to be overcome. The conversion showed by the Zaragoza University membranes slightly overcame the TR-EC. Other parameters such as reaction pressure or sweep factor have a positive effect on conversion. All the membranes were also characterized by means of permeation measurements with a pressure drop (for single gas) and concentration gradient (for gas mixture) methods. The experimental work provided valuable information about the different membrane types and gives useful experimental information on the membrane WGS reactor concept.

Carbon Dioxide Capture for Storage in Deep Geologic Formations – Results from the CO₂ Capture Project Capture and Separation of Carbon Dioxide from Combustion Sources - Volume 1
Edited by: David C. Thomas, Senior Technical Advisor, Advanced Resources International Inc, USA

(684 Kb)      View   Download

    June, 2005

Vol 1 Chapter 23: Grace: Pre-Combustion De-Carbonisation Hydrogen Membrane Study

Peter Middleton, Paul Hurst and Graeme Walker

Abstract: This chapter details the GRangemouth Advanced CapturE (GRACE) project to develop new membrane technology to preferentially permeate hydrogen as part of a pre-combustion de-carbonisation process to capture CO₂. The project forms part of the wider CO₂₂ via either pre-combustion de-carbonisation, the use of oxygen-rich combustion systems or post-combustion CO₂ recovery. In addition to developing a new hydrogen membrane, the remit of the GRACE project includes applying the new technology to a specific scenario to evaluate installation costs and the amount of CO₂ emissions that could be avoided if the technology were to be implemented. In this study, the capture of 2 million tonnes/year of CO₂ from BP’s Grangemouth complex in Scotland has been selected as the “real-life” scenario. Previous study work completed by the GRACE project identified a Palladium/Silver metal membrane, developed by SINTEF, as the best membrane technology for hydrogen permeation. This study is based on the use of the SINTEF membrane coupled to conventional hydrogen production technology. The results of this study are that:

• the option of using conventional hydrogen production technology and the SINTEF hydrogen membrane to capture CO₂ and produce hydrogen suitable for combustion is technically feasible;
• a SINTEF membrane module design has been developed;
• the fabrication cost of each membrane module is estimated to be $3.12 million;
• the total cost to capture 2 million tonnes of CO2 from the Grangemouth complex using pre-combustion de-carbonisation technology that incorporates the SINTEF membrane is estimated to be $251 million;
• this cost represents the lowest cost of any technology developed in the CCP programme, and represents a 28% cost reduction compared to the CCP baseline technology (post-combustion amine absorption);
• the selected process incorporates a high degree of self-sufficiency in terms of power demand.

However, a certain amount of electrical power will have to be imported from local sources. Assuming that conventional gas turbines are used to generate this shortfall, this reduces the amount of CO₂ emitted to atmosphere that is avoided by implementing the selected process scheme to about 112 million tonnes per year.

Carbon Dioxide Capture for Storage in Deep Geologic Formations – Results from the CO₂ Capture Project Capture and Separation of Carbon Dioxide from Combustion Sources - Volume 1
Edited by: David C. Thomas, Senior Technical Advisor, Advanced Resources International Inc, USA

(500 Kb)      View   Download

    June, 2005

Vol 1 Chapter 25: Oxyfuel Combustion for CO₂ Capture Technology Summary

Ivano Miracca, Knut Ingvar Aasen, Tom Brownscombe, Karl Gerdes and Mark Simmonds

The mission of the Oxyfuel Team within the CO₂ Capture Project (CCP) was to investigate the potential savings that combustion using pure oxygen with the hydrocarbon fuel (oxyfiring) may give in CO₂ capture, compared to conventional combustion with air. This involved monitoring and sponsoring research and development that may contribute to further reduction of CO₂ capture costs by the year 2010.

Carbon Dioxide Capture for Storage in Deep Geologic Formations – Results from the CO₂ Capture Project Capture and Separation of Carbon Dioxide from Combustion Sources - Volume 1
Edited by: David C. Thomas, Senior Technical Advisor, Advanced Resources International Inc, USA

(215 Kb)      View   Download

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