Applied Energy 231 (2018) 1179–1190

Contents lists available at ScienceDirect

Applied Energy
journal homepage: www.elsevier.com/locate/apenergy

Design and techno-economic optimization of a rotary chemical looping T

combustion power plant with CO2 capture
⁎
Chukwunwike O. Iloeje , Zhenlong Zhao, Ahmed F. Ghoniem
Massachusetts Institute of Technology, Department of Mechanical Engineering, 77 Massachusetts Avenue, Cambridge, MA 02139, United States

H I GH L IG H T S

• Techno-economic optimization of a rotary chemical looping power plant is presented.

• The optimization model captures and exploits reactor-system feedback effects.
• Optimizing an economic objective function identified lower cost solutions.
• Scaling and technology maturity projections suggest commercial viability.

A R T I C LE I N FO A B S T R A C T

Keywords: The rotary chemical looping combustion reactor design - which utilizes oxygen carriers in a matrix of micro
Carbon capture channels for indirect fuel conversion - provides a viable path for fossil-based electric power generation with CO2
Chemical looping combustion capture. Its thermally integrated matrix of micro channels minimizes irreversibilities associated with heat
Rotary reactor transfer in the reactor, and establishes multiscale coupling between oxygen carrier kinetics, reactor geometry
Power plant optimization
and plant operating conditions. In this study, we implement an optimization framework that exploits this
Techno-economics
Energy system modeling
multiscale coupling for simultaneous reactor design and power plant economic optimization. Results for the
methane-fueled power plant reveal optimized thermal efficiencies of 54–56% for a rotary chemical looping
recuperative Brayton cycle plant, with compressor pressure ratio in the 3–7 range. By switching from an effi-
ciency to an economic objective, we identified solutions that reduced electricity cost by about 11%; by per-
forming scaling and technology maturity projections, we show competitive economics for the rotary chemical
looping plant with CO2 capture.

1. Introduction
Carbon capture technologies are important for decoupling energy
use from CO2 emissions [1], but face efficiency penalties and extra
separation costs due to CO2 separation. Among a variety of potential
CO2 capture options, chemical looping combustion technology is widely
recognized as a promising, low-penalty solution, thanks to its efficient
CO2 separation process [2–4]. At the core of chemical looping tech-
nology is an oxygen carrier material, which transfers oxygen and
thermal energy between an oxidizer and a fuel stream [5] (Fig. 1a),
thereby eliminating the energy penalty associated with exhaust CO2
separation [3]. Oxygen carrier materials for chemical looping com-
bustion include metals like nickel, copper and iron, as well as a number
of hybrid materials [2,6–14]. The choice of oxygen carrier is often a
tradeoff between favorable material properties and cost.
Significant progress has been made in developing the circulating
fluid bed chemical looping reactor design, which cyclically oxidizes and
reduces the circulating oxygen carrier in corresponding oxidation and
reduction reactors [4,15]. Yet it faces some challenges with maintaining
particle circulation at high temperatures and pressures, particle attri-
tion and entrainment [15–17]; the temperature swing in systems with
endothermic reduction reaction increases reactor irreversibilities cre-
ated by the temperature gradient between each reactor and the in-
coming circulating particles, which penalizes thermal efficiency
[18,19]. The rotary chemical looping reactor design provides an alter-
native path to addressing these challenges by replacing the circulating
particles with an oxygen carrier-coated microchannel matrix, and by
taking advantage of the high degree of thermal coupling between these
channels to minimize redox temperature swings. A rotating drum
houses the channel wall matrix, each composed of a dense substrate
layer supporting a porous oxygen carrier layer. The dense layer forms a
continuous conduction path that enables efficient heat transfer to

⁎
Corresponding author.
E-mail address: nwike@mit.edu (C.O. Iloeje).

https://doi.org/10.1016/j.apenergy.2018.09.058
Received 24 February 2018; Received in revised form 17 April 2018; Accepted 6 September 2018
0306-2619/ © 2018 Elsevier Ltd. All rights reserved.
C.O. Iloeje et al. Applied Energy 231 (2018) 1179–1190

Fig. 1. Chemical looping combustion schematic diagram representing: (a) generic chemical looping combustion concept (b) Rotary chemical looping reactor drum
showing inlet sectors (c) Rotary chemical looping reactor drum showing outlet zones.

maintain thermal equilibrium in the reactor [6,20]. Both ends of the MWthermal ∝ (N ∗D 2 ∗L) (1)
rotating drum connect respectively to a fixed, four-sector inlet chamber
Here, MWthermal is the total thermal power capacity of the plant, D is
and a fixed, two-zone exit chamber (Fig. 1b and c). As the drum rotates,
the reactor diameter, N refers to the number of reactors and L is the
the air and fuel streams in the corresponding sectors respectively oxi-
reactor length. The three right-hand-side variables in Eq. (1) represent
dize and reduce the oxygen carrier on the channel walls, creating se-
three degrees of freedom at the designer’s disposal for determining the
parate CO2-rich and N2-rich exhaust. The purge sectors use steam to
plant layout. Assuming a fixed reactor length, doubling the thermal
ensure CO2 separation.
power capacity of the rotary plant could entail using two reactors or a
The development of the rotary chemical looping reactor is geared
single reactor with Dnew = D 2 . Fig. 2 illustrates the former option, a
towards integration in energy conversion systems, with significant in-
modular design that facilitates operational flexibility. However, the
terest in electric power applications. A number of studies have per-
optimal design must take into account the specific technology appli-
formed system-level analysis for chemical looping plants, including
cation, space constraints, economic considerations and technical chal-
fundamental thermodynamic studies [5,21,22], modeling and perfor-
lenges inherent in each choice. In summary, the rotary chemical
mance evaluation of specific plant designs [23–26], and techno-eco-
looping plant necessitates a rearrangement of the power island, given
nomic analysis [27–33], with emphasis on circulating reactor designs
the geometric differences between the rotary reactor and a conven-
for applications ranging from electricity production to fuel reforming.
tional combustor.
Here, we focus on the rotary chemical looping reactor design, and il-
This study presents a rotary chemical looping (recuperative Brayton
lustrate its application in power generation using a recuperative
cycle) plant for efficient, carbon neutral electricity generation, using a
Brayton cycle power plant configuration, whose concept layout is
modeling framework that represents the integrated system as an as-
shown in Fig. 2. Although the layout in Fig. 2 represents only one of
sembly of coupled interactions. The heterogeneous redox reactions in
several possible configurations, it highlights the key differences be-
the reactor microchannel matrix create a strong coupling between the
tween the rotary chemical looping plant and a conventional power
oxygen carrier reaction kinetics and the reactor geometry. This in turn
plant design.
influences the reactor thermal balance, which affects steam demand,
Firstly, chemical looping creates separate streams as the fuel is
system stream flows and recuperative heat exchanger balance. This
oxidized, and oxygen from air is absorbed on the metal such that, de-
cascade of interrelated effects propagate across scales to determine the
pending on the plant design, it might require a pair of turbines, com-
thermal efficiency and economics of the overall plant. Thus, by re-
pressors and heat exchangers for each stream. Secondly, the rotary
taining finite rate surface kinetics and internal heat transfer within the
reactor lends itself to a modular design, with unique implications for
reactor, this framework captures important feedback interactions be-
scaling, as illustrated in Eq. (1).
tween reactor-scale and system-scale phenomena, which improves

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Fig. 2. A rotary chemical looping (recuperative Brayton cycle) plant concept.

modeling predictions. We take advantage of this ability to represent key

feedback interactions between oxygen carrier properties and overall
system behavior to perform a techno-economic optimization of a nickel-
based, rotary chemical looping plant, and analyze its operational fea-
tures.

2. Method

To model the rotary chemical looping power plant at a resolution

that sufficiently captures the effect of coupled interactions inherent in
the integrated system, we adopt an equation oriented flowsheet mod-
eling strategy [34,35], which transforms the thermodynamic relations
that describe each system component into a system of linear and non-
linear constraints that define the feasible space for optimizing a thermal
efficiency or economic objective function. This equation oriented for-
mulation is illustrated in Fig. 3, where x is the vector of process vari-
ables, f (x ) is the objective function, and H (x ) and G (x ) are the math-
ematical formulations for the component models, expressed as sets of
equality and inequality constraints.

2.1. Objective function

We consider two objective functions for this problem: thermal ef-

ficiency and the levelized cost of electricity. Optimizing thermal effi-
ciency addresses the performance barrier to technology adoption, while
optimizing the levelized cost of electricity addresses the economic
hurdle. Also, by accounting for the operating costs over the lifetime of Fig. 3. Optimization logic for the rotary chemical looping plant.
the plant, the levelized cost of electricity also indirectly captures the
effect of thermal efficiency via fuel consumption rate. 2.3. Levelized cost of electricity

2.2. Thermal efficiency
Thermal efficiency expresses the ratio of the net-work output of the
plant to the total heat input, as shown in Eq. (2).
∑ Wk
η=
n∗LHV
η is the plant thermal efficiency, Wk represents work output from
component k, where k refers to the set of turbines and compressors,
with W defined as positive for turbines and negative for compressors.
LHV is the lower heating value of the fuel, n is the fuel molar flow rate,
and the denominator represents the total heat input to the system.
Levelized cost of electricity (LCOE) is a measure of the economic
competiveness of a power plant technology, and represents the dis-
counted cost (per MWh) of building and operating the plant over an
assumed financial life [36]. The levelized electricity cost estimation
strategy in this study follows a bottom-up approach, described in the
NETL cost-estimation guidelines [37]. First, we estimate the capital cost
(2)
of individual equipment. Then we incorporate relevant factors and
parameters to determine, in sequence, the bare erected cost, the en-
gineering, procurement and construction costs, the total plant cost, and
finally, the total overnight cost. This total overnight cost is then used to
compute the levelized cost of electricity.

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Table 1
Equipment capital cost fitting parameters.
Equipment i Ak = 1 Ak = 2 Ak = 3 βk = 1 βk = 2 βk = 3 M Source

Rotary reactor – – 2.398E6 – – 0 $/module See supplemental material (Section A)

Air and gas-side compressors 1.098E5 – – 0.2133 – – KWNet [38]
CO2 pump 1.110E6 – 7.0E4 – – 0 MWCO2 [39]
Air and gas-side turbine 7.778E3 – – 0.7035 – – KWNet [38]
Recuperator (steam section) 1.454E-4 5.125 1.237E3 2 1 0 ΔHsteam [40]
Recuperator (air/gas section) 1.509E1 – 2.847E3 1 – 0 ΔHgas [40]

2.4. Capital equipment cost Table 3

Bare erected cost parameters.
The total capital equipment cost for the key components of the ro- Category, m Am βm
tary chemical looping plant takes the general form expressed in Eq. (3).
Piping 0.003596 1.149
Ci = (∏ f j, i ) ∑ Ak, i (M ) βk, i Electrical installations 0.0009276 1.173
j k (3) Instrumentation and control 0.02446 0.9903
Civil and structural 0.03604 1.067
Ci is the capital cost for component i , f j, i are cost factors that modify the Balance of plant 0.1111 0.978
base cost to correct for effects like material selection or inflation
(Table 2), Ak, i and βi are power-law coefficients derived from fitting
cost data (Table 1), and M is the fit variable for the different cost which are lumped in the factor, Fcontractor in Eq. (6).
correlations: power output for compressors, pumps and turbines, and
plant
heat duty for recuperators (Table 1). These parameters are summarized CEPCC = Fcontractor CBEC (6)
in Tables 1 and 2. The reactor base cost was determined from a com-
Total plant cost (TPC): This adjusts the EPCC cost to accommodate
bination of material cost data, vendor data for honeycomb regenerators
process and project contingencies, as shown in Eq. (7).
and an estimate of fabrication energy costs (supplemental material,
Section A). The turbine and compressor base cost parameters were CTPC = CEPCC (1 + Fprocess + Fproject ) (7)
determined by fitting cost data obtained from Pauschert et al. [38]
while those for the CO2 pump were estimated using the cost correlation Total overnight capital cost (TOCC): This adjusts the total plant
from McCollum et al. [39]. For the recuperators, we worked around the cost to include other pre-production costs, inventory capital costs and
challenge of finding publicly available cost data for high temperature, other owners’ costs, as shown in Eq. (8).
multiphase, multi-stream heat exchangers by considering the cost of
CTOCC = CTPC (1 + Fpreprod + Finventory + FOtherOwners ) (8)
separate heat exchanger units for gas-preheating and steam generation.
The relevant cost data were generated using Aspen Economic Analyzer®
Having determined the total overnight capital cost, we evaluate the
[40], and we fitted cost curves to this data as a function of heat duty.
cost of electricity (COE), which is defined as the revenue per net MWh
After computing the individual equipment costs, we sum them to obtain
for the first year, assuming an escalation rate equivalent to the general
the total capital cost, as shown in Eq. (4).
inflation rate over the life of the plant [37] (Eq. (9)).
Ccapital = ∑ Ci op
(FCC CTOCC ) + C fixed op
+ (FCap Cvar )
i (4) COE =
Bare erected cost (BEC): This accounts for all the major con-
FCap ( )(
Days
Year
Hours
Day ) MWnet
(9)
struction costs associated with piping, electrical installations, in- op
strumentation & control, civil & structural installations, and general FCC is the capital charge factor; are the fixed and variable
C fixed , op
Cvar
facilities (balance of plant). The BEC correlation is defined in Eq. (5). operating costs, and FCap is the plant capacity factor. The denominator
is the effective net megawatt-hour of energy generated in one year. The
CBEC = ∑ Am (Ccapital ) βm levelized cost of electricity (LCOE) is then obtained using Eq. (10).
m (5)
plant
LCOE = (COE )(FL) (10)
CBEC is the bare erected cost for the plant, Am and βm are fit parameters
for construction cost category, m , based on data from Pauschert et al. FL is the levelization factor, an algebraic function of the levelization
[38], as described in Table 3. period, discount rate and inflation rate. Table 4 summarizes the cost
Engineering, procurement and construction costs (EPCC): EPCC estimation parameters discussed in this section. See the supplemental
accounts for the costs of services provided for detailed engineering material (Section B) for additional cost model formulation details and
design, project execution, permitting costs and other contractor costs, the complete set of cost estimation parameters.

Table 2
Equipment cost factors.
Equipment i f j=1 f j=2 f j=3 f j=4 Source
Cost index Material Size Contingency

Rotary reactor – – – 1.33 See supplemental material (Section A)

Air and fuel-side compressors 220/169 (2016/2008) 1/2.86 (air/fuel-side) – – [41,42]
CO2 pump 220/159.9 (2016/2005) – – – [41]
Air and fuel-side turbine 220/169 (2016/2008) – 0.7 – [41,43]
Recuperator (steam section) – 1.67/2.86 (air/fuel-side) – – [42]
Recuperator (gas section) – 1/2.86 (air/fuel-side) – – [42]

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Table 4 reactor model developed in an earlier study [44], the recuperator with a
Cost estimation parameter values. multi-stream heat exchanger model for both gas preheating and steam
Parameter Symbol Unit Value generation, and each turbine and compressor unit with an enthalpy
balance model that incorporates a specified isentropic efficiency.
Base year 2016
Contractor services Fcontractor % of BEC 9
cost
2.6. The rotary reactor
Process contingency Fprocess % of EPCC 55a
Project contingency Fproject % of EPCC 25
Pre-production factor Fpreprod % of TPC 2 In an earlier study [44], we described in detail the formulation for a
Inventory capital Finventory % of TPC 0.5 reduced fidelity model of the rotary chemical looping reactor, and va-
Other owners cost FOtherOwners % of TPC 15 lidated it against the detailed rotary reactor model from Zhao et al.
Levelization factor FL See supplemental material [6,45]. This reduced model uses a quasi-steady state approximation of
(Section B) the periodic stationary behavior of the rotary reactor to simplify com-
Fuel cost $/MMBTU 3
putation, and describes the reactor as a set of design constraints that
a
The NETL guidelines recommend about 30–70% process contingency for govern fuel conversion, CO2 separation, reactor energy balance, oxygen
new technologies. Since most of the equipment in this system, are off-the-shelf carrier conservation, and other geometric specifications, as illustrated
components, a process contingency of 55% was applied. in Eq. (11)

2.5. Constraint formulation 1

Fig. 4a shows a high-level schematic diagram of the rotary chemical
looping power plant flow sheet, with short descriptions of sub-models
used for each component, while Fig. 4b sketches the corresponding
temperature-entropy diagram. The path 1-2-3-4-5-6 represents isen-
tropic compression, isobaric pre-heating, isobaric combustion, isen-
tropic expansion and isobaric exhaust heat recovery. The accompanying
labels ‘f’ and ‘a’ denote the fuel and airside streams, and the dotted lines
describe the respective cycle paths when accounting for irreversi-
bilities. We simulate the reactor with the rotary chemical looping
H ⎛θk , uk , l, D , ⎛ ⎞ ⎞ ⩽ 0
⎝ ⎝ ω ⎠⎠ (11)
θk , uk , l, D , ω are the sector sizes, sector feed gas velocities, reactor
channel length, reactor diameter and rotational speed. The subscript, k ,
refers to the fuel, fuel-purge, air and air-purge sectors of the rotary
reactor, and H is the system of linear and nonlinear reactor design
constraints specifications. We present a summary of the key reactor
model constraint specifications here, and refer the reader to the sup-
plemental material (Section C), as well as our previous work [44] for
formulation details and reactor model validation. Eqs. (12)–(16) sum-
marize the reactor model constraints.

Fig. 4. Schematic diagram of the rotary chemical looping (recuperative Brayton cycle) plant showing (a) key sub-components with corresponding model descriptions,
(b) temperature-entropy diagram.

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n
∫0
lreactor
dz ⩾ (1 + κ )
1 ψ (z )
∫ψ (0) ⎛ ψ ⎟⎞ dψ
⎜
ζ ⎝ 1−ψ ⎠ (12)

lreactor dz θ
∫0 uk
⩽ k
ω (13)
−1 −1
⎛ dX ⎞ ⎛ θfuel ⎞ ⩽ ⎛ dX ⎞
⎜ ⎟ ⎛ θair ⎞
⎝ dt ⎠reduction ⎝ ω ⎠ ⎝ dt ⎠oxidation ⎝ ω ⎠ (14)

∑ nk (uin,k ) hk̂ (Tin,k )− ∑ nz hẑ (Tad) = 0 (15)

∑ θi = 1 (16)
Eq. (12) describes the fuel conversion criterion, which ensures that
the reactor channel length is sufficient for target fuel conversion. Here κ
is an adjustable safety factor, ψ (z ) is a measure of the extent of fuel
conversion at channel length z , ζ is a function of the fuel conversion
kinetics, which depends on pressure, channel surface to volume ratio,
oxygen carrier layer thickness, fuel fraction and reactor temperature
[44]. Eq. (13) describes the carbon separation criteria, which prevents
carry-over between the fuel and air sectors by requiring that the
channel residence time in each purge sector be longer than the effective
gas residence time in the respective individual channels. Eq. (14) spe- Fig. 6. Implementation procedure.
cifies the oxygen carrier conservation requirement, which ensures that
for cyclic stationary operation, the amount of oxygen carrier oxidized in satisfy the 1st law of thermodynamics, while the pinch balance (Eq.
the air sector should balance that reduced in the fuel sector. Here, X is (18)) enforces a minimum temperature difference between the hot and
the fractional oxygen carrier conversion and the inequality accom- cold streams in the exchanger unit, thus avoiding a violation of the 2nd
modates some oxygen carrier conversion in the fuel purge sector. Eq. law.
(15) is the energy balance criterion and ensures zero net enthalpy
∑ Fi (Tiin−Tiout ) + ∑ Fj (T in out
j −T j ) = 0
change of the reactor streams. Here, h^ (T ) expresses enthalpy as a i ∈ Hot j ∈ Cold (17)
function of temperature, subscript z represents the reactor exit fuel and
air zones, and Tad is the adiabatic reactor exit temperature. This energy ∑ Fi (max(0, ΔT jout )−max(0, ΔT in ∑ Fj (max(0, ΔTiin )
j ))−
balance effectively controls air supply flow rate for reactor temperature i ∈ Cold i ∈ Hot
regulation. Finally, the geometric consistency requirement in Eq. (16)
−max(0, ΔTiout )) ⩽ ε (18)
ensures that the fractional sector sizes sum up to unity.
Here, ε is a conditioning tolerance factor, F is the thermal capacity
2.7. The recuperator rate of hot/cold streams (i/ j ) , Ti , Tj are the hot and cold heat integration
sub-streams, ΔTj = Tj−[T p−ΔTmin], ΔTi = Ti−T p , p ⊂ P̄ , and P̄ is the set
The demand for purge steam in the rotary reactor requires steam of pinch point candidates whose temperatures are defined as the set of
generation, which takes place in the recuperators. Since this heat ex- heat integration inlet streams, i.e., T p = [{Tiin}, {T in
j + ΔTmin}]. The pinch
changer also preheats the inlet gas streams, each recuperator unit is criterion in Eq. (18) enforces a minimum temperature difference (ΔTmin )
modeled as a multiphase, multi-stream heat exchanger using a modified between the hot and cold streams. Further discussion on the im-
implementation of the Duran-Grossman model [46]. plementation of this recuperator model have been included in the
As illustrated in Fig. 5, this model transforms the heat exchanger supplemental material (Section D).
process streams into a set of heat integration streams corresponding to
each phase transition. This transformed scheme is then used to for- 2.8. Turbines and compressors
mulate energy balance and pinch balance relations for the hot and cold
streams. The energy balance (Eq. (17)) ensures that enthalpy changes For steady state, adiabatic operation, energy conservation for a

Fig. 5. Integrated multi-stream heat exchanger model accounting for streams capable of phase change. The two physical process streams are transformed into four
heat integration streams.

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Fig. 7. Optimized rotary chemical looping (recuperative Brayton cycle) flow sheet results at the reference case conditions.

applied to account for irreversibilities in a real turbine:

Power plant performance
20 h (Tin )−h (Tout ) Tin−Tout
ή isen = =
MW

15 h (Tin )−h ̂(Tout

̂ ) ̂
Tin−Tout (21)
10
Similarly, for the compressor,
5
T^out = Tin π^
α
0 (22)
-5
-10 h (Tin )−h^ (Tout ) T −T^
Air-side Air-side Fuel-side Fuel-side CO2 Net ή isen = = in out
h (Tin )−h (Tout ) Tin−Tout (23)
compressor Turbine compressor Turbine compressor
The compressor model accommodates the flexibility of choosing
Fig. 8. Breakdown of contributions to net power output. The air-side con- multistage compression with intercooling, with the inter-stage pressure
tribution dominates because of the larger air-side flowrates, determined by ratio for an n-staged compressor defined as
oxidation and temperature control requirements in the reactor.
1
πi ̂ = π n̂ (24)
Table 5
Reactor Geometry at the optimized reference case.
2.9. CO2 pump
Fuel sector size 16π
25
Fuel-purge sector size 2π CO2 gas is first compressed to its critical pressure, and then pumped
25 up to the supercritical transport pipeline pressure. The compression
Air sector size 30π
25 phase is as described in Eqs. (19)–(24), while the pumping phase is
Air-purge sector size 2π modelled using the correlation by McCollum et al. [39].
25
Reactor length (m) 1.0
Reactor diameter (m) 4.6
ṁ in ⎛ ΔP ⎞
Wp = ⎜ p ⎟
ρCO2 ⎝ ή isen ⎠ (25)

control volume defined around the turbine or compressor gives: Here, ṁ in is the mass flow rate in kg/s; ρCO2 is the average density of
supercritical CO2 in kg/m3; ή isen
p
is the pump isentropic efficiency and
W + nh ̇ ^ (Tout , x~) = 0
̇ ^ (Tin, x~)−nh (19) ΔP is the pump pressure change in Pascal.

W is the turbine or compressor work input, ṅ is the molar flow rate, h ̂ is 2.10. Implementation
the specific molar enthalpy, x ̃ refers to component mole fractions. For
an ideal, isentropic turbine, To implement this model, we formulated the two objective func-
̂ = Tin π|̂ −α
Tout (20) tions, and the component models, as described in Eqs. (2)–(25). Then
cp
we collated the component models into a single set of constraints,
−1
Pin generated a random set of initial values and solved the resulting
Here π ̂ =
cv
Pout
is the turbine pressure ratio, α = cp , cp, c v are re-
cv
equation oriented optimization problem. These steps are illustrated in
spectively the specific heat capacity at constant pressure and volume, Fig. 6. We developed the model in Matlab®, used both thermal effi-
̂ is the isentropic outlet temperature. An isentropic efficiency, ή isen , is
Tout ciency and levelized cost of electricity as objective functions, and

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Fig. 9. Cycle efficiency vs compressor pressure ratio: (a) The predicted efficiency profile agrees with the expected inverse relationship for the Brayton cycle, with a
peak value at pressure ratio = 4. (b) The spread highlights favorable cycle efficiencies values over this range of pressure ratios.

bounds.

3. Results & discussion

3.1. Efficiency optimization

Fig. 10. Rotary chemical looping plant economics: the turbines account for
about 50% of the total cost, followed by the rotary reactor at 20%, with the
remaining fraction split between the compressor units and the recuperator
modules.
implemented the optimization using the non-linear constrained mini-
mization solver’s SQP algorithm [47]. We modelled a single reactor of
25 MW thermal capacity, with a nickel-based oxygen carrier whose
properties were obtained from Zhao et al. [20]. The CO2 compression
unit delivers supercritical CO2 at 110 bars and 303 K to an external CO2
pipeline. The reference case system and reactor-level design specifica-
tions are included in the supplemental material (Section E). Thermal
properties were computed from NIST correlations [48] and IAPWS IF97
standards [49]. Since the optimal solution is not unique, we ran the
model from a randomized set of initial points within pre-defined
The flow sheet in Fig. 7 shows simulation results for the nickel-
based rotary chemical looping (recuperative Brayton cycle) plant, op-
timized for efficiency at the reference compressor pressure ratio of 5.
The predicted thermodynamic states, compositions and flow rates of the
process streams appear in bold font. Notice that the recuperators pro-
vide high temperature streams to the reactor, which reduce reactor
temperature gradients and speed up kinetics [50]. Fig. 8 summarizes
the cycle performance results for this nickel-based rotary chemical
looping plant. The breakdown of contributions to the net power output
show that the air-side turbine and compressor account for about 85% of
the respective gross output and input power, with CO2 compression
amounting to about 3% of net power output.
Since the reactor design is integrated with system-level optimiza-
tion, the model also simultaneously predicts corresponding reactor
geometry, as well as operating parameters like channel flows and ro-
tating speed that ensure carbon separation and complete fuel conver-
sion. Table 5 shows a sample prediction for the reactor geometry at the
reference case solution.
In Fig. 9a, the optimal thermal efficiency values is plotted over a
range of pressure ratios, and has a value of about 55% at the reference
condition. The efficiency profile peaked at a pressure ratio of 4, and

Fig. 11. Optimizing levelized cost of electricity vs efficiency. (a) Predicted efficiencies are similar because levelized electricity cost captures the contribution from
plant efficiency via required fuel consumption. (b) The average capital equipment cost predicted by optimizing the levelized cost of electricity is lower than that by
optimizing efficiency because, optimizing an economic objective discriminates in favor of lower cost solutions. (c) This in turn improves the levelized cost of
electricity for the plant.

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Fig. 12. Pressure ratio parametric plots. These Figures illustrate how the coupling between reactor kinetics, geometry, and thermal integration determine the
relationship between operating conditions and plant-level techno-economic performance.

Fig. 13. Effect of technology (recuperator pinch) and economic (gas price) factors on the levelized cost of electricity: (a) Changes in recuperator effectiveness
significantly impacts efficiency and levelized cost of electricity. (b) Gas price is also an important determinant of the economic outlook for the rotary chemical
looping plant.

decreased monotonously with increasing pressure, in line with the in-
verse relationship between efficiency and pressure ratio for the Brayton
cycle. The actual pressure ratio at which maximum efficiency occurs
depends on a number of additional factors, including the effectiveness
of heat recovery and the purge steam demand, which, in turn, is a
function of the prevailing conditions in the reactor [44]. We see from
the spread in Fig. 9b that the rotary chemical looping plant maintains a
high efficiency over a reasonably wide range of compressor pressure
ratios. This high efficiency is due, in large part, to the high degree of
thermal integration in the rotary reactor; thermal integration minimizes
temperature gradients between the fuel and air zones, which leads to
higher efficiencies for most cycle configurations [18,19]. Similarly high
efficiencies for a thermally integrated recuperative Brayton chemical
looping plant was reported by Ishida et al. [51], albeit with a more
complex flow sheet heat-integration strategy involving solid-gas heat
exchangers between the air-side and fuel-side reactors. The advantage
here is that the rotary reactor keeps reactor heat integration simple by
avoiding external gas-solid heat exchangers.
Fig. 10 breaks down the capital equipment cost for the reference
case rotary chemical looping plant. The reactor accounts for about 20%
of the total capital cost, with 50% for the turbine, and the rest dis-
tributed between the compressor units and the recuperator modules.
Given that the reactor amounts to a significant portion of the capital
equipment cost, we have an incentive to use an objective function that
incorporates a cost minimization criteria.
3.2. Economic optimization
The surface-dependent reactions in the rotary chemical looping re-
actor couple kinetics with geometry, which in turn defines equipment
size and cost. This makes it more appropriate to optimize an economic
indicator, like the levelized cost of electricity, instead of efficiency.
Moreover, the reactor configuration at optimal efficiency is not unique,
as several combinations of reactor parameters-with different economic

1187
C.O. Iloeje et al.
Fig. 14. Quantifying the effective cost of CO2 capture: Additional equipment
(50%) and technology uncertainty (50%) account for the electricity cost dif-
ference between the no-capture Brayton cycle plant and the rotary chemical
looping Brayton cycle plant.
footprints-can achieve the same thermal efficiency objective. Thus, by
introducing an incentive for minimizing costs, optimizing the levelized
cost of electricity leads to more economical plant specifications.
Fig. 11 compares predictions for sample optimization runs, with
efficiency and levelized cost of electricity as the respective objective
functions. As shown in Fig. 11a, both optimization objectives predict
similar thermal efficiencies. However, we see a reduction of about 14%
in the average capital equipment cost (Fig. 11b), and about 11% in the
levelized cost of electricity (Fig. 11c). This drop in the predicted capital
equipment and electricity costs results primarily from gains in reactor
size reduction. This reduction is achieved by finding an improved
combination of reactor length-to-diameter ratios, sector channel velo-
cities and rotating speed for the same reactor thermal capacity rate
[44].
In Fig. 12, we use a pressure ratio parametric plot to illustrate how
this integrated model captures the relationship between rotary reactor
behavior and overall system economics. In the rotary reactor, operating
pressure typically inhibits fuel conversion rate– due to the saturation of
oxygen carrier surface sites as gas concentration increases [50,52].
Slower kinetics mean larger reactors (Fig. 12a), which generally in-
creases reactor costs (Fig. 12b). Larger reactors also mean higher purge
steam demand, but its net contribution to cost is a trade-off between its
effect on reactor thermal integration, on recuperator thermal balance,
Fig. 15. Economic projections for the rotary chemical looping plant. (a) With technology maturity, levelized cost of electricity for the rotary chemical looping plant
drops from about 30% to 15% above a no-capture plant, demonstrating potential as a competitive technology option. (b) The combined effect of plant scale-up and
technology maturity leads to very competitive electricity prices for the rotary chemical looping plant.
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Applied Energy 231 (2018) 1179–1190
and on overall system flow rates. Higher purge steam demand increases
the steam generation load on the recuperator. As pressure ratio in-
creases - and the turbine exhaust temperature drops -, the recuperator
heat recovery dips, leading to lower reactor inlet temperatures, slower
kinetics and larger reactors. However, lower reactor feed temperatures
also reduce the air flow rate required for temperature regulation in the
reactor, which in turn reduces the required sizes of other air-side
equipment, and subsequently, their capital costs. The net effect of this is
shown in Fig. 12c. This relationship between reactor feed temperature
and required air flow also helps explain the results at pressure ratio of 3
in Fig. 12a and b, both of which deviate from the trend at higher
pressures. At this pressure ratio, the hotter turbine exhaust streams
entering the recuperator create higher temperature reactor inlet
streams. As a consequence, the reactor size increases to accommodate
the increase in air flow rate now required for temperature regulation.
The profile of the levelized cost of electricity in Fig. 12d arises from
a tradeoff between these feedback effects, coupled with the contribu-
tion from the corresponding thermal efficiency values. In summary,
economic optimization selects for optimal combinations of system and
reactor parameters that flexibly adapt to changes induced by varying
operating conditions, in a manner that minimizes cost. This is of par-
ticular benefit to developing cost effective rotary chemical looping
plant designs, given the complex nature of these coupled interactions.
3.3. Effect of recuperator effectiveness and gas prices
The relatively high thermal efficiency achieved by the rotary che-
mical looping plant derives, in part, from the effectiveness of exhaust
heat recovery in the recuperator. The recuperator effectiveness depends
on the design pinch ΔT, and, as shown in Fig. 13a, the plant thermal
efficiency is very sensitive to this value, dropping by 2% for every 10-
degree increase in ΔT, which corresponds to an equivalent increase in
levelized cost of electricity of 1.5% for the same ΔT change. Thus a 20 K
increase in recuperator pinch increases electricity cost by about $3/
MWh. This indicative analysis underscores the importance of designing
cost effective, high temperature recuperators that meet tighter pinch
specifications. Another important factor is the gas price, which was set
at $3/MMBTU for this study. In the last 5 years, US monthly average
national gas prices has varied between $1.8/MM and $5/MMBTU, and
the effect of this price uncertainty is captured in Fig. 13b. We see, from
this Figure, a 5% change in electricity cost for a corresponding 20%
change in gas price, corresponding to an equivalent cost variation of
about $4/MWh.
C.O. Iloeje et al.
3.4. Technology maturity and scaling projections
A primary objective of optimizing the design of the rotary chemical
looping power plant technology is to achieve electricity costs that are
competitive with other capture technologies. To better assess the po-
tential of the rotary chemical looping plant, we put the results pre-
sented so far in this context, and show how technology maturity and
power plant scaling could improve the economics of this technology.
Fig. 14 compares the levelized cost of electricity for the nickel-based,
rotary chemical looping plant with that of a conventional Brayton cycle
plant (with no CO2 capture and no steam injection), both modelled with
the same specifications. The no-capture electricity cost is about 27%
lower than that for the rotary plant. The changes in capital equipment
requirements between the two account for about 50% of this difference.
The remaining 50% has to do with the respective technology maturity
levels, applied as process contingency penalty in estimating the leve-
lized cost of electricity [37].
The case can be made that most components of the rotary plant are
off-the-shelf technologies, which creates a pathway for downscaling the
uncertainty cost applied in the economic assumptions. Thus, with in-
creasing rotary chemical looping technology experience, the levelized
cost of electricity could drop by a further 15% to about $76/MWh, 16%
above the conventional plant (Fig. 15a). Another important cost driver
is scale, which further improves the economic outlook for the rotary
chemical looping plant. To capture the effect of scale, we assume that
the cost of the overall plant scales as that of the turbine, which is the
dominant cost item. This scaling law is represented in Eq. (26), where
n = 0.7215 was determined from data by Pauschert et al. [38]
n
Sizenew (MW ) ⎞
Costnew ("$") = Costref ("$") ∗ ⎛⎜ ⎟
⎝ Sizeref (MW ) ⎠ (26)
Fig. 15b presents the projected combined effect of scaling and
technology maturity on the levelized cost of electricity for the rotary
plant. Increasing the net power plant capacity from 13 MW to 85 MW
led to a 30% reduction in electricity cost to approximately $63/MWh. A
further 15% drop is projected as the plant moves up the technology
maturity scale, giving a projected electricity cost of about $55/MWh. A
number of studies in literature have evaluated the economics of com-
mercial scale CO2 capture plants for chemical looping, integrated ga-
sification and post-combustion capture technologies, based on the
natural gas combined cycle (NGCC) configuration [27–33]. The pro-
jected electricity cost for these plants range from $63/MWh to $107/
MWh while that for a conventional NGCC plant with no CO2 capture is
about $54/MWh. Thus, even accounting for 20–30% capital cost esti-
mation error generally expected this type of scaling projection, the
economics of the rotary chemical looping plant falls in a window that
makes it a competitive option for sustainable electricity generation.
4. Conclusion
A diversified portfolio of carbon capture-enabled energy conversion
technologies can support the sustainable utilization of global fossil-
based resources, but energy and economic penalties integral to CO2
capture limit their widespread adoption. Chemical looping technology -
which eliminates CO2 separation costs - reduces these barriers. But most
chemical looping combustion reactor designs face operational chal-
lenges associated with circulating oxygen carrier particles. In this study,
we presented the rotary chemical looping design for power generation,
whose thermally integrated reactor micro-channels eliminate the pro-
blems of circulating oxygen carrier particles, and ensure thermal
equilibrium in the reactor. The feedback interactions between reactor-
scale and system-level behavior enabled the application of optimization
to improve plant economics, and consequently, commercial viability.
Since plant performance and economics depend on oxygen carrier
properties, an important next-step for this study will be to compare
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Applied Energy 231 (2018) 1179–1190
different oxygen carrier materials and establish a techno-economic as-
sessment criteria for oxygen carrier selection. Future studies will also
explore pilot operation to more accurately characterize the thermal
performance, kinetic behavior, and long-term stability of the rotary
reactor.
Author contributions
C.O.I designed the study, developed the simulation models, per-
formed the analysis and wrote the manuscript. Z.Z. contributed to the
simulation models and reviewed the manuscript. A.F.G directed the
project and reviewed the manuscript. All authors participated in the
discussion of the results.
Acknowledgements
This study was financially supported by a grant from the Masdar
Institute of Science and Technology and the King Abdullah University
of Science and Technology (KAUST) Investigator Award.
Declaration of interests
There are no conflicts to declare.
Appendix A. Supplementary material
Supplementary data associated with this article can be found, in the
online version, at https://doi.org/10.1016/j.apenergy.2018.09.058.
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