Performance Model for Evaluating Chemical Looping Combustion

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A performance model for evaluating chemical looping combustion (CLC) processes for CO2 capture at gas-fired power plants Hari Chandan Mantripragada, and Edward S. Rubin Energy Fuels, Just Accepted Manuscript • DOI: 10.1021/acs.energyfuels.5b02441 • Publication Date (Web): 05 Feb 2016 Downloaded from http://pubs.acs.org on February 14, 2016

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A performance model for evaluating chemical looping combustion (CLC) processes for CO2 capture at gas-fired power plants Hari C. Mantripragada*† and Edward S. Rubin† † Department of Engineering and Public Policy, BH 129, 5000 Forbes Ave, Carnegie Mellon University, Pittsburgh, PA 15213, USA. KEYWORDS. Chemical looping combustion (CLC); oxygen carrier; performance models; natural gas combined cycle (NGCC).

ABSTRACT.

Chemical looping combustion (CLC) is an indirect combustion process in which a carbonaceous fuel is combusted without direct contact with air. Rather, transfer of oxygen between air and fuel takes place with the aid of an oxygen-carrier (OC) material, yielding a CO2 stream of very high purity. This is attractive for CO2-capture applications since it does not require additional energy to separate CO2 from N2, as in post-combustion CO2 capture processes. In this paper, a mass and energy balance model is developed to estimate the performance of a CLC system using different OC materials. To simplify the calculations, the specific heats of all gases and solids are assumed 1 ACS Paragon Plus Environment

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to be constant over the range of temperatures considered. The model is then applied to evaluate the effect on system performance of several design and operating parameters using three different OC materials. Given input conditions such as fuel, reactor operating temperature, fuel and OC material, the model calculates the amount of OC required and the resulting temperature and system flow rates. The model can be applied to any gaseous fuel containing CH4, CO and H2. The CLC model, coupled with a plant-level systems model, was used to evaluate the performance of a conceptual CLC-based natural gas combined cycle (NGCC) power plant, using three different OC materials. Two configurations were studied for each case: (1) the LP-HRSG case where the flue gases from the fuel reactor are first expanded in an expander and then sent to a CO2 compressor after condensing the water vapor; and (2) the HP-HRSG case, where the flue gases are cooled at high pressure and the CO2 compressed after condensing the water vapor. In general, the CLC-NGCC plant power output and efficiency (>50%, on HHV basis) are comparable or higher than that of the conventional NGCC power plant without CCS, whose net plant efficiency is close to 50% (HHV). The LP-HRSG configuration had higher net power output (about 10 MW) and net plant efficiency (around 2% points) than the HP-HRSG configuration. Among the three OC materials, Ni-OC systems gave slightly better performance than the Fe-OC and Cu-OC systems. Considering that CO2 capture is inherent in CLC-NGCC plants, CLC appears to be a highly competitive CO2 capture technology, at least in terms of overall plant performance.

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Nomenclature A

Cross-sectional area of reactors (m2)

Cp,i

Specific heat of species ‘i' (kJ/kmol-K)

∆Hf,i

Standard heat of formation of species ‘i' (kJ/kmol)

∆Hrxn,298.15,i

Heat of reaction at 298.15K (kJ/kmol)

Mi

Molar flow rate of species ‘i' (kmol/s)

Me

Reduced form of metal oxide

MeO

Oxidized form of metal oxide

MWi

Molecular weight of species ‘i' (kg/kmol)

P

Pressure (bar)

T

Temperature (oC)

ai

Stoichiometric coefficient of reactant

bi

Stoichiometric coefficient of product

eair

Molar excess air ratio

erich

Rich O2-loading

elean

Lean O2-loading

∆e

Fractional conversion of OC

k1 , k2

Average equilibrium constants

minventory

Solids inventory (kg)

xMeO

Weight fraction of MeO in the OC


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1. INTRODUCTION Carbon dioxide capture and storage (CCS) has been widely recognized as a potentially important technology for controlling CO2 emissions from fossil fuel power plants1,2. The three main approaches to CO2 capture are post-combustion, pre-combustion and oxy-combustion, in which CO2 is separated from N2, H2 and H2O, respectively. Most CO2 capture technologies available today result in large energy penalties that significantly reduce the net power plant efficiency and increase the plant cost3. Current research and development programs are thus keenly focused on new capture options with smaller energy penalties and lower overall cost. This paper focuses on chemical looping combustion (CLC), an indirect combustion process in which fuel is combusted without direct contact with air4,5. Instead, transfer of oxygen between air and fuel takes place with the aid of an oxygen-carrier (OC) material. The oxygen-carrier extracts O2 from air in an air reactor (AR) and transfers it to fuel in a fuel reactor (FR). Since the fuel does not come in direct contact with air, the products of combustion contain only carbon dioxide (CO2) and water vapor (H2O). CO2 stream of very high purity can then be obtained by condensing the water vapor. This is attractive for CO2-capture applications since it does not require additional energy or chemical processing to separate CO2 from N2 or H2, as is the case of a post- or pre-combustion CO2 capture processes. Thus, there is a significant scope for CLC to be a competitive CO2 capture technology in these applications. A schematic of the CLC process is shown in Figure 1. Oxygen carriers are usually oxides of transient metals (Co, Cd, Cu, Fe, Mn and Ni). CuO/Cu, Fe2O3/Fe3O4 and NiO/Ni are the most commonly studied OC materials for CO2 capture6. Cu- and Fe-based materials are widely available and much less costly than Ni-based materials. Both Fe- and Ni-based OCs can be operated at high temperatures (around 1100oC). On the other hand, the melting point of Cu is 4 ACS Paragon Plus Environment

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relatively low (1085oC), which precludes it from being used in high-temperature applications6. Ni-compounds are also known to have adverse health effects7, requiring special care in design to prevent any releases and ensure safe as well as reliable operation. Thus, these three materials have their relative advantages and disadvantages, which will affect final system costs (not in the scope of this paper). The reduction and oxidation reactions can be represented as shown in reactions R1 and R2 below, where MekOl and MeyOx are the reduced and oxidized forms of metals, respectively: afuelMeyOx + fuel CO2 + H2O + bfuelMekOl

(R1)

MekOl + aO2O2 bO2MeyOx

(R2)

where, afuel, bfuel, aO2 and bO2 are the stoichiometric coefficients of reactants and products of each reaction. The stoichiometric coefficients for different reactions and other relevant properties of metals are shown in Table 1. For simplicity, the reduced form of OC is represented as ‘Me’ and the oxidized form as ‘MeO’ hereafter in this paper. CLC has received considerable attention in recent years, with research covering the development and testing of oxygen carriers (especially Cu, Fe, Ni and Mn-based OCs), conceptual process designs, experimental evaluation and applicability to different kinds of fuels8-11. In addition, some innovative and novel OC materials have also been studied12,13. One of the first applications envisioned for CLC was for the combustion of natural gas in order to improve the combustion efficiency5. The research then developed into the application of CLC to different gaseous fuels including CH4, CO, H2 and syngas, as well as solid fuels including coal and biomass4,14,15. In one pathway, solid fuels are first converted to syngas which then is combusted through a CLC process16-18.


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N2, O2

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CO2, H2O MexOy

Air Reactor

Fuel Reactor MexOy-1

Air (N2, O2)

Fuel (CnH2m)

Figure 1. Chemical looping combustion process. Oxygen carrier is oxidized in the air reactor and reduced in the fuel reactor.

The biggest gas-based CLC system to be experimentally tested is a 120 kW experimental reactor at the Vienna University of Technology24. Alternatively, there are lab-scale and small pilot-scale experiments using solid fuels such as coal directly in a CLC system25-27. Non-combustion based applications of chemical looping include chemical looping reforming (CLR), chemical looping oxygen uncoupling (CLOU) and chemical looping gasification14,28,29. A number of experimental and conceptual studies16,24,31-33 use interconnected fluidized bed reactors for CLC systems. The air reactor is usually a high velocity riser and the fuel reactor is a bubbling fluidized bed design. High velocity is preferred for air reactors since the volumetric flow rate of air is about 10 times than of the fuel reactor (because of the presence of N2). Thus, without a high velocity the size of the reactor becomes unacceptably large. However, there are still no medium to large-scale pilot facilities to demonstrate CLC processes for different applications.


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Table 1. Stoichiometric Coefficients and Relevant Properties of Metals9,19. Reduction: CH4 / CO / H2 + aiMeO CO2 + 2H2O + biMe Oxidation: Me + aO2O2 bO2MeO MeO/Me NiO/Ni CuO/Cu* Fe2O3/Fe3O4 4 4 12 aCH4 1 1 3 aCO 1 1 3 aH2 4 4 8 bCH4 1 1 2 bCO 1 1 2 bH2 0.5 0.5 0.25 aO2 1 1 1.5 bO2 148.96 (600-800oC) 55.24 51.00 157.76 (800-1000oC) Cp,MeO (kJ/kmol-K) 166.35 (1000-1200oC) 234.65 (600-800oC) 31.90 26.83 257.03 (800-1000oC) Cp.Me (kJ/kmol-K) 279.47 (1000-1200oC) 74.69 79.55 159.69 MWMeO (kg/kmol) 58.69 63.55 231.53 MWMe (kg/kmol) -239,858 -155,719 -824,682 ∆Hf,MeO (kJ/kmol) 0 0 -1,118,918 ∆Hf,Me (kJ/kmol) -179,749 141,735 ∆Hrxn,298.15,CH4 (kJ/kmol) 161,020 -239,858 -622,876 -944,360 ∆Hrxn,298.15,O2 (kJ/kmol) Support material (Al2O3) properties – MWsupport – 101.96 kg/kmol; Cp,support – 134.76 kJ/kmol-K * Some studies20,21 consider a reduction reaction pathway of CuO-Cu2O-Cu for the CuO-CH4 system. In this study, we have assumed a simple CuO-Cu reduction mechanism, as was done in several other studies22,23.

The conceptual designs proposed for capturing CO2 via CLC in power generation applications span a wide range of systems including CLC for natural gas combined cycle power plants, retrofitted coal-based power plants, coal-based direct chemical looping power plants, and integrated gasification combined cycle power plants5,17,33-37. Though most experimental studies deal with atmospheric pressure systems, there is a recognition that pressurized CLC processes


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will lead to cost-effectiveness38,39. High pressure fluidized bed reactors have been tested at different scales around the world, including a 360 MW coal-fired power plant using a highpressure (about 10 atm) CFB boiler that has been in operation since 200140. However, systems using interconnected CFB reactors at high pressure have not seen much progress41. Recently, pressurized fixed bed CLC reactors have been evaluated for methane combustion42,43 and H2 production44. Pressures as high as 20 bar were considered. The choice of reactor technology (fixed or fluidized bed) will eventually depend on their long-term operational success. Among studies involving NGCC designs, the common basis is a combustion chamber replaced with a CLC reactor system. Thermodynamic analyses of several CLC combined cycles fueled by natural gas or syngas found overall efficiencies ranging from 48 – 55% (lower heating value)5,33. Given that CO2 capture is inherent in a CLC process, this efficiency range is much higher than that of conventional power plants with post-combustion CCS, suggesting that CLC may be a more attractive option in terms of performance. 2. OBJECTIVES AND SCOPE OF THIS PAPER To more carefully study the potential of CLC systems, a system performance model is needed for a high-level design of power plant concepts. In this paper, such a model is developed to estimate the performance of a CLC system using different OC materials. The performance model includes mass and energy balance equations for the air and fuel reactors. Combined with previously developed power plant models, these models are used to evaluate CLC-based power plant designs under different design and operating conditions. In the text that follows, the basics of the CLC performance model is first explained in brief. The model is then applied to evaluate alternate CLC designs using three different OC materials. The


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CLC performance model is then combined with an NGCC power plant systems model to evaluate the overall performance of a CLC-based NGCC power plant. Sensitivity analyses are also performed to understand the effect of different design and operating conditions on the performance of the overall power plant. 3. THE CLC PERFORMANCE MODEL The objective of the performance model is to estimate the amounts of material (OC, air, etc) and energy needed to achieve the combustion of a given quantity of fuel under different operating conditions. A performance model, suitable for a spreadsheet environment, is developed here to aid in top-level design of a CLC system. Mathematical models are developed for calculating the mass and energy balance of the air and fuel reactors of a CLC system, based on equilibrium thermodynamics. The specific heats of all gaseous and solid components were found to vary very little over the temperature ranges considered here, hence, they are assumed constant over the range of temperatures considered. Only for Fe3O4 and Fe2O3 for which specific heats vary by more than 10% in the temperature range, different specific heats are used in different temperature intervals, as shown in Table 1. This assumption avoids the need for more complex and time-consuming use of iterative calculations, and gives results that are very close to those obtained in comparisons assuming temperature-dependent specific heats. Thus, the model is well-suited for preliminary evaluation of conceptual process designs. Given input conditions such as fuel composition, operating temperature of the reactors, and OC, the model calculates the amount of oxygen carrier material required and the resulting temperatures and flow rates of different components. The models can be applied to any gaseous fuel containing CH4, CO and H2.


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Previously developed performance models for other major process equipment such as compressors and gas turbines are used for power plant systems studies. Brief descriptions of the CLC process models are given in this section. For each reactor, mass and energy balance equations are solved as functions of process parameters such as solids conversion, inlet gas and solid temperatures, and excess air ratio. 3.1. Mass Balance Equations The overall solids mass balance is governed by the O2-requirement to achieve complete conversion of fuel. The stoichiometric mass flow depends on the specific reaction. For a generic reaction, the stoichiometric flow rate of MeO can be defined as shown in Eqn 1. , = , + , + ,

(1)

The mass balance of the AR can be written as:

,, = , , = , ,

(2)

In the fuel reactor, one mole of fuel consumes stoichiometric amount of MeO. Therefore, for full conversion of fuel, MMeO,consumed,FR = MMeO,stoic

(3)

For mass balance, MeO consumed in the FR is the same as MeO formed in the AR. Hence, MO2,consumed = (aO2/bO2)MMeO,stoic and, ,,! = , , =

"#,$%&'(

(4)

The OC consists of MeO, Me and the support material. The actual flow rate of OC depends on the corresponding mass fractions of these three components. The amount of support material is


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calculated based on a fully oxidized sample of OC. So, support material can be defined as shown in Eqn 5, where xMeO is the mass fraction of MeO in the OC. )) =

+,-."# / ."#

1"#

01

$233&4%

5

(5)

The flowrate of Me depends on the conversion of OC in the two reactors. The higher the conversion in fuel reactor, higher is the fraction of Me at the FR outlet. Likewise, higher the conversion in the air reactor, higher is the fraction of MeO in the AR outlet. With this view, we define rich loading (erich) and lean loading (elean) of O2 (shown in Eqns 6 and 7) as the fractions of MeO at the inlet and outlet of the fuel reactor, which are outlet and inlet of air reactor respectively. 67 =

"#,'8,9:

(6)

6 < =

"#,&2%,9:

(7)

"#,'8,9: ; "#,'8,9:

"#,&2%,9: ; "#,&2%,9:

∆6 = 6 < − 67

(8)

Based on these definitions and the overall solids mass balance equations described before, mass flow rates of all the components at the inlet and outlet of AR can be calculated, as depicted in Table 2. The

overall

mass

flow

of

OC

into

the

air

reactor

can

? , , = , , @ + , , @ + )) @))

be

expressed

as:

(9)

Thus we see that the mass flow rate of OC (MeO+Me+Support) depends on the reaction stoichiometry and also on the conversion of OC in the reactors.


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Table 2. Air Reactor Mass Balance Equations Component Support MeO Me O2 N2

Molar flow into AR (Mi,in,AR)

0

1

6
50%, on HHV basis) are comparable or higher than that of the conventional NGCC power plant without CCS, whose net plant efficiency is close to 50% (HHV). Considering that CO2 capture is inherent in CLC-NGCC plants, CLC appears to be a highly competitive CO2 capture technology, at least in terms of overall overall plant performance. The LP-HRSG configurations had higher net power outputs (about 10MW)


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and net plant efficiencies (around 2% points) compared to the HP-HRSG configurations, indicating that the power generated in the flue gas expander is much higher than that saved from compressing CO2 from a higher pressure to pipeline pressure. Among the three OC cases, Ni-OC systems gave the best performance (power output and net plant efficiency), followed by Fe-OC and then Cu-OC systems, although the differences in net plant efficiency were small. The low TIT (950oC) in the Cu-OC system is the main reason for its lower performance. However, Nibased materials are much costlier than Fe- and Cu-based materials. A cost model is therefore needed to see if the better performance of Ni-OC systems would lead to economic benefits for the overall system. The performance model was also used to conduct sensitivity analyses on key operating parameters. It was found that higher fractional conversion of OC in the reactors was needed for better performance, for all the OC cases. On the other hand, higher fractional conversion would lead to higher solids inventories which could possibly increase the initial capital cost of the system. The net plant efficiency was found to be increase with temperature up to about 1100oC. There was no significant improvement in efficiency beyond 1100oC. Thus, for a CLC-NGCC power plant, Ni- and Fe-based materials, which can withstand higher temperatures, do not have a significant advantage in performance over low-temperature materials based on Cu. Consequently, cost is likely to be of higher significance in choosing OC materials for CLC-based power plants.

AUTHOR INFORMATION Corresponding Author *email: [email protected]; Tel: +1-412-268-5284 31 ACS Paragon Plus Environment

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Performance Model for Evaluating Chemical Looping Combustion

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