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138 IPCC Special Report on Carbon dioxide Capture and Storage fin heat exchanger, fabricated in stainless steel or high nickel alloy by vacuum brazing or diffusion bonding. to further integrate the gasification of the fuel (if solid), the shift reaction, and in-situ CO2 removal with CaO. The overall reaction aimed in the system is: Carbonation of calcium oxide: CaO + C + 2 H2O → CaCO3 + 2H2 (5) An SMR reactor consists of alternate passages having fins, which are coated with catalyst or porous catalyst insets. Heat is produced by catalytic combustion of fuel gas premixed with air and transferred by conduction to the adjacent passage fed with the steam/hydrocarbon mixture, where the reforming reaction takes place (Babovic et al., 2001). Very compact high efficiency systems can be produced. Although these units are being currently developed by a number of groups for small- scale H2 production for fuel cell applications, they also show promise in larger H2 plants. 3.5.3.4 Conversion to hydrogen and carbon The regeneration of the sorbent produces pure CO2 when carried out in a separate reactor by calcining CaCO3. A range of systems can be developed under this general reaction scheme depending on the technology adopted for gasification, carbonation-calcination, hydrogen utilization route and storage option for CO2. The first of these concepts was proposed at the Los Alamos National Laboratory (USA) and is currently under development as the Zero Emission Coal Alliance (ZECA) process. The full system includes (Lackner et al., 2001) a hydro- gasification reactor, solid oxide fuel cell and a technology for mineral carbonation. However, the fuel cell will require more development and mineral carbonation is only at the laboratory investigation stage (see Section 7.2 for a discussion of mineral carbonation). Thermal cracking or pyrolysis of methane is the reaction where methane reacts to carbon and hydrogen through: Methane pyrolysis: CH4 → C + 2 H2 (4) The main advantage of the process is that it can potentially yield a clean gas (free of carbon oxides) that could be used directly for power production, but a disadvantage is that the chemical energy from the oxidation of carbon to CO2 is not released. The cracking reaction is endothermic and so heat has to be supplied to the reaction. If the natural gas is converted fully, the theoretical yield of hydrogen corresponds to 60% of the heating value of the natural gas. The amount of carbon, which can be obtained, corresponds to 49% of the heating value, with the extra 9% of the energy in this calculation being provided as endothermic heat shown by reaction (4) above. Therefore full conversion can be achieved only if heat is supplied from an external source. If full conversion of methane is not achieved, the remaining methane will be combusted to produce heat. There are many different methods under development for reactors based on this principle, including thermal catalytic, thermal non-catalytic and plasma cracking. The HyPrRing process (Lin et al., 2002) is being developed by the Center for Coal Utilization of Japan. It integrates gasification, reforming and in situ CO2 capture in a single reactor at pressures above 12 MPa and temperature above 650oC. Projects in Norway using natural gas and in Germany using brown coal (Bandi et al., 2002) are also underway developing pre-combustion systems using capture of CO2 with CaO. Finally, General Electric (Rizeq et al., 2002) is developing an innovative system involving the capture of CO2 in the gasification reactor by a high temperature sorbent and with calcination in a separate reactor by burning part of the fuel with an oxygen carrier. In the plasma cracking process natural gas or other hydrocarbons are supplied to a plasma reactor where the hydrocarbons are cracked under pyrolysis conditions (i.e., in absence of oxides, e.g., steam, which can supply oxygen to form CO or CO2). The plasma arc, for which electricity is used, supplies the heat for the cracking reaction. Advantages of the process are its flexibility with respect to the fuel and the high quality carbon black which can be produced. Two small-scale plasma cracking processes for hydrogen/syngas production have been in development. The Glid Arc process has been developed by the Canadian Synergy Technologies Corporation. The second process is the Kvaerner CB&H process. Kvaerner has reported results for a pilot plant producing 1000 Nm3 hydrogen per hour and 270 kg or 500 kg carbon black using natural gas and aromatic oil respectively (IEA GHG, 2001). All these systems are at an early stage of development. Detailed process simulations show that the efficiencies are potentially high because most of the energy employed for sorbent regeneration is effectively transferred to the H2 generated in reaction (5). The systems are aimed at very large-scale generation of electricity and/or H2 and cement production (from the deactivated sorbent, CaO). However, many uncertainties remain concerning the performance of the individual units and their practical integration. The main challenge may be the regeneration of the sorbent at very high temperatures (>9000C), to produce a pure stream of CO2. Another is the operating conditions to achieve sufficient conversion towards hydrogen, without the use of a catalyst for the shift reaction. 3.5.3.5 Technologies based on calcium oxide 3.5.4 Enabling technologies The performance and cost of a pre-combustion capture system is linked to the availability of the enabling technologies that complete the system. In this section we consider the availability of industrial systems, to produce heat from the de-carbonized fuel and gas turbines and fuel cells to produce power. There is a range of pre-combustion systems that make use of the carbonation reaction of CaO at high pressures and temperatures,PDF Image | CARBON DIOXIDE CAPTURE AND STORAGE
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