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Membrane Technologies for CO2 Separation A Journal of Membrane Science 359 (2010) 115–125 Contents lists available at ScienceDirect Journal of Membrane Science journal homepage: www.elsevier.com/locate/memsci Membrane technologies for CO2 separation A. Brunetti a, F. Scura a, G. Barbieri a,∗, E. Drioli a,b a National Research Council, Institute for Membrane Technology (ITM–CNR), Via Pietro BUCCI, c/o The University of Calabria, Cubo 17C, 87030 Rende CS, Italy1 b The University of Calabria, Department of Chemical Engineering and Materials, Cubo 44A, Via Pietro BUCCI, 87030 Rende CS, Italy article info abstract Article history: Today, all the existing coal-fired power plants present over the world emit about 2 billion tons of CO2 per Received 21 July 2009 year. The identification of a capture process which would fit the needs of target separation performances, Received in revised form 6 October 2009 together with a minimal energy penalty, is a key issue. Because of their fundamental engineering and Accepted 17 November 2009 economic advantages over competing separation technologies, membrane operations are, now, being Available online 26 November 2009 explored for CO2 capture from power plant emissions.The aim of this work is to provide people interested in the use of membranes in CO2 capture a general overview of the actual situation both in terms of Keywords: materials studies and global strategy to follow in the choice of the membrane gas separation with respect Membrane systems to the other separation technologies. Firstly, an overview on the polymeric membranes currently studied CO2 separation Flue gas for their use in CO2 capture and of their transport properties is proposed. Up to now, the most promising materials developed at laboratory scale show a selectivity of 100–160. Then, some important design parameters have been introduced in order to evaluate the advantages potentially offered by membrane systems with respect to the other separation technologies (adsorption and cryogenic). These parameters, based on specific considerations related to the output to be obtained as the product purity and the final destination of the product and to the feed conditions, might constitute guidelines for the choice of the separation technology.Considering as case study a flue gas stream containing 13% of CO2, some general maps of CO2 recovery versus permeate purity have been introduced. This might constitute a simple tool useful for an immediate and preliminary analysis on the membrane technology suitability for CO2 separation from flue gas, also on the light of specific considerations, strictly related to the output to be obtained. © 2009 Elsevier B.V. All rights reserved. 1. Introduction Currently, the main strategies for the carbon dioxide capture in a fossil fuel combustion process are [5]: Electricity production from fossil fuel based power plants will be challenged by growing concerns that anthropogenic emission • Oxy-fuel combustion: This option consists in performing the oxy- of green house gases such as carbon monoxide are contributing to gen/nitrogen separation on the oxidant stream, so that a CO2/H2O the global climate change. Today, all the existing coal-fired power mixture is produced through the combustion process. The advan- plants present over the world emit about 2 billion tons of CO2 tage of feeding an oxygen-enriched gas mixture (95% oxygen) per year. The regulation of the carbon dioxide emissions implies instead of air, is the achievement of a purge stream rich in CO2 the development of specific CO2 capture technologies that can and water with very low N2 content, therefore the CO2 can be be retrofitted to existing power plants as well designed into new easily recovered after the condensation of the water vapor. • plants with the goal to achieve 90% of CO2 capture limiting the Pre-combustion capture: This solution is developed in two phases: increase in cost of electricity to no more than 35% [1]. Therefore, the (i) the conversion of the fuel in a mixture of H2 and CO (syngas recovery of CO2 from large emission sources is a formidable tech- mixture) through, e.g., partial oxidation, steam reforming or auto- nological and scientific challenge which has received considerable thermal reforming of hydrocarbons, followed by water-gas shift; attention for several years [2–4]. In particular, the identification of a (ii) the separation of CO2 (at 30–35%) from the H2 that is then capture process which would fit the needs of target separation per- fed as clean fuel to turbines. In these cases, the CO2 separation formances, together with a minimal energy penalty, is a key issue. could happen at very high pressures (up to 80 bar of pressure difference) and high temperatures (300–700 ◦C). • Post-combustion capture: In this case, the CO2 is separated from ∗ the flue gas emitted after the combustion of fossil fuels (from a Corresponding author. Tel.: +39 0984 492029; fax: +39 0984 402103. E-mail address: [email protected] (G. Barbieri). standard gas turbine combined cycle, or a coal-fired steam power 1 www.itm.cnr.it. plant). CO2 separation is realized at relatively low temperature, 0376-7388/$ – see front matter © 2009 Elsevier B.V. All rights reserved. doi:10.1016/j.memsci.2009.11.040 116 A. Brunetti et al. / Journal of Membrane Science 359 (2010) 115–125 from a gaseous stream at atmospheric pressure and with low CO2 creating a pressure difference through the membrane will require concentration (ca. 5–25% if air is used during combustion). SO2, significant amounts of power, which will in turn lower the thermal NO2 and O2 may also be present in small amounts. This possibil- efficiency of the power plant. However, a modelling study of poly- ity is by far the most challenging since a diluted, low pressure, meric membranes in gas turbine power plants by Carapellucci and hot and wet CO2/N2 mixture has to be treated. Nevertheless, it Milazzo [10] shows more encouraging the use of membrane opera- also corresponds to the most widely applicable option in terms of tion in post-combustion capture, proposing a polymeric membrane industrial sectors (power, kiln and steel production for instance). system that can effectively separate out carbon dioxide from gas Moreover, it shows the essential advantage of being compatible flues. to a retrofit strategy (i.e. an already existing installation can be, The composition of flue gases varies greatly depending on the in principle, subject to this type of adaptation) [4]. fuel source, power plant and prior treatment. For instance, the flue gas coming out from a power plants and from a steel production Particularly referring to the post-combustion capture that will plant exhibits a significant difference in CO2 concentration. The use be the topic of this paper, the conventional separation processes of membrane technology for CO2 separation is, thus, also strictly for CO2 separation are: absorption (with ammines), adsorption related to the conditions of the stream to be treated. However, the (with porous solids with high adsorbing properties such as zeo- main role in its application on large scale might be assigned to the lite or active carbon) and cryogenic separation [6,7]. Amine-based membrane properties but also on the influence of the operating absorption with an aqueous monoethanolamine (MEA) solution is conditions on the whole process. the most common technology for post-combustion capture, since it In this work the potentialities and the applications of mem- is capable to achieve high level of CO2 capture (90% or more) from brane gas separation (GS) in the post-combustion capture will be flue gas due to fast kinetics and strong chemical reaction. How- explored, giving general guidelines on some design parameters to ever, its use is by far the best available technology owing to the take into account in the choice of a technology suitable for the CO2 fact that the ammines are corrosive and susceptible to degradation separation. by trace flue gas constituents (particularly sulphur oxides)). Fur- In this work the potentialities and the applications of mem- thermore, they require significant amount of energy (in the range brane gas separation (GS) in the post-combustion capture will be 4–6 MJ/kg recovered) related, in particular, to the significant explored, giving general guidelines on some design parameters to CO2 energy consumption in the regeneration step. This option requires take into account in the choice of a technology suitable for the CO2 large-scale equipment for the CO2 removal and chemicals handling. separation. DOE/NETL (Department of Energy – National Energy Technology The relation between membrane properties and main variables Laboratory) has estimated that MEA-based process for CO2 capture affecting the process performance will be analysed introducing will increase the cost of the electricity for a new power plant by some general maps of CO2 purity versus CO2 recovery. The most about 80–85%, also reducing the plant efficiency of about 30% [1]. important objective is to provide to people interested in the A relatively novel CO2 capture technology is based on cryogenic prospects for membranes in CO2 post-combustion capture, a sim- removal of CO2 [8,9]. This operation has been used in the last years ple tool useful for an immediate and preliminary analysis on the for the removal of CO2 from natural gas and its introduction in the light of specific considerations, strictly related to the output to be CCS (Carbon Capture and Storage) concept in relatively new. Great obtained. advantages of cryogenic CO2 capture with respect to absorption are that no chemical absorbents are required and that the process 2. Membrane gas separation technologies for CO capture can be operated at atmospheric pressures. The main disadvantage 2 in post-combustion of this system is that the water content in the feed stream to the cooling units should be minimal in order to prevent plugging by ice Membrane GS is most often listed as potential candidate for or an unacceptably high rise in pressure drop during operation.
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