WO2012176176A1 - Système mcfc à empilements multiples et procédé de séparation de c02 d'un gaz de combustion contenant des sox et des nox - Google Patents

Système mcfc à empilements multiples et procédé de séparation de c02 d'un gaz de combustion contenant des sox et des nox Download PDF

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WO2012176176A1
WO2012176176A1 PCT/IB2012/053197 IB2012053197W WO2012176176A1 WO 2012176176 A1 WO2012176176 A1 WO 2012176176A1 IB 2012053197 W IB2012053197 W IB 2012053197W WO 2012176176 A1 WO2012176176 A1 WO 2012176176A1
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block
stacks
burner
anodes
mcfc
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WO2012176176A8 (fr
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Paolo Capobianco
Biagio Passalacqua
Angelo Giovanni PERFUMO
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Ansaldo Energia SpA
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Ansaldo Energia SpA
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
    • H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
    • H01M8/04097—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants with recycling of the reactants
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/32—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by electrical effects other than those provided for in group B01D61/00
    • B01D53/326—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by electrical effects other than those provided for in group B01D61/00 in electrochemical cells
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0662—Treatment of gaseous reactants or gaseous residues, e.g. cleaning
    • H01M8/0668—Removal of carbon monoxide or carbon dioxide
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0662—Treatment of gaseous reactants or gaseous residues, e.g. cleaning
    • H01M8/0675—Removal of sulfur
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/14—Fuel cells with fused electrolytes
    • H01M8/144—Fuel cells with fused electrolytes characterised by the electrolyte material
    • H01M8/145—Fuel cells with fused electrolytes characterised by the electrolyte material comprising carbonates
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/249—Grouping of fuel cells, e.g. stacking of fuel cells comprising two or more groupings of fuel cells, e.g. modular assemblies
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/30—Sulfur compounds
    • B01D2257/302—Sulfur oxides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/40—Nitrogen compounds
    • B01D2257/404—Nitrogen oxides other than dinitrogen oxide
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/50—Carbon oxides
    • B01D2257/504—Carbon dioxide
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2258/00—Sources of waste gases
    • B01D2258/02—Other waste gases
    • B01D2258/0283—Flue gases
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

Definitions

  • the present invention relates to a multi-stack
  • MCFC system for separating C02 from combustion flue gas containing NOx and Sox, and to a method for separating C02 from combustion flue gas containing NOx and SOx by means of a multi-stack MCFC system.
  • the invention relates to the field of systems for separating C02 from combustion flue gas, and more specifically to the field of processes and devices capable of selectively extracting C02 from the flue gas it is diluted into, in order to provide it concentrated in a gaseous stream from which it can be easily separated.
  • MCFC-CCS systems i.e. systems where by means of molten carbonate fuel cells (MCFC) , C02 is extracted from the flue gas it is diluted into and is concentrated in a gaseous stream rich in H20 vapor and substantially free from diluting N2, so as to facilitate the subsequent capture thereof (CCS
  • MCFC systems have also been suggested where the stacks have the cathode supply, the anode supply or both supplies in series (as shown for example in EP442352, US5413878, EP0947022), according to logics aimed to meet specific needs on a case by case basis, usually related to the increase in efficiency or improvements to thermal management.
  • these are solutions designed for systems where all the C02 built up at the anode outlets is sent to the cathodes since it is required for the cathode supply within the same MCFC system, which circumstance actually leaves no margin for an extraction and capture thereof.
  • all the circulating C02 is released to the atmosphere through one or more cathode outlets.
  • hybrid multi-stack systems are also known in the art, meaning that they incorporate fuel cells of a different line in a fluid series connection (as shown for example . in US6033794, US6623880, US5541014) .
  • MCFC-CCS systems even when configured as multi-stack (i.e. consisting of multiple MCFC cell stacks electrically connected to one another) , they are described as consisting of identical stacks, or all fluidly arranged in parallel, or organized as strings fluidly arranged in parallel, with each string consisting of two or more stacks in a series, and they are supplied so that the stacks (if all in parallel) or all the strings of stacks, respectively, work in the same nominal process conditions.
  • the manipulating members of the anode exhausts may be one for each of the single stacks or in any case for multiple stacks; in the second case, one for every single string, a common one for multiple strings, or also one for single stacks of a string, as indicated in patent application MI2009A002259.
  • the manipulation members of anode exhausts may be one for each of the single stacks in parallel, a common one for multiple stacks of a same string or also one common to multiple strings.
  • the combustion flue gas may be very different by type and level of critical contaminants found, but they usually have in common the fact of having some above the thresholds allowed by MCFC (sometimes well above them) .
  • MCFC-CCS systems that use DIR stacks as backbone for the capture of C02 from the flue gas (and for producing electrical power with high efficiency associated thereto) and which nevertheless are suitable for accepting higher SOx contents in input.
  • stacks without direct internal Reformer are also found in such multi-stack systems, the cathodes of which are the only inlet way of the flue gas into the same MCFC-CCS system.
  • DIR stacks are operated on dirty flue gas at the inlet of the MCFC-CCS system by having the cathode supply downstream of a stack without DIR which, in addition to a complementary role in capturing C02, carries out a filtering action (Italian patent application MI2009A002259) .
  • the limits to SOx are those (much milder) valid for stacks with indirect internal reformer or without internal reformer and not the very restrictive ones required by DIR stacks.
  • the S found in the flue gas (in the form of SOx) is almost integrally captured by the electrolyte of the first stack that encounters on its path (and then released as H2S in the anode exhaust of said stack) . Since in the solution described in MI2009A002259 this first stack is not provided with direct internal reformer, the thermal management and the H2 availability therein are not affected by the release as H2S in the anode compartment of SOx entered on the cathode side. SOx is absent in the supply of the DIR stack cathodes and therefore the vitality of catalyst, directly arranged into the anode compartment, is not affected.
  • MI2009A002259 only relates to the arrangement in series of a stack without DIR and of a DIR, the teaching that can be derived therefrom is wider: placing two stacks in a series on the cathode side makes the downstream one work with cleaner oxidant and without SOx.
  • the SOx level in the cathode being the same, the penalization extent is very sensitive to the composition and use of the anode gas: gases rich in H2 and low H2 use reduce it.
  • the SOx contents must be brought below the valid threshold when the specific type of stack used works with poor anode gas.
  • the NOx found in the cathode gas in fact tend to react with the electrolyte, forming alkaline nitrites and nitrates that are diffused in the die.
  • the anode side removal by the effect of the anode gas much more effective when the anode gas is richer in H2, takes place almost entirely generating N2 and in a minimal part NH3 (ratio in the order of 100:1)..
  • NOx cause a penalization of the performance, so also in this case a steady working point can only be obtained at reduced current density and with a lower voltage than would be found in the same conditions with clean gases.
  • Trapping N2 in the anode loop would unavoidably inhibit the wash off, on the anode side, of nitrites and nitrates formed in the electrolyte by the effect of the cathode reaction with the NOx. This would force the NOx in the flue gas to be of few ppm, so as not to affect the stack efficiency.
  • the N2 build up would prevent the use of the same stacks as an instrument for further reducing the NOx emissions to the atmosphere by the hosting system, making the capability that is intrinsic to the MCFC but strictly related to the onset and the persistence of anode side washing conditions, of converting a significant portion of the NOx entered on the cathode side into N2, useless.
  • MCFC-CCS system which, compared to known systems, works at a high electrical efficiency and at the same time with higher thresholds on SOx and NOx in the cathode gas.
  • the present invention therefore relates to a system and a method for separating C02 from combustion flue gas by means of multi-stack molten carbonate fuel cells (MCFC ) as defined in essential terms in the annexed claims 1 and 12, respectively, as well as, for the preferred additional characters, in the dependent claims.
  • MCFC multi-stack molten carbonate fuel cells
  • the MCFC-CCS system is organized into two or more blocks of stacks, blocks having the respective cathode lines connected in series;
  • the anodes of the stacks of the first block are made to operate as much as possible in excess of H2, making as much H2 as possible pass through them than what is globally required for supplying the entire MCFC- CCS system as a whole, optionally adding more H2 that can be used by the hosting system or by other users;
  • the stacks of the first block can work with rich anode gas in input and with low use of H2, and thus with rich gas (anode exhaust) in output too; this condition, for a given level of SOx and Ox, respectively, in input minimizes the performance penalization of the stacks of the first block with respect to those obtainable in the same working points with clean gases and at the same time it maximizes the capability of draining SOx and NOX from the flue gas supplied to the cathodes;
  • the separation devices for C02 recovery located on the anode outputs of the stacks of the various blocks, and the lines that manipulate the anode exhaust are organized so that said H2S and N2 can be expelled from the MCFC-CCS system without making H2S generated by the SOx found in the flue gas pass in the anodes of the stacks of the second block (and of the following ones) ;
  • the stacks of the blocks following the first one work on substantially clean oxidants, at most containing NOx residues brought again below the thresholds that affect performance.
  • the main component elements of the invention therefore are:
  • an MCFC-CCS comprising at least two blocks of MCFC stacks (there are no bars for the type of stacks which may for example be of the DIR type, IIR type, without internal reformer, etcetera) ;
  • connection system configured so that:
  • the flue gas to treat with the MCFC-CCS system only supplies the cathodes of the stacks of the first block (with or without addition of air) ; the following blocks are only supplied with flue gas that has already passed through the cathodes of stacks of the first block;
  • the various blocks are in fluid connection in series on the cathode side, i.e., the outputs of the stack cathodes of the first block supply cathodes of the stacks of the second block (with or without addition of air) and if the blocks are more than two, the outputs of the stack cathodes of the second block supply (with or without addition of air) cathodes of the stacks of the third block and so on, for any following blocks;
  • separator devices connected to the anode outputs of all the cells of the stacks of all blocks and that remove H20 and separate a stream containing C02 for the capture from a stream rich in H2; said separator devices are organized so as:
  • At least one portion of the fuel required by other blocks, by the hosting system or by other external users passes, in the form of H2, through the anodes of the stacks of the first block or alternatively, at least one portion of the stream rich in H2 exiting from separator devices connected on the anode outputs of stacks of other blocks passes through the anodes of the stacks of the first block (and thus through the separator connected to the anode outputs of the stacks of the first block) before reaching the system internal or external burner.
  • the system as a whole is therefore configured to increase the H2 content in the anode gas of the stacks of the first block (in input but also in output), without causing fuel wastes.
  • the invention achieves the following specific advantages compared to MCFC-CCS systems made according to the prior art .
  • the present invention is capable of keeping the current generation mechanism in the MCFC system active, which leads to the removal of C02 from the combustion flue gas, in spite of input SOx and NOx contents higher than those set as thresholds for known solutions .
  • the present invention allows the actual use of the potential of MCFC cells to act as an instrument for reducing the emissions of residues not just of CO and SOx but also of NOx found in the flue gas .
  • the invention achieves: the efficiency being the same, higher thresholds of both SOx and of NOx contents in the flue gas; and SOx and NOx levels being the same, higher efficiency;
  • the invention achieves much higher thresholds on NOx and capability of using the same stack as a further instrument for removing NOx;
  • the invention achieves much higher thresholds for both SOx and for NOx, along with a wide freedom in the selection of the type of stacks to make the blocks of the CFC-CCS system.
  • FIG. 1 shows a schematic view of a system for separating C02 from combustion flue gas by means of molten carbonate fuel cells (MCFC) made according to a first embodiment of the invention
  • FIG. 2 shows a schematic side view of a second embodiment of the invention
  • a system 1 comprises: a first MCFC-CCS block 11 of MCFC stacks, at least a second MCFC-CCS block 12 of MCFC stacks, at least one burner 13 provided with reformer 14, and a connection system 15 that connects blocks 11, 12 and burner 13.
  • system 1 may include a series of second blocks 12.
  • Blocks 11, 12 comprise respective groups of stacks 21, 22 of MCFC cells, having respective cathodes 23, 24 (or cathode compartments) and anodes 25, 26 (or anode compartments), and respective separators 27, 28 acting on the anode exhaust of stacks 21, 22.
  • Cathodes 23, 24 of the two blocks 11, 12 are connected in series; if multiple second blocks 12 are provided, they have the cathodes of the respective stacks connected in series.
  • stacks 21, 22 of both blocks are provided with internal reformer 31, 32, for example indirect (IIR) or direct (DIR) internal reformer.
  • IIR indirect
  • DIR direct
  • System 1 has a flue gas inlet 33, through which the combustion flue gas to be processed coming from a hosting system and generally containing SOx and Ox, enter into system 1.
  • the flue gas inlet 33 is arranged upstream of burner 13 and is connected to burner 13, which for example is a catalytic burner, via a flue gas supply line 34, through which the flue gas enters into burner 13;
  • reformer 14 for example is a MIR ("modular integrated reformer") .
  • air is added to the flue gas supplied to system 1, through an air supply line 35 which fits onto the flue gas supply line 34.
  • Burner 13 has an outlet connected to cathodes 23 of stacks 21 of the first 'block 11, through a cathode inlet line 36; cathodes 23 are therefore supplied with oxidizing gas consisting of the flue gas coming from the hosting system, optionally enriched with air and with the combustion products into burner 13.
  • cathodes 23 The outlet of cathodes 23 is connected through a cathode line 37 to the inlet of cathodes 24 of stacks 22 of the second block 12.
  • an air supply line 38 fits onto the cathode line 37 for adding air to the stream supplied to cathodes 24.
  • the stream exiting from cathodes 24 is collected by a venting line 39 which leads to a vent 40.
  • Anodes 25 of the first block 11 are supplied with a stream coming from reformer 14 through an anode inlet line 41; reformer 14 is supplied with fuel through a fuel supply line 42, for example CH4, and with a flow rate of H20 (vapor) needed for converting the fuel into H2.
  • the fuel flow rate supplied to reformer 14 serves for covering all the uses of blocks 11, 12 (if only stacks without internal reformer are used) or the part in excess to that already covered by the hydrogen produced into the stacks (if stacks with internal reformer are provided) and also for supplying a fraction of the energy of the hosting system.
  • the streams exiting from anodes 25 of stacks 21 of the first block 11 are sent, through an anode line 43, to separator 27 (of the known type) , configured so as to remove H20 and extract C02 and H2S, in a sequence or concurrently .
  • the stream rich in H2 and containing residual fuels exiting from separator 27 is partly sent to anodes 26 of stacks 22 of the second block 12, through a further anode line 44 (either directly or passing through reformer 32), and partly to the hosting system, through an anode outlet line 45, to be used therein.
  • the streams exiting from anodes 26 of stacks 22 of the second block 12 are sent, through an anode line 46, to separator 28 (of the known type) which removes H20 and extracts C02.
  • the stream rich in H2 and containing residual fuels exiting from separator 28 is sent through a recirculation line 47 to burner 13, where the residual fuels contained in such a stream are burnt and the heat is recovered for supporting the reactions within reformer 14 and for heating the oxidizing gas containing the combustion flue gas supplied to the first block 11 (optionally, the flue gas is preheated through thermal exchange with the stream exiting from cathodes 24 of the second block 12).
  • the conversion into H2 of a fuel flow rate in excess of the requirement of the first block takes place within reformer 14, i.e. upstream of anodes 25 of the first block 11.
  • An additional flow rate of H2 is thus generated that can pass unaltered through anodes 25 of the first block 11, contributing to reduce the use of H2 and thereby to increase the output H2 percentage too. This contributes to creating more favorable conditions for the removal of sulfur and nitrites/nitrates from the electrolyte. It should be noted that this happens without the need for additional fuel since a part of the fuel used by the hosting system is used without consuming it.
  • the internal reformers 31, 32 of stacks 21, 22 are supplied through respective fuel supply lines .48, 49 with fuel (CH4) and vapor flow rates needed for allowing the thermal management of the respective stacks 21, 22, through the heat absorption associated with the endothermic reaction of H2 production from the fuel reforming.
  • the H2 streams produced within reformers 31, 32 are supplied to anodes 25, 26 of the respective stacks 21, 22.
  • reformer 14 Since reformer 14 is arranged upstream of anodes 25 of the first block 11, all the hydrogen generated within system 1, with the exception of that strictly necessary to generate within the internal reformer 32 of stacks 22 of the second block 12 for ensuring the thermal management thereof, enters into anodes 25 of stacks 21 of the first block 11. This is essential for enriching with H2, both in input and in output, the anode gases of stacks 21 of the first block 11 to the maximum extent allowed, the fuel flow rate supplied to system 1 being the same.
  • the devices used for enriching the anode gas of stacks 21 of the first block 11 are effective since they do not trigger build-up mechanisms of H2S (which is removed by separator 27) or of N2 (which is partly eliminated through the anode exit line 45 and partly through the venting line 39) .
  • the entire stream rich in H2 exiting from separator 27 of the first block 11 is sent to anodes 26 of stacks 22 of the second block 12, through the anode line 44 (whereas the anode exit line 45 shown in figure 1 is not used) .
  • the stream rich in H2 exiting from separator 27 is not sent to anodes 26 of stacks 22 of the second block 12, but it is partly sent to the hosting system, through the anode exit line 45, to be used therein, and it is partly recirculated through an anode recirculation line 51 (shown with a dashed line in figure 1) which fits onto the anode inlet line 41, to anodes 25 of stacks 21 of the first block 11 (whereas the anode line 44 is not used) .
  • the stream rich in H2 exiting from separator 27 is partly recirculated to anodes 25 of stacks 21 of the first block 11, through the anode recirculation line 51, and for the remaining part to burner 13, reaching it either through the recirculation line 47, after having passed through anodes 26 of stack 22 and through separator 28 of the second block 12, or directly through a further recirculation line 52 (also shown with a dashed line in figure 1) which fits onto said line 47, and/or to an external user (for example the hosting system), either directly or after passing through anodes 26 of stack 22 of the second block 12 (or of following blocks, if provided) .
  • the streams rich in H2 exiting from separators 28 of the second block 12 are entirely or partially sent (rather than or in addition to burner 13) to anodes 25 of stacks 21 of the first block 11, through an auxiliary line 53 that branches off the recirculation line 47 and fits onto the anode inlet line 41, before being sent to burner 13 (or another burner, internal or external to the MCFC-CCS blocks 11, 12) , or to an external user.
  • burner 13 may be internal or external to the MCFC-CCS blocks 11, 12.
  • the flue gas passage in burner 13 favors the heating of the oxidizing gas to the inlet temperature to the stacks.
  • the flue gas heating may also be carried out in a different way, for example by recovering heat, with suitable exchangers, from one or more of the hot streams circulating within system 1 and that need to be cooled (such as for example the stream exiting from cathodes 24 of the second block 12 and collected by the venting line 39, or the anode discharges exiting from anodes 25, 26 through the anode lines 43, 46) .
  • the outlet of burner 13 where the combustion of residual fuels not used by stacks 21, 22 of blocks 11, 12 takes place is connected to cathodes 23 of stacks 21 of the first block 11, which are therefore supplied with the gaseous stream exiting from burner 13.
  • system 1 in order to increase the capture of C02, comprises a supplementary MCFC group 55, consisting of one or more stacks 56 of MCFC cells having respective cathodes 57 and anodes 58, and the outlet of burner 13 is connected to cathodes 57 of group 55, so that the gaseous flow exiting from burner 13 supplies cathodes 57 (optionally enriched with air) .
  • Group 55 has an anode outlet connected, via an anode line 60, to a separator 59 that removes H20 and C02 from a residual stream containing H2.
  • the combustion flue gas coming from the hosting system is supplied, rather than to burner 13 as described above, to cathodes 23 of stacks 21 of the first block 11 (optionally after adding air through the air supply line 35) .
  • the flue gas inlet 33 is placed upstream of cathodes 23 and the flue gas supply line 34 directly enters into the first block 11 and supplies cathodes 23.
  • the fuel supply line 42 supplies, in addition to reformer 14 as described above, also anodes 58 of the supplementary group 55.
  • system 1 still has the general configuration described above and the variations already mentioned with reference to figure 1 are possible, especially as regards the management of the stream rich in H2 and containing residual fuels exiting from separator 27 of the first block 11, which may be sent to one or more of:
  • the streams rich in H2 (and containing residual fuels) exiting from separator 28 of the second block 12 is partially sent directly to burner 13 through the recirculation line 47, and partially also to anodes 25 of stacks 21 of the first block 11, through an auxiliary line 53 that branches off line 47 and fits onto the anode inlet line 41 (that connects reformer 14 to anodes 25) before being sent to burner 13 (or another burner, internal or external to the MCFC-CCS blocks 11, 12), or to an external user.
  • the stream exiting from burner 13 is also sent to the inlet of cathodes 24 of stacks 22 of the second block 12, and/or, in the case of multiple blocks 12 in series, of the cathodes of the stacks of one of the following blocks.
  • separator 27 is configured so as to separate from the anode exhaust exiting from anodes 25 of stacks 21 of the first block 11 a stream of H20 and, separately, a stream substantially of pure H2; this stream of "pure" H2 is recirculated to the same anodes 25 through the anode recirculation line 51; the residual stream of separator 27, containing C02, H2, residual fuels, H2S, etcetera, is conveyed via a treating line 62 to burner 13 (or another burner) , where residual fuels, remained with the C02 to be sent to capture, are eliminated by combustion in 02 or in mixtures 02/C02, and then to another final separator 63 of C02.
  • stack 22 of the second block 12 includes MCFC cells with indirect internal reformer, with recirculation of the stream rich in H2 exiting from separator 28 on anodes 26.
  • the system comprises a further auxiliary separator 64 arranged between the outlet of reformer 14 and anodes 25 of stack 21 of the first block 11 and thus along the anode inlet line 41.
  • the auxiliary separator 64 removes C02 and H2o from the stream supplied to anodes 25.
  • the invention also allows a wide freedom of selection as regards the type of stacks to be used for the different blocks.
  • stacks with indirect internal reformer IIR or without internal reformer for the first block and stacks with internal reformer (either direct DIR or indirect IIR) for the second block (and any following ones) is the preferable choice in most cases, where it is convenient to work at atmospheric pressure. But also different combinations may conveniently be used in special situations.
  • the use of cells with DIR reformer in the first block may also be contemplated, where while it removes C02, it mainly plays the role of reducing the NOx to the benefit of the following blocks, in the case of sulfur-free flue gas.

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  • Treating Waste Gases (AREA)

Abstract

L'invention concerne un système MCFC à empilements multiples (1) destiné à séparer du C02 d'un gaz de combustion contenant des NOx et des SOx. Ce système comprend : un premier bloc MCFC-CCS (11) d'empilements de MCFC et au moins un deuxième bloc MCFC-CCS (12) d'empilements de MCFC, pourvus de séparateurs respectifs (27,28) agissant sur les échappements anodiques, au moins un brûleur (13) et un système de connexion (15) qui connecte les blocs (11,12) et le brûleur (13) de sorte que : les cathodes (23,24) des empilements (21,22) des deux blocs (11,12) soient connectées en série; le gaz de combustion à traiter pénètre seulement dans les cathodes (23) des empilements (21) du premier bloc (11), avec ou sans ajout d'air; dans le deuxième bloc (12), et dans tout bloc suivant, aucun gaz de combustion ne pénètre sans avoir traversé les cathodes (23) des empilements (21) du premier bloc (11); les anodes (25,26) des empilements (21,22) de chaque bloc (11,12) soient connectées aux séparateurs respectifs (27,28) qui éliminent H20 et séparent un flux contenant du C02, conçu pour être capturé par un flux riche en H2; les séparateurs (27,28) et les lignes qui manipulent les échappements anodiques soient organisés de sorte que H2S et N2 soient rejetés du système.
PCT/IB2012/053197 2011-06-24 2012-06-25 Système mcfc à empilements multiples et procédé de séparation de c02 d'un gaz de combustion contenant des sox et des nox Ceased WO2012176176A1 (fr)

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