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Chemical-Looping Combustion for Combined Cycles With CO2 Capture

Stefano Consonni1
e-mail: stafano.consonni@polimi.it

Giovanni Lozza Giampaolo Pelliccia
Dipartiamento di Energetica, Politecnico di Milano, Milan, Italy

Stefano Rossini Francesco Saviano
Enitecnologie, San Donato Milanese, Milan, Italy

Chemical-Looping Combustion (CLC) is a process where fuel oxidation is carried out through an intermediate agent—a metal oxide—circulated across two fluidized bed reactors: a reduction reactor, where an endothermic reaction reduces the metal oxide and oxidizes the fuel, and an oxidation reactor, where an exothermic reaction oxidizes the metal oxide in air. Overall, the system carries out the same job of a conventional combustor, with the fundamental advantage of segregating the oxidation products ͑ CO 2 and H 2 O ͒ into an output flow free of nitrogen and excess oxygen. The flow exiting the reduction reactor consists of water and CO 2 , the latter readily available for liquefaction, transport and long-term storage. The hot, vitiated air from the oxidation reactor is the means to produce power through a thermodynamic cycle. This paper reports of a study supported by the ENI group to assess the potential of the integration between CLC and combined gas-steam power cycles. More specifically, we focus on four issues: (i) optimization of plant configuration; (ii) prediction of overall efficiency; (iii) use of commercial gas turbines; (iv) preliminary economic estimates. The CLC system is based on iron oxides which, to maintain their physical characteristics, must operate below 900 – 1000°C. Given the crucial importance of the temperature of the vitiated air generated by CLC on the performance of the combined cycle, we consider two options: (i) ‘‘unfired’’ systems, where natural gas is fed only to the CLC system, (ii) ‘‘fired’’ systems, where the vitiated air is supplementary fired to reach gas turbine inlet temperatures ranging 1000 – 1200°C. Results show that unfired configurations with maximum process temperature 850 – 1050°C and zero emissions reach net LHV plant efficiencies ranging 43% – 48%. Fired cycles where temperature is raised from 850 to 1200°C by supplementary firing can achieve 52% net LHV efficiency with CO 2 emission about one half of those of a state-of-the-art combined cycles. Fired configurations allow significant capital cost and fuel cost savings compared to unfired configurations; however, a carbon tax high enough to make them attractive (close to 50 ញC /ton) would undermine these advantages. ͓DOI: 10.1115/1.1850501͔

1

Background and Scope

The use of fossil fuels is so widespread and deep-rooted in industrial societies ͑and man’s habits͒ that its reduction as a means to reduce greenhouse gas emissions will require an unprecedented, daunting effort ͓1͔. In the short- and medium-term, substantial reductions of greenhouse gas emissions could still be achieved by sequestering the CO2 generated by fossil fuels oxidation. The capture and long-term storage of CO2 —or possibly other carbon-laden compounds ͓2͔—could thereby ease the transition toward the long-term goal of a society relying on most environmentally benign energy sources and conversion systems. CO2 sequestration appears to make most sense for large-scale power stations, either due to economies of scale and to the complexity of the systems needed for capture and storage. In this case there appear to be three crucial issues: 1. CO2 capture in fossil fuel-fired power plants; 2. CO2 transport to storage site; 3. availability of appropriate, long-term storage sites. This paper focuses on the first issue, assuming that a system does exist for transporting liquid, supercritical CO2 at 85 bar to a safe,
1 To whom correspondence should be addressed. Contributed by the International Gas Turbine Institute ͑IGTI͒ of ASME for publication in the JOURNAL OF ENGINEERING FOR GAS TURBINES AND POWER. Paper presented at the International Gas Turbine and Aeroengine Congress and Exhibition, Vienna, Austria, June 13–17, 2004, Paper No. 2004-GT-53503. Manuscript received October 1, 2003; final manuscript received March 1, 2004. IGTI Review Chair: A. J. Strazisar.

long-term storage site like depleted oil or gas fields, underground caverns, aquifers or deep oceanic waters. Should higher pressures be required, they can easily be achieved with very low pumping energy requirements. In a fossil fuel-fired power plant, CO2 capture can be carried out by a variety of processes and technologies. A host of recent studies focus on three concepts involving relatively well-known technologies: i. CO2 removal via amine chemical absorption from flue gas ͓3,4͔; ii. fuel decarbonization, i.e. conversion of fossil fuel into hydrogen and CO2 , which is removed ahead of combustion ͓5,6͔; iii. oxy-combustion, where nearly-pure CO2 is obtained by knocking out the water from the gas generated by burning the fuel into oxygen ͓7,8͔. This paper focuses on yet another technology, often named as Chemical Looping Combustion ͑CLC͒, reporting the outcome of a research commissioned by Enitecnologie, a company of the ENI group, to the Energy Department of Energy Engineering Politecnico di Milano. The CLC concept is illustrated in Fig. 1. Natural gas enters a ‘‘reduction reactor’’ where solid metal oxides are reduced by giving up oxygen to the fuel, which is therefore oxidized to CO2 and water. Reduced metal oxides then flow into an ‘‘oxidation reactor’’ where they are oxidized in air. The flow of solid, oxygen-rich metal oxides and vitiated air exiting the oxidation reactor enters a cyclone, where the solid oxides are separated from the gas stream JULY 2006, Vol. 128 Õ 525

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The metal oxide floats ͑or circulates͒ in the beds as a relatively fine powder to make available the solid–gas contact surface needed to carry out the heterogeneous reactions with natural gas ͑in the reduction reactor͒ and with oxygen ͑in the oxidation reactor͒. with the fundamental advantage that the oxidation products (CO2 and H2 O) are made available in a flow nearly free of diluents. consequently. 1 must be coupled to a thermodynamic cycle. Fe looks more attractive than Ni due to its lower cost and higher reactivity.9 Ϫ1033.3 kJ͒. the operating conditions.Table 1 Reduction and oxidation reactions for selected metals to be used for CLC. the maximum temperature reached by the metal oxide equals the temperature of the vitiated air discharged by the oxidation reactor. according to Ref. we aim at: a. 1 Chemical looping combustion concept and recycled ͑whereby the term ‘‘looping’’͒ to the reduction reactor ͓9. JULY 2006 Downloaded 24 Jul 2008 to 131.9 kJ per mole of CH4 to be supplied to the reactants are the difference between the heat needed to reduce the metal ͑for 8 moles of Fe3 O4 . ⌬ H R maximum system temperature is reached at the outlet of the RR when the reduction reaction is exothermic „Cu.7 Ϫ978 Ϫ802. carry out a preliminary economic evaluation.Ni…. the system in Fig. All this while accounting for the limits imposed by the CLC process and by state-of-the-art power plant technology. their heat 526 Õ Vol.9 kJ (1) where the 230. On the other hand.2 kJ (2) If the reactors are adiabatic.Mn…. iron and nickel show very high CH4 to CO2 conversion rate in the reduction reactor. Table 1 summarizes the reactions taking place in the reduction and oxidation reactors. 1033. the temperature in the reduction reactor decreases. 1 can be implemented in a number of ways. 128. besides being relatively cheap and easy to supply. Fe and Ni are preferable because the reduction reaction is endothermic. Here the CLC system is modeled based on simplifying assumptions which are insufficient to define the actual Transactions of the ASME 2 CLC Technology The CLC concept depicted in Fig.org/terms/Terms_Use. the reduction reactor reduces hematite (Fe2 O3 ) to magnetite (Fe3 O4 ) according to the endothermic reaction: CH4 ϩ 12 Fe2 O3 → CO2 ϩ 2 H2 Oϩ 8 Fe3 O4 Ϫ 230. exactly what is needed to maximize power plant performance for a given maximum temperature of the solid in the beds. the solid particles comprise also inert material—or possibly a catalyst—to warrant adequate physical.asme. In order to generate power. the type of reactor. one may consider copper. CLC requires a clean fuel like natural gas to avoid contamination and degradation of the circulating solids. we will not deal with the details of reactor chemistry and kinetics.͒.5 Ϫ284. of reaction determines—under adiabatic conditions—a temperature decrease in the reduction reactor.193. nor with the issues related to the thermo-fluid-dynamic and structural design of the reactors and their ancillary components ͑cyclones. CLC temperatures͒ affect efficiency and specific output.3 Fig. depending on the type and physical characteristics of the oxide that carries out the chemical loop. In a CLC system based on iron oxides and fed with pure methane. basic constraint regards the fuel input. c. show how the operating parameters ͑gas turbine pressure ratio. the cycle would operate with a maximum temperature lower than the maximum temperature tolerable by the metal oxide—a situation which would penalize performance. 2. With Cu and Mn the temperature at the outlet of an adiabatic reduction reactor would be higher than the temperature of the vitiated air sent to the power cycle. This paper addresses the integrated process where CLC is coupled to a combined gas-steam power cycle. the system is equivalent to a conventional combustor. Moreover. see http://www. etc. referred to the combustion of one mole of 0 Äheat of reaction at 25°C. Redistribution subject to ASME license or copyright.2 kJ needed to reduce Fe2 O3 are given back by the oxidation taking place in the OR: 8Fe3 O4 ϩ 2 O2 → 12Fe2 O3 ϩ 1033. These topics are being investigated by Enitecnologie. d. This unfavorable situation could be improved by cooling the reduction reactor to generate high-pressure steam—which however would significantly complicate the design of the reduction reactor and increase its cost. In this paper we consider iron oxides because. As an alternative to iron. One first. In addition to the metal oxide. feeding systems. For adiabatic reactors.cfm .1 Approach Adopted to Estimate Performances. the maximum temperature is reached at the outlet of the oxidation reactor and coincides with that of the vitiated air exported to the CC.234. Therefore.2 Ϫ379. Metal Cu Fe Mn Ni RR OR RR OR RR OR RR OR overall Reactions 8 CuOϩ CH4 ↔ CO2 ϩ 2 H2 Oϩ 4 Cu2 O 4 Cu2 Oϩ 2 O2 ↔ 8 CuO 12 Fe2 O3 ϩ CH4 ↔ CO2 ϩ 2 H2 Oϩ 8 Fe3 O4 8 Fe3 O4 ϩ 2 O2 ↔ 12 Fe2 O3 12 Mn2 O3 ϩ CH4 ↔ CO2 ϩ 2 H2 Oϩ 8 Mn3 O4 8 Mn3 O4 ϩ 2 O2 ↔ 12 Mn2 O3 4 NiOϩ CH4 ↔ CO2 ϩ 2 H2 Oϩ 4 Ni 4 Niϩ 2 O2 ↔ 4 NiO CH4 ϩ 2 O2 ↔ CO2 ϩ 2 H2 O ⌬H0 R (kJ) Ϫ517. the CH4 .2 kJ͒ and the heat released by the oxidation of 1 mole of methane ͑802. In this paper we consider a pressurized system where both reactors are fluidized beds. assess the use of commercial gas turbines. at the outlet of the OR when the reduction reaction is endothermic „Fe. thermal and chemical kinetic characteristics ͑not investigated here͒.192. Since this paper focuses on the potential of CLC for power generation. b. This is why our attention is restricted to natural gas-fired systems and the results obtained here will be compared to the ones achievable by other NG-fired power plants with CO2 capture.10͔ Altogether. manganese and nickel.8 175. assess plant configuration.5 Ϫ422. Operating temperatures and flow rates crucially depend on the type of metal oxide.8 230. Thus. The 1033. ͓11͔. More specifically.

98 1.86 45.25 33. The steam cycle includes three evaporation pressure levels with reheat. thesaturation pressure of water at 6. % mol H2 . 1. In the ‘‘unfired’’ scheme. high-efficiency combined cycles.1% C3 H8 .11 0.09 0 0 64.538 design of the CLC components. ͑ii͒ heat recovery from the pressurized. % wt Gaseous flow mass flow. In the ‘‘fired’’ scheme. Fuel is natural gas with molar composition 92% CH4 .0 54.0 316.2 986.Table 2 Composition and conditions calculated for the flows at the outlet of the reactors for iron and nickel oxides. turbine inlet temperature ͑TIT͒. which however would lessen the benefit of smaller solid oxide flow. because there is a value that maximizes efficiency and another that maximizes specific work.706 MJ/kg.179 0. TIT is determined by the maximum temperature tolerable by the CLC system.009 47. % mol Ar. % mol CO2 .e. pressure is 20 bar. vitiated air.21 50.. In both cases. Since this issue does not apply to CLC plants—at least for ‘‘unfired’’ cycles—NG is heated up to about 300°C. all the NG input goes to the reduction reactor and the gas turbine is fed by hot. c. pressure drops. This inert material is necessary to achieve appropriate physical characteristics of the solid particles and to realize a favorable temperature distribution across the reactors. the CO2 -rich flow is further cooled down to nearly ambient temperature to knock out most of the water. a fraction of the NG input goes to a combustor placed between the CLC and the gas turbine expander. excess hematite. 3.6 6. under the same assumptions. etc. The composition at the outlet of both reactors is at equilibrium. The pressure at which the CO2 -rich flow goes through the evaporators.5 43. ͑ii͒ narrower temperature range spanned by the solid oxides along the loop ͑986 –1050°C for iron vs 707–1050°C for nickel͒.008 0.6 1050 0. ␤ is subject to optimization. %͒ which is further dried and compressed up to 85 bar in an inter-cooled compressor to make it suitable for transport and long-term storage. temperature differences.e.2 43. pressure of CO2 -rich flow.0 707.10 0.7 15.03 0 0 498.087 0 0 65. 2. A catalyst may be needed.2% C2 H6 . pressed air discharged by the gas turbine compressor is fed to the oxidizing reactor and vitiated air is fed to the gas turbine expander. the reactant residence times are higher than the characteristic times of chemical kinetics and of heat/mass transport. which reduces material stresses. iron is likely to be a better choice than nickel due to: ͑i͒ higher reactivity and much lower cost. respectively. °C N2 . 3.3% N2 . 0. but are fully adequate to predict the heat/mass balances and thus the overall performance of the integrated CLC-CC system. lowering the pressure of point 10 in Fig. Both reactors are adiabatic. i. 5. % mol CO. Redistribution subject to ASME license or copyright. In practice.8 1050 82.75 and 46. the performances of the integrated CLC-CC plant depend on the following basic cycle parameters: a. a rather complex arrangement representative of large-scale.e. 3 Power Cycle In unfired plants. of the system components conform to the state-of-the-art of power plant technology. the power generated by such expander can be greater than the extra-power needed for CO2 compression.6 707.0 50.6 bar.47 0.2 353. After accounting for pressure losses. thermal losses.3 1050 82. Downstream of this heat recovery.64 0. kg/s temperature. 6.asme. carrying out the chemical loop according to reactions ͑1͒ and ͑2͒.03 0 0 RR outlet (CO2 rich flow͒ 47. More specifically. gas turbine pressure ratio ␤. because the flow to be compressed is at much lower temperature and has been deprived of most of the water. Hematite (Fe2 O3 ) and magnetite (Fe3 O4 ) are the sole reactive solid species. % mol H2 O. the economizer and the trim cooler shown between points 9 and 10 in Fig. As shown in Fig. kg/s temperature. i. because at point 9 in Fig. In fired plants. 0.32 6. % mol O2 . heat recovery from the CO2 -rich flow takes place across three evaporators ͑each feeding one of the HRSG drums͒ and an LP economizer. with major benefits on performance but also significant increase of CO2 emissions.98 1.5 50. The temperature range spanned by nickel could be reduced by increasing the amount of inert material.8 49. 2 one may place a turboexpander. 2. leaving highly concentrated CO2 ͑94 –96 vol. The table also reports the operating conditions obtained. the higher the efficiency͒ but it is determined by constraints imposed by the gas turbine or by the limits on CO2 emissions. Table 2 exemplifies the CLC operating conditions corresponding to these assumptions. % wt inert material. i. CO2 -rich flow discharged by the reduction reactor generates steam that adds to the steam generated in the HRSG.192. Once it is assumed that efficiencies. it is not fully pursued due to the difficulty of operating fuel control valves above 100–150°C. This is why we assume here that the CO2 -rich flow stays at the pressure of the reduction reactor ͑except for pressure losses͒. TIT is not subject to optimization ͑the higher the TIT. °C reduced Me. Even after properly accounting for expansion and compressor efficiencies. 2. Direct firing with NG allows increasing TIT much above the value tolerable by CLC. b. Maintaining some excess oxygen is essential to warrant the full oxidation of natural gas. the dew point is about 162°C. 2 decreases the dew point temperature2 and ends up in a much lower rate of heat recovered ͑LP steam. 2 could be lower than the pressure at the discharge from the reduction reactor. maximum temperature is 1050°C and air enters the oxidation reactor at 300°C.47 0. d. Although this preheating is always beneficial to the efficiency. Thus. Excess oxygen. preliminary calculations demonstrated that efficiency and power output are rather insensitive to the pressure at point 10. 128 Õ 527 Downloaded 24 Jul 2008 to 131. Due to the lower molecular weight of its reduced and oxidized form. the reduction reactor is fed with 10 kgÕs of natural gas at 15°C „ 467 MWLHV… . see http://www. The simplified scheme of the integrated plant considered here is reported in Fig.org/terms/Terms_Use. % wt oxidized Me.234. we have assumed the following: 1. in the reduction reactor is 10%. 3. the mol fraction of water in the flow exiting the reduction reactor is about two thirds. Coupling a CLC system with a combined cycle implies two types of interaction between the CLC island and the power cycle: ͑i͒ the CLC system substitutes the gas turbine combustor: comJournal of Engineering for Gas Turbines and Power JULY 2006.2 1. To reduce heat transfer irreversibilities and maximize electricity production. % mol Nickel Iron Nickel OR outlet 2507 1050 0. we have also considered NG preheating with saturated water bled from the HP drum. feedwater͒. steam cycle evaporation pressures. Despite this advantage. Unlike TIT. achieving significant investment cost 2 With NG as fuel. Vol.cfm . 3. the pressure ratio ␤ determines the pressure of CLC reactors.193. However.14 RR outlet 2470 986. nickel gives a dramatic reduction of the mass flow circulating across the reactors. 4.18 0.1% higher hydrocarbons. Iron Solids mass flow. if the reactor operates at 10 bar.42 15. HHV and LHV are 51. Inert solid material is 50% of the total flow of solids entering the oxidation reactor. with nickel oxide.3% CO2 .47 OR outlet ͑vitiated air͒ 474.5 1.72 33.1 Basic Cycle Parameters.

fuel cells ͓19͔ and essentially all processes encountered in advanced power plants. 2 Simplified scheme of CLC integrated with a combined cycle reductions ͑elimination of a gas expander. evaluating the flows of reversible work in and out of each component. Those for the power plant are representative of combined cycle technology. After reaching convergence.193.I.Fig.21͔. The performances estimated by the model are for design conditions. etc. see http://www. Table 3 summarizes the most important assumptions maintained throughout most calculations ͑exceptions are discussed further below͒. each belonging to one of fourteen basic types: pump. Results presented here are therefore applicable to ‘‘greenfield’’ construction. included in our code. combustor. which is calculated by ASPEN Plus ͓23͔ based on the Peng-Robinson model ͓24͔. heat exchanger. which conform to S. tables ͓22͔ and the highly concentrated CO2 . with negligible efficiency penalties. the actual values are calculated by our code based on similarity parameters.cfm . Redistribution subject to ASME license or copyright. The energy balance of components with reactive flows is solved together with the equations that warrant chemical equilibrium ͑if required͒ and 528 Õ Vol.org/terms/Terms_Use.asme. compressor. Thermodynamic properties are calculated according to the JANAF tables ͓20.e.234. turbine. Gas turbine cooling flows are calculated based on TIT. the code can perform a full 2nd-law analysis. the maximum allowTransactions of the ASME Downloaded 24 Jul 2008 to 131. JULY 2006 the conservation of atomic species.192. handled by the CO2 compression and drying system. it is assumed that all plant components have been specifically designed ‘‘from scratch’’ to operate at the conditions reached upon convergence. i. The polytropic efficiencies of gas turbine compressor and expander reported in the table are the asymptotic values reached without scale effects. chemical reactors ͓18͔. 4 Calculation Model and Assumptions Heat and mass balances of the integrated CLC-CC plants have been estimated by a computer code originally developed to assess the performance of gas/steam cycles for power production ͓12– 15͔ and later extended to handle gasification of coal and biomass ͓16͔. unconventional fuels ͓17͔. except for water and steam. steam cycle. Basic characteristics and mass/energy balances of each component are calculated sequentially and iteratively until the conditions at all interconnections converge toward stable values. As for the evaporation pressures of the steam cycle. Chemical equilibria are calculated by a model originally developed by Reynolds ͓25͔. smaller heat transfer areas for heat recovery due to higher gas density͒. smaller CO2 compressor. they have been varied with the outlet temperature of the gas turbine to maximize electric efficiency. The system of interest is defined as an ensemble of components. 128.

subcooling ⌬T HRSG Pressure Levels Condensing pressure HRSG thermal losses Mechanical losses.29͔.7% of thermal input 0. the efficiency of its conversion into electricity is lower than the efficiency of the combined cycle. Ambient Conditions NG supply NG flow rate Approach ⌬ T in NG heater Compressor air leakage Compressor polytropic efficiency Turbine polytropic efficiency Max T of turbine nozzles/blades Approach. because inert materials provide a means to store thermal energy. our predictions tend to underestimate both power output ͑because we do not considered the contribution of the CO2 going through the gas turbine expander͒ and CO2 emissions. Excess oxygen in reduction reactor Inert mass fraction in circulating solids Stage compr ratio of CO2 compressor Compressor stage isentropic efficiency Temperature at intercooler outlet Mechanical/electric efficiency Liquid CO2 to disposal 15°C.14. valves. Steam conditions at the inlet of the HP and MP steam turbine ͑see points 12 and 13͒ are moderate due to the low temperature at the outlet of the gas turbine ͑443°C. unless one goes to very high inert fractions. i. by isothermally expanding it to its atmospheric partial pressure of about 35 Pa. With more inert the temperature of the flow exiting the reduction reactor ͑point 9 in Fig. not only because specific production is low ͑due to the low carbon intensity of NG͒.org/terms/Terms_Use. This effect however is minimal. About half of the mass flow discharged by the reduction reactor ͑see difference between points 9 and 10͒ is removed as condensed water. 1 atm 60% RH 15°C.Table 3 Main assumptions adopted for calculating the performances of the integrated CLC-CC systems. the reader must consider that efficiency is net of the power for CO2 compression.e. 2͒ increases. Since such heat goes only through the steam cycle. Varying the inert fraction causes significant effects on the temperatures across the reactors. actual values have been optimized depending on GT outlet temperature. JULY 2006.26͔. Figure 5 shows that the major irreversibilities take place in the reactors and the steam cycle. 20 bar 10 kg/s ͑476 MWt͒ 20°C 0. reactors. ϱ ϭ 0.asme. implies that the gas turbine changes with TIT and ␤. gas turbine power output is slightly higher than 50% of total net Journal of Engineering for Gas Turbines and Power output—significantly less than in conventional. excess oxygen. etc. thus. According to Johansson et al. In practice one would proceed differently because.234. Obviously. it is more likely that one would tailor the CLC to an existing gas turbine.8% of inlet flow rate ␩ pc.193. and that they all decrease when the maximum temperature increases. Vol. The rest is provided by burning natural gas in a supplementary combustor placed between the exit of the oxidation reactor and the gas turbine expander. which is then compressed to 85 bar ͑point 11͒.e. heat losses will have to be verified based on the design and the operating experience of actual plants. but especially because CLC makes available CO2 at the relatively high pressure of the reduction reactor ͑8 –12 bar͒. see http://www. 2. referring to a given machine makes no sense.3%/0.5% pressure drop across the CLC system includes all losses from compressor discharge to gas turbine inlet: ducts. 128 Õ 529 Downloaded 24 Jul 2008 to 131.93 830°C/800°C 25/10/10°C 3 bar/20 bar/110 bar͑*͒ 0. i. Table 4 gives the breakdown of the power output and power consumption ͑also for the fired systems discussed in the next paragraph͒. i. 6 Results for Fired Systems In the ‘‘fired’’ system. „*… Maximum values. in a parametric analysis aimed at assessing the influence of basic parameters like TIT and ␤. CO2 compression accounts only for few percent of gross power output. and a larger fraction of the fuel heating value ends up as heat recovered in the pressurized boiler between points 9 and 10 of Fig. At the low TIT considered for these unfired systems. then such exergy should not be considered a loss.5% ␧ϭ10% ␬ϭ50% Х2 85% 30°C 96%/96% 30°C. Nonetheless. Figure 5 shows the results of the 2nd-Law analysis. rather than tailoring the gas turbine to a given CLC system. 85 bar Fig. The top portion of the stacked bars is the exergy of the liquid CO2 made available at 85 bar. the calculated gas expansion path and a number of parameters interpreting state-ofthe-art cooling technology ͓13.CLC . As typical of all gas turbine cycles and combined cycles. the difference being the oxygen captured in the oxidation reactor ͑compare points 2 and 3ϭ4͒.7% thermal input chemical equilibrium 7. Its value is significant because it includes the work ⌬ Exmix generated by reversibly mixing CO2 into the atmosphere ͓28. ϱ ϭ 0. Maintaining the same NG input for all calculations. The assumptions adopted for the CLC island are reasonable guesses based on the experience of Enitecnologie and a preliminary assessment of CLC technology.90 ␩ tc.cfm . ͓27͔. CLC provides only a fraction of the input to the thermodynamic cycle. a minor fraction ͑about 2%͒ of the CO2 generated in the reduction reactor leaks to the oxidation reactors.e.. 5 Results for Unfired Systems Figure 3 shows net electric efficiency vs specific power output ͑referred to the mass flow of air entering the gas turbine compressor͒ for three T max. If CO2 capture is among the objectives one wishes to achieve with the integrated CLC-CC plant.CLCϭ 850°C. Notice that the large 7. ⌬ Exmix accounts for about two thirds of the exergy of CO2 . 3 Efficiency vs specific work of unfired systems able metal temperatures reported in the table. To appreciate properly the values in the diagram. leaving about 2. but a useful outcome. the pressure ratio yielding maximum efficiency increases with TIT. and keeping a constant NG input appears the most sensible choice. specific features like pressure drops. At the lowest value of 850°C. pinch. NG-fired CC. Redistribution subject to ASME license or copyright.192. 2 for T max.5% 99% 0. Figure 4 shows the sensitivity to the fraction of inert material circulating in the beds together with the metal oxides. The issues related to the use of commercial gas turbines are discussed in Sec. cyclones. see point 5͒. The mass flow across the gas turbine expander is smaller than that discharged by the compressor.05 bar 0. the same power of the CLC island. it refers to the net output of a NG-fired system with zero CO2 emissions. 7.6 kg of ϳ97% pure CO2 per kg of NG.3%/0. when the inert fraction increases the efficiency of the whole system decreases. the gas turbine is uncooled. Table 5 gives the detail of the operating conditions at the points marked in Fig. Since this leakage has not been considered here. compressor/GT/ST Generator efficiency Thermal loss of CLC reactors Composition at reactors outlet CLC pressure loss.

4 Ϫ3.5 467.76 18. p in bar.7 14.3 7.76 260 Fig.17 30 3ϭ4 665.5 Table 5 Thermodynamic conditions at points shown in Fig.4 279.6 ␤ϭ14 218.58 14. T SFÄ1200°C. ␤ϭ16 1 M p T 987.1 52.4 787.cfm . T SFϭ 1200°C. 6 Comparison between the heat rate and the CO2 emissions of fired CLC-CC systems with those of unfired CLC-CCs „point ‘‘U’’… and those of conventional NG-fired CC „point ‘‘C’’….9 Ϫ3.84 260 Fired-T max.33 30 4 866.5 8 277. 5 Second-law losses for unfired cycles Fig.33 78. the temperature at the outlet of the reduction reactor is 850°C.7 447. see http://www.19 14.0 467.2 1.9 Ϫ3.4 417.56 85 30 5 669. In all cases.1 45.2 7 10 16.CLC or T SF°C GT compression ratio Power Output.CLCÄ850°C.193.8 Ϫ3.3 – 467. JULY 2006 Transactions of the ASME Downloaded 24 Jul 2008 to 131.48 303.2 1.01 107.1 14.4 108.7 391. 4 Sensitivity to the mass fraction of inert material in the solids circulating in the reactors Fig.19 7.CLCÄ850°C.1 103.2 9 47.4 14 31.03 443. MWLHV Suppl.03 537.Table 4 Power outputs and net efficiency for unfired and fired CLC systems at optimum gas turbine compression ratio.0 – – 2 702.5 1. 2 for unfired plant with T max.8 365.2 12 95. T max.8 ␤ϭ16 270.56 505.61 7.4 7 10 8.4 2 894.9 6 669.asme.3 135. MWe Gas Turbine Steam Turbine CO2 Compressor Auxiliaries Net Power Output NG input. g/kWhe 850 950 1050 1000 Fired 1100 1200 ␤ϭ8 111.5 10 26.5 224.9 9 47.6 – 467. ␤ϭ8 1 M p T 712. Unfired T max.56 85 30 5 950. For all fired CLC systems.65 1.3 Ϫ4.9 0 ␤ϭ10 159.7 1.1 50.8 303.81 Ϫ4. % CO2 emission.9 Ϫ4.37 16.64 2.1 43. ␤Ä14 m in kgÕs.1 259.org/terms/Terms_Use.4 214. ␤Ä8 and fired plant with T max.01 15 8 M p T 0.6 6 950.7 1.2 0 ␤ϭ10 118.9 0 ␤ϭ12 122.6 Ϫ4.192.9 186 Ϫ3.9 16 406.1 1.5 136. 530 Õ Vol.CLCϭ 850°C.7 94.8 3 857.1 98. T in °C Unfired-T max.2 13 72.5 12 55.6 13 121. firing CLC system Net Efficiency.1 47. 128.3 Ϫ4.5 Ϫ5.8 850 10 26.01 15 8 M p T 8.2 467.2 175.2 14 28.4 509.234. Redistribution subject to ASME license or copyright.25 142.2 287.8 787.3 Ϫ3.3 201.2 413.1 47.3 155.53 18.CLCÄ850°C.0 – 467. A generation system comprising unfired CLC-CCs and conventional CCs would lie on the line connecting points C and U.CLCϭ 850°C.4 850 11 26.25 108.36 1200 11 26.01 97.

The ensuing increase of efficiency and power output must be weighed against the CO2 emissions generated by the fuel burnt in the supplementary combustor. Given the outcome of the analysis illustrated in the previous chapters. 6͒.2’’ by Siemens͒. Therefore: m in.asme. Instead. actual implementations of CLC will have to resort to commercial gas turbine designed for conventional. 7 Net efficiency and CO2 emission vs specific work of fired CLC-CC systems. R the gas constant. the large engines introduced in the 1980s and upgraded in the early 90s ͑‘‘E’’ technology by General Electric. i. because the molecular weight of air is slightly higher than the weighted average of CO2 and H2 O generated by the combustion of NG. 6͒ and a NG-fired.CLCÄ 850°C This supplementary combustor allows de-coupling the maximum temperature of CLC from the maximum temperature of the thermodynamic cycle. For T SFϭ 1200°C..cfm . T 0 and p 0 the total temperature and pressure at turbine inlet. conventional CC ͑point ‘‘C’’ in Fig. From the technological point of view. as well as efficiency and CO2 emissions. In all cases. T decreases. because in CLC there is no fuel addition and part of the oxygen is given up in the oxidation reactor. the fired CLC-CC plant reaches a net efficiency of 52% with CO2 emissions about one half of conventional NG-fired CC. ‘‘. When a gas turbine designed for NG-fired operation is fed by a CLC system. Fig.234. for the same pressure ratio ␤. ␤. the temperature at the outlet of the oxidation reactor is 850°C. the fired system can be considered as a linear combination of an unfired CLC-CC plant ͑point ‘‘U’’ in Fig.193. about 7 percentage more than a state-of-the-art combined cycle. its pressure ratio would decrease to compensate the lower mass flow through the turbine. ␤ϭ14͒. i. Since such cooling has not been considered in our calculations. Redistribution subject to ASME license or copyright. Figure 6 show that this is not the case and that fired cycle do make thermodynamic sense. TIT and thus T 0 are lower. Table 4 gives the breakdown of power outputs. Vol. T • ͱR • T 0 / ͑ p 0 • A ͒ where m in. The point representing its heat rate and CO2 emissions will lie on the line connecting points ‘‘U’’ and ‘‘C’’ in Fig. because the optimum cycle parameters of integrated CLC-CC plants are not too far from those of commercial ‘‘second generation’’ heavyduty machines.Fig. To understand the turbine behavior under CLC conditions. see http://www. more specifically at a position determined by the ratio between the combustion power ( m fuel* LHV) of CLC and the total combustion power. Being fed with an oxidizer at high temperature ͑in our case vitiated air at 850°C͒ such combustor would be subject to critical cooling issues. it is likely that some cooling fluid ͑air from compressor discharge or steam bled from the steam turbine͒ will have to be used. The losses of CLC and the exergy of the CO2 captured decrease when supplementary firing increases because their absolute value stays constant. Figure 8 reports the breakdown of 2nd-Law losses. ␤ϭ8 with the fired case with the same T max. the gas turbine expander typically operates in ‘‘choked’’ conditions.CLCϭ 850°C. because a combination of unfired CLCCCs and conventional CCs could generate power with the same CO2 emissions but higher efficiency—or with the same efficiency but lower CO2 emissions. mass flows͒ of an integrated CLC-CC plant.T is the flow at the turbine inlet. In order to warrant adequate operating conditions to the liner and the other components exposed to the hot gas. A an equivalent flow cross section.1 MWe at the exJournal of Engineering for Gas Turbines and Power pense of 391 MWLHV of NG. 7 Use of Commercial Gas Turbines Unless CLC becomes the technology of choice for power generation. Figure 7 shows net electric efficiency and CO2 emissions vs specific power output for systems with increasing supplementary firing temperature and constant maximum CLC temperature of 850°C. at constant reduced mass flow. thus fully exploiting the capabilities of gas turbine technology independently of the constraints posed by CLC.192. 8 Second-law losses for fired cycles with T max. 6.org/terms/Terms_Use. NG-fired CC. This implies a ‘‘marginal efficiency’’ of 63%. Table 5 gives the details of the operating conditions ͑also for T SFϭ 1200. T SFϭ 1200 and ␤ϭ14: supplementary firing increases net power output by 447. 128 Õ 531 Downloaded 24 Jul 2008 to 131.e. TIT. it is unlikely that manufacturers will ever offer a gas turbine designed to operate at the optimum conditions ͑␤. the operating conditions of the gas turbine ͑TIT. Should the point representative of the fired system lie above line C–U. The turbine reduced mass flow G ͑a nondimensional quantity͒ is defined as: G ϭ m in. The improvement brought about by supplementary firing can be appreciated by comparing the unfired case with T max.7–201. p 0 is lower JULY 2006.6ϭ246. R is slightly lower.e. TOT͒ and of the steam cycle ͑evaporation pressures. In fact. With this regard. superheat and reheat temperatures͒ can be kept much closer to those adopted in conventional CCs.CLC . a fired cycle adds to the issues of CLC the challenge of the supplementary combustor. one can assume that the compressor air flow is the same of the NG-fired engine ͑the compressor operates at the same speed and with similar ␤͒. With supplementary firing. while NG input increases. using such ‘‘conventional’’ gas turbine should not imply great handicaps. our predictions for fired cycles may be somewhat optimistic. The optimum pressure ratio increases from about 8 for the unfired plant to about 16 for the plant with T SFϭ 1200°C. then the fired system would make no thermodynamic sense.

6 139.8 264. kg/s TOT. MWe Net efficiency.0 146. On the other hand. the V94. To exemplify the application of CLC with existing.3 25. these machines have been modeled to reproduce the performance quoted by the manufacturer ͓30͔. same hardware͒.6 130. it is possible to develop preliminary comparative estimates that can give a sense of the conditions under which CLC can be competitive with other low-CO2 emission technologies. because the exTable 7 Reference plants for economic analysis NG-fired Unfired CC SC-CA PO-CA CLC Net power output. Investment costs are summarized in Table 9.3 43. 4.1 625 41..Table 6 Performance and cost „1 EuroÄ1.5 145. while the fired plant is the one with T SFϭ 1100°C and ␤ϭ14. m2 Turbine outlet flow.5 171.3. MWe ST output.cfm . 7͒. analyzed in ͓18͔.4 190. For plants other than CLC.10 237.7 30. 128.4 20. the last two rows of Table 6 show that the derating ͑i. 34 MC ញ for the fired plant. 3..7 532 Õ Vol.CLCϭ 850°C and TSFϭ 1200°C.47 233.8 404. For the CLC island we have assumed a cost of 42 MC ញ for the unfired plant. PO-CA refers to the plant with Partial Oxidation and Chemical Absorption of CO2 from synthesis fuel.2 Natural gas GT inlet air flow. 3 and 7: V94. 3͒. T . The overall picture emerging from Table 6 indicates that there should be no major technical issue preventing the use of existing heavy-duty machines in CLC-CC plants.2 132. The lower cost of the fired plant accounts for the lower volumetric flow to be handled by CLC as a consequence of higher pressure ratio and specific power output. First. discussed in Ref. For fired gas turbines ͑NGCC. kg/s CO2 emission. Other assumptions relevant to cost evaluation are listed in Table 8: we have considered a relatively high natural gas cost to conform to midterm projections. V94.6 131.2 132.asme. commercial gas turbines we have considered two large heavy-duty machines offered by Siemens.44 9. respectively.8 our predictions because the pressure loss across the CLC system ͑we have assumed 7.3 121.3 10.63 10. Nonetheless.2 157.94 25.4 24. An additional 5% for contingencies was added for non-mature technologies.9 427. the base specific cost is 475 and 125 ញ C /kWe. % GT output.4 77.192.5 35.1 0.e. 2.7 34. i. JULY 2006 Downloaded 24 Jul 2008 to 131. SC-CA refers to a Semi-Closed cycle with Chemical Absorption of CO2 from enriched flue gases. The former typically prevails and thus ␤ must decrease to maintain the same value of G ͑the actual variation depends on the specific situation͒.5 GTW 2003 CLC fired 508.8 13.9 our predictions 519. Redistribution subject to ASME license or copyright.3 155. kg/s TIT.CLCϭ 850°C.4 177.1 1105 847 11.org/terms/Terms_Use. to avoid discrepancies coming from different scales. together with the resulting Cost of Electricity ͑COE͒ and the cost of avoided CO2 . perience gained so far is just at the laboratory scale ͓9. which increases by about 30% for the fired cycle and more than doubles for the unfired cycle.9 11.6 197.18͔.193. a value giving performance very similar to those at optimum pressure ratio ͑Fig. °C Turbine inlet pressure bar Turbine cooling flow. all but NGCC. adapted to an exchange rate 1.9 157. MC ញ C /kW Specific Cost.378 0.CLCϭ 850°C. MW Net LHV efficiency.5 1245 1178 13.6 18.1 537.0 48.SC-CA. the decrease of p 0 gives an opposite effect. These figures were evaluated after preliminary estimations and must simply be regarded as an educated guess based on the authors’ experience. While the decrease of m in. with some variation to account for modified market conditions and some additional assumption specific to CLC plants: 1.99 20.e.2 480.0 2. Investment costs have been estimated by the methodology described in ͓6͔.8 13.2 decreases its pressure ratio from 11.7 403.1 GTW 2003 CLC unfired Siemens V94. which feature cycle parameters not too far from the optima shown in Figs. % 1st nozzle cross section.8 13.8 519.2A… Siemens V94.4 898.11͔. with a 20% reduction for unfired systems to account for the absence of the combustor and the downsizing of the electric generator. Transactions of the ASME 8 Economic Estimates and Comparison With Other Low-CO2 Emission Technologies Whether CLC will actually play a role in the mitigation of the greenhouse problem will ultimately depend on the cost of the CO2 it can deliver for long-term storage.09 226.56 12.. somewhat higher than that in Table 6 to account for is 160 ញ turn-key installation and auxiliaries.2A Natural gas 519. At the current stage of CLC development. °C Net power output.0 34. R and T 0 tends to decrease G. kg/s Compression ratio Turbine inlet flow.6 394. see http://www.e. For CLC applications the cost is made specific to the air flow ͑i.54 8.8 – – – – – – 584. MWe Air flow rate. lower power output following reduced TIT and smaller turbine mass flow͒ causes a large increase in the gas turbine specific cost ͑ញ C /kW͒. the V94.430 518. % Total Cost.2 USD… of the gas turbines considered for integration in unfired CLC „Siemens V94.6 625 35. The CLC plants considered for the economic assessment are sized to a power output of about 400 MWe.7 477.31 463.1 50.6 20. with a scale factor of 2/3 with respect to a base 380 MW NGCC plant. ញ Source 508.CLCϭ 850°C and ␤ϭ8.2 ϳ0 Fired CLC 365.2 498.8 625 356 331. Their performance are taken from Table 4: the unfired CLC plant is the one with T max.PO-CA͒ specific cost C /kWe. costs are obviously very uncertain.0 35.6 51.234.2 for the unfired cycle with T max.95 0.9 508. For the steam section and the balance of plant ͑including cost of engineering and contingencies͒.3 – – – – – – 537.430 0. ͓6͔.4 583.3 1424.0 190.2 USD/euro.2 25.2 56. we assumed the same cost of the additional hardware given in previous works ͓6.17 222. in the fired cycle with T max.378 531.3 to 10. showing that: in the unfired cycle with T max. the same model has been used to predict the performances of the integrated CLC-CC plant.9 565.2A for the fired cycle with T SFϭ 1200°C. Then.5% in Table 3͒ is higher than the 2%–3% typical of heavy-duty gas turbine combustors.2 456. which is very close to the optimum for fired CLC ͑Fig.2… and in fired CLC „Siemens V94.25 218. The results are reported in Table 6. same airflow. g/kWh 373.2A maintains its pressure ratio.9 11. Table 7 summarizes the performance assumed for the plants considered for the comparative economic analysis.

38 636.72 2.31 54. The points marked on the lines identify the situation of the plants in Table 8.58 71. On one hand. these economic estimates are subject to great uncertainty and could change significantly once more accurate estimates will be available.45 38. R.78 60. Figure 9 is not very encouraging for CLC.69 185. An important potential exists for unfired CLC systems operating at higher temperatures ͑i.70 2.64 77. MP.192.62 52.38 405. but this consideration crucially depends on the cost of natural gas. A preliminary economic analysis indicates that the cost of CO2 avoided by integrated CLC-CC plants with maximum CLC temperature 850°C is about 50 ញ C /ton for both the fired and unfired Table 9 Investment costs. this compares unfavorably with the cost of alternative technologies like Semi-Closed Cycles or Partial Oxidation with Chemical Absorption ͑35 ញ C /ton͒. Acknowledgment The authors gratefully acknowledge the support of the ENI group for the development of the research presented in this paper. However.59 59. Vol.04 Unfired CLC Fired CLC Nomenclature ϭ ϭ ϭ ϭ T max. The points marked on the lines show the investment cost of low-CO2 plants as depicted by Table 9: if the carbon tax is higher than that corresponding to these points. one must also notice that capital cost estimates are very preliminary. Kurani and D. mainly due to its interesting cycle efficiency. Fig. version. Journal of Engineering for Gas Turbines and Power JULY 2006.00 151.29 61. 9 Specific investment cost of a power plant with CO2 capture that gives the same COE of a NG-fired CC without CO2 capture.99 2. since the working fluid of the thermodynamic cycle—vitiated air—is segregated from the combustion products.35 3. Redistribution subject to ASME license or copyright.04 29. 2002. see equation in Sec. Energy and Environmental Policy Managing Transtions. because the carbon tax needed to make them competitive ͑48 –52 ញ C /ton͒ is higher than that required for the competitiveness of the other technologies. 9 Conclusions Integrated CLC-CC plants offer the potential for generating electricity with near-zero emissions.12 51.asme.19 – 37. 7 Mass flow. see http://www. MJ/kg High/medium/low pressure Heat recovery steam generator Natural gas Oxidation reactor Partial oxidation-chemical absorption Reduction reactor Semi-closed cycle chemical absorption Steam turbine Turbine inlet temperature Turbine outlet temperature Reduced mass flow.0 559.45 2.63 12.34 41.45 3.21 42.6 8. then the plant in Table 9 would be cost-effective with respect to the NG-fired CC without capture.66 83.08 216..55 42. cost of electricity „COE… and cost of avoided CO2 for the same plants listed in Table 7 NG-CC PO-CA SC-CA Gas Turbine MC ញ Steam section MC ញ Power plant BOP MC ញ Other Equipment MC ញ Net Capital Cost MC ញ Specific Cost C /MWh COE investment ញ C /MWh COE o&m ញ C /MWh COE fuel ញ C /MWh COE CO2 storage ញ C /MWh COE Total ញ C /ton Cost of Avoided CO2 ញ 38.CLC ϭ T SF ϭ ␤ ϭ G m p T Acronyms CC COE GT HHV. bar Temperature.06 48.11 32.78 3.14 34.09 50. Fired CLC is not much better than the unfired cycle.234. kg/s Pressure. edited by K.52 216. LP HRSG NG OR PO-CA RR SC-CA ST TIT TOT ϭ ϭ ϭ ϭ ϭ ϭ ϭ ϭ ϭ ϭ ϭ ϭ ϭ ϭ Combined cycle Cost of electricity Gas turbine Higher/lower heating value..e. °C Maximum temperature of CLC Temperature of supplementary firing. calling for a relatively low carbon tax ͑30 ញ C /ton͒.7 13. °C Gas turbine pressure ratio 69.98 52.69 2. ‘‘Toward Zero Emissions for Trasnportation Using Fossil Fuels.54 58. 128 Õ 533 Downloaded 24 Jul 2008 to 131.79 11. and that the picture given in Fig. over 1000°C͒.cfm . S.Table 8 General assumptions for cost evaluations Discount rate Inflation rate Operating plant life Mortgage plan duration Revenues tax rate Capital charge rate Capacity factor Annual insurance cost and O&M Natural gas cost Cost of storage of CO2 10%/yr 2%/yr 25 years 20 years 40% 14.02 66.31 37.47 550.1 592. provided that their technical feasibility can be demonstrated by further R&D developments. 9 we have reported the specific investment cost that could make low-CO2 emission technologies competitive with NG-fired CC without CO2 capture as a function of a carbon tax.29 32.’’ in VIII Biennal Asilomar Conference on Transportation. on the other. Fired configurations where temperature is raised from 850 to 1200°C by supplementary firing can achieve 52% net efficiency with CO2 emission about one-half of those of a modern combined cycle. Considering that such a solution would be much simpler to develop. the opposite is true if the carbon tax is lower. the potential of CLC systems should not be underestimated.35 34. Unfired configurations with maximum process temperature 850–1050°C can reach net efficiencies ranging 43%– 48%. LHV HP. Nonetheless.193.00 33. 9 may change significantly once more accurate estimates will be available.10 References ͓1͔ Williams.46 0 40.91%/yr 7000 h/yr 3% of plant cost C /GJ 4.64 56.64 52.88 256.58 31.org/terms/Terms_Use. H.93 0. operate and maintain than PO-CA and SC-CA ͑once the critical design issues of the CLC island are solved͒ and that it would benefit of the virtual absence of NOx and CO emission.90 4.3 11. in Fig.44 46. 9 shows that an unfired system reaching 1050°C would represent the winning solution. Fig.50 ញ 10 ញ C /ton Given the high uncertainties in the estimates of investment cost.

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