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Energy Convers. Mgmt Vol. 39, No. 16±18, pp.

1653±1663, 1998
# 1998 Published by Elsevier Science Ltd. All rights reserved
PII: S0196-8904(98)00078-8 Printed in Great Britain
0196-8904/98 $19.00 + 0.00

COMPARISON OF TWO CO2 REMOVAL OPTIONS IN


COMBINED CYCLE POWER PLANTS

OLAV BOLLAND$ and PHILIPPE MATHIEU%*


$
NTNU, The Norwegian University of Science and Technology, Department of Mechanical
Engineering, 7034 Trondheim, Norway
%
Universite de LieÁge, Institut de MeÂcanique, Rue E. Solvay 21/C3, B4000 LieÁge, Belgium

AbstractÐIn this paper, two concepts of CO2 removal in CC are compared from the performance
point of view. The ®rst concept has been proposed in the framework of the European Joule II pro-
gramme and is based on a semi-closed gas turbine cycle using CO2 as the working ¯uid and a combus-
tion with pure oxygen generated in an air separation unit. This is a zero emission system as the excess
CO2 produced in the combustion process is totally captured without the need of costly and energy con-
suming devices. The second concept calls for a partial recirculation of the ¯ue gas at the exit of the
heat recovery boiler of a CC. The remaining ¯ow is sent to a CO2 scrubber. Ninety percent of the CO2
is removed in an absorber/stripper device. The two systems are compared to a state-of-the-art CC when
the most advanced technology is used, namely a 9FA type gas turbine and a three pressure level and
heat recovery boiler. Our results show also that the CO2 semi-closed CC cycle performances are not
very dependent on the con®guration of the heat recovery boiler and that the recirculated gas CC per-
formances are only slightly sensitive to the recirculation ratio. A high value of this latter mainly gives a
signi®cant reduction of the size and hence of the cost of the CO2 scrubber. From the performance
point of view, the results show that the system eciency with partial recirculation and a CO2 scrubber
is always higher by 2±3% points than the CO2-based CC eciency in comparable conditions. # 1998
Published by Elsevier Science Ltd. All rights reserved

CO2 removal CO2/O2 combustion CO2 semi-closed cycle Flue gas recirculation

NOMENCLATURE

ASU=Air separation unit


CC=Combined cycle
GT=Gas turbine
HRSG=Heat recovery steam generator
MEA=Monoethanolamine
Cp=Speci®c heat (kJ kgÿ1 Kÿ1)
R=Gas constant (kJ kgÿ1 Kÿ1)

SCOPE AND OBJECTIVES


The objective of this study is to assess the impact of CO2 removal and transportation on de-
sign and performance of a natural gas-®red gas turbine plant. Two di€erent concepts were ana-
lysed; one including downstream removal of CO2 from combined cycle power plant ¯ue gas and
one with air separation prior to a CO2-based power cycle with near stoichiometric oxygen com-
bustion. These alternatives are compared to a standard natural gas ®red combined cycle where
no measures are taken in order to reduce the CO2 emissions.
The two mentioned options are considered here for a comparison because the Norwegian and
Belgian research teams under the leaderships of O. Bollard and Ph. Mathieu, developed respect-
ively a modelling of the CC with ¯ue gas partial recirculation and of the semi-closed CO2-based
power cycle.
In the semi-closed cycle option, the big advantage is the 100% extraction of the excess CO2
produced in the combustion process from the CO2 working ¯uid with a simple valve, hence
without an energy consuming and costly device like the MEA scrubber but on the other hand it
requires an ASU. This is a zero CO2 emission concept.

*To whom all correspondence should be addressed.

1653
1654 BOLLAND and MATHIEU: COMPARISON OF TWO CO2 REMOVAL OPTIONS

The asset of the recirculation option is avoiding an ASU but using a well-known CO2 scrub-
ber with a size and cost reduced according to the recirculation rate. However it does not remove
all the excess CO2.
Both authors believe that it is worth comparing fairly the two options and recalculating the
performance of the two systems each on his side with his own model and tools using the same
assumptions and boundary conditions. Finally a cross-check of the results showed a good agree-
ment and provided us with a reliable base for a comparison.
The problem of storing the CO2 is not discussed in the paper, but the underlying idea is to
either dispose CO2 into an empty oil/gas well or use the CO2 as an injection gas in order to
enhance oil recovery.
The combined cycle (gas and steam) is today probably the most competitive type of large-
scale natural gas-®red power plants. The high eciency, low investment costs, improved operat-
ing ¯exibility, short installation time and the low environmental impact are factors which have
made the combined cycle very attractive for both medium and base load power generation as
well as for cogeneration of heat and power. The combined cycle power plant atmospheric dis-
charge of CO2 is low compared to other technologies based on fossil fuels, because of the high
hydrogen/carbon ratio of natural gas and the high cycle eciency.
The recovered CO2 has to be compressed and dried before transportation to the disposal lo-
cation, where the required delivery pressure is assumed to be 150 bar. The two systems call for
a special device requiring its own model, namely the air separation unit (ASU) for the semi-
closed cycle and the CO2 chemical absorber/stripper or MEA scrubber for the CC with ¯ue gas
recirculation.

Air separation unit (ASU)


There exists three main commercial methods for separating air, which are cryogenic separ-
ation, pressure swing absorption (PSA) and liquid membranes. The cryogenic technique is typi-
cally used for medium to very large production rates, the PSA technology is considered
competitive with cryogenic processes for production rates of less than 40 tons per day of high
purity oxygen (>90 %) [18]. For use of oxygen production techniques in conjunction with
power plants, the liquid membrane technique is here considered as not applicable and is there-
fore in the following not further discussed. The PSA technique may also be regarded as giving a
too small production rate for use with power plants, so the only feasible method of producing
oxygen for the power plant scale is cryogenic separation.
The minimum work necessary to separate air can be calculated to approximately 0.06 kWh/
kg O2. In gas separation the actual energy consumption is considerably higher than the ideal,
and it will vary because it depends on the product purities and is a result of an optimisation
between power cost and capital costs. In the present work it is assumed that oxygen is generated
(atmospheric pressure) at 0.25 kWh/kg O2 (or 0.89 MJ/kg O2).

CO2 scrubber
There are three main methods for removal of CO2 from power plant ¯ue gas [10]: amine
scrubbing, cryogenic fractionation and membrane separation, where the amine scrubbing is
reported to be the most cost e€ective process [9]. The CO2 recovery process in the present study
is based on commercially available, specially designed MEA (monoethanolamine) processes
where a recovery plant are the adsorption column, the lean/rich heat exchanger and the stripper
column. The main energy requirement for the process is the stripper column reboiler duty,
which is provided by steam from the power plant. Additionally, energy is required because ¯ue
gas compression is necessary to overcome the system pressure drop. The reboiler thermal con-
sumption is taken as 4 MJ and the electricity consumption as 0.11 MJ per kg captured CO2 [13].
The thermal consumption of 4 MJ/kg gives a steam consumption close to 1.7 kg/kg CO2
removed as reported by Fluor Daniel [17] and Elkem Technology [12], both using MEA addi-
tives (copper containing solution). The further analysis is based on this ®gure for steam con-
sumption
BOLLAND and MATHIEU: COMPARISON OF TWO CO2 REMOVAL OPTIONS 1655

STANDARD COMBINED CYCLE WITH RECIRCULATION OF EXHAUST GAS


The reference combined cycle power plant consists of a large heavy-duty GT (General Electric
9FA) from which the exhaust gas is led to an un®red heat recovery steam generator (HRSG).
Steam is raised at three di€erent pressures with a reheat loop (triple pressure reheat boiler).
Parameters necessary for the calculation of the turbine and for the design of the boilers and
steam turbine, are chosen according to common practice for high eciency combined cycles and
re¯ects proven combined cycle technology. In the case of downstream CO2 recovery (see Fig. 1),
steam (at 3.5 bar, 4 MJ/kg CO2) is bled from the low-pressure steam turbine in order to supply
heat for the stripper reboiler in the CO2 absorption plant. The return condensate from the strip-
per is going to the feedwater tank (FWT). The exhaust gas from the HRSG is cooled down to
258C in a cooler where water vapour is condensed. A fraction of the exhaust gas is recirculated
to the gas turbine compressor.
Recirculation of exhaust gas is a well known compressor anti-icing method and has been
investigated as a measure to reduce GT NOx emissions [1]. When recirculating exhaust gas it is
important to cool the exhaust gas before it is put back into the power cycle in order to maintain
a low temperature of cycle heat rejection and thereby maintaining a high cycle eciency.
Besides, cooling is important because for a given gas turbine the power output is inversely pro-
portional to the compressor inlet temperature. A description of the computational methods is
given in [4, 8].
Recirculation of exhaust gas when using air for the combustion is possible without any major
modi®cation of the combined cycle plant equipment [2].
The reason for recirculating a fraction of the exhaust gas is to reduce the volumetric ¯ow and
increase the concentration of CO2 before the absorption column of the downstream CO2 recov-
ery plant. The amount of recirculation is limited by the combustor. When recirculating exhaust
gas, the gas composition through all the GT components changes. The recirculation ratio is here
de®ned as the fraction of the exhaust gas cooler exit (after condensation of water) that is passed
back to the gas turbine compressor inlet. For the present fuel composition and the selected type
of GT, the maximum recirculation ratio is approximately 0.64. A further increase in recircula-
tion ratio is not possible because there is not enough oxygen in the combustion air, unless that
the ®ring temperature is lowered which will cause a signi®cant reduction in plant eciency. At

Fig. 1. Combined cycle with downstream removal of CO2 from the exhaust gas by absorption.
1656 BOLLAND and MATHIEU: COMPARISON OF TWO CO2 REMOVAL OPTIONS

Table 1. Computational details


Standard combined Combined cycle
cycleÐno removal with recirculationÐ Semi-closed
of CO2 removal of CO2 combined cycle
Gas turbine compressor ¯ow rate kg/s 601 596 100
Compressor inlet molecular weight kg/kmol 28.9 29.0 42.6
Cooling air ¯ow rate kg/s 90 89 16.3
Combustor exit temperature 8C 1319 1319 1319
Turbine exit temperature 8C 597 614 670
HRSG exit steam pressureÐHP bar 105.6 105.6 105.6
HRSG exit steam temperatureÐHP 8C 562 562 562
HRSG steam ¯owÐHP kg/s 73.8 78.4 18.5
HRSG exit steam pressureÐRH bar 25.0 25.0 25.0
HRSG exit steam temperatureÐRH 8C 561 561 561
HRSG steam ¯owÐRH kg/s 78.7 81.6 18.3
HRSG exit steam pressureÐIP bar 25.8 25.8 Ð
HRSG exit steam temperatureÐIP 8C 300 300 Ð
HRSG steam ¯owÐIP kg/s 5.65 4.0 Ð
HRSG exit steam pressureÐLP bar 3.4 3.4 3.4
HRSG exit steam temperatureÐLP 8C 220 220 214
HRSG steam ¯owÐLP kg/s 15.8 12.3 2.1
Steam condenser pressure bar 0.04 0.04 0.04

this maximum recirculation ratio, the gas turbine combustor is operating with a stoichiometric
amount of oxygen. The exhaust gas will nevertheless still contain a certain amount of oxygen,
due to the oxygen content of the turbine cooling air which is bled from the compressor around
the combustor. For the present study, a recirculation ratio of 0.4 was chosen. The reason for
this choice is that a typical gas turbine combustor normally should have a combustion air oxy-
gen concentration of minimum 16±18% [1]. When using a recirculation ratio of 0.4 the exhaust
gas fractions of CO2 and O2 are, respectively, 6.3% and 8.1%, compared to 3.7% and 12.8%
when no recirculation is used. The CO2 concentration is around 10% for a 60% recirculation
ratio, which is actually the design value for the MEA scrubber.
At the inlet of the GT compressor the recirculated exhaust gas is mixed with fresh air before
compression. In order to maintain a high ¯ow rate through the GT the recirculated exhaust gas
is cooled to 258C. The cooling of the exhaust gas may be accomplished in di€erent ways: an
extra tube bundle at the heat recovery steam boiler exit, a packed column or a spray tower. A
packed column was found to be advantageous.
The computational data are in Table 1.

SEMI-CLOSED COMBINED CYCLE FIRED WITH OXYGEN


This concept is based on the combined cycle (Fig. 2) [5±7, 16]. Instead of using air for the
combustion, oxygen is produced in an air separation plant (ASU). The oxygen is fed to the gas
turbine combustor in a near stoichiometric ratio by using an intercooled compressor. To keep
the turbine inlet temperature at a permissible value, exhaust gas (CO2 and H2O) is cooled down
to 258C and recirculated to the compressor, compressed and fed into the combustor. It was
found that the di€erence between a dual- and triple-pressure steam cycle was very small, and it
was chosen to select a dual pressure reheat cycle [14, 15]. The cooling of the turbine is accom-
plished by extracting gas (CO2 and H2O) from the compressor discharge which is fed into the
turbine. The gas turbine deviates from a standard gas turbine mainly due to a di€erent working
¯uid composition (higher molecular weight) and the use of two separate compressor lines feed-
ing the turbine. This concept requires a completely new gas turbine design. However, the tech-
nology level of this gas turbine is assumed to be equal to that of the GE 9FA described
elsewhere in the paper.

DISCUSSION OF THE RESULTS


CC with recirculation
The performance of the combined cycle is depicted in Fig. 3. The removal of CO2 decreases
the eciency approximately by 8% points and the power output is reduced to 86%. The recircu-
BOLLAND and MATHIEU: COMPARISON OF TWO CO2 REMOVAL OPTIONS 1657

Fig. 2. Combined cycle with feed of oxygen from an air separation plant.

lation only slightly increases the eciency and the power output according to Fig. 3, but the
variation is small compared to the uncertainty in component eciencies when recirculating
exhaust gas. The results show that the eciency remains almost constant at 47% and that the
power output increases by less than 2% when the recirculation ratio increases up to 40%. In

Fig. 3. Net plant performance as function of recirculation ratio. The performance of the combined
cycle without removal of CO2 is shown in the upper half of the diagram.
1658 BOLLAND and MATHIEU: COMPARISON OF TWO CO2 REMOVAL OPTIONS

Fig. 4. Exhaust gas composition behind gas turbine and after cooling down to 258C.

Fig. 4 the gas composition is shown as a function of the recirculation ratio. In particular, it can
be observed how the O2 and the CO2 concentrations respectively decrease and increase with this
parameter. The CO2 content in the ¯ue gas on its side increases almost linearly with the recircu-
lation ratio. Note that the concentrations at the CO2 scrubber inlet (continuous lines) are a bit
higher than at the GT exhaust (dotted lines) because of the water extraction in the exhaust
cooler (Fig. 1).
In Table 2 are shown the most signi®cant quantities at the inlet of the CO2 scrubber, namely
the composition, temperatures and throughput of the exhaust gas as well as the steam consump-
tion in the reboiler (for a heat consumption of 4 MJ per CO2 removed or 1.7 kg steam/kg CO2
and a CO2 recovery factor of 90%.
The results show that, when the recirculation ratio goes up to 40%, the exhaust gas mass ¯ow
rate entering the CO2 scrubber decreases down to around 43% of its value without recirculation
whilst the CO2 content increases from 3.7% up to 6.3%. On the other hand, the exhaust gas
temperature and molecular weight change only slightly as well as the bleeding rate from the
steam turbine.

Table 2.
(CO2 capture
without recirculation)
Recirculation ratio (%) 0 10 40 60
CO2 at the turbine exit (kg/s)/% 35.2/3.7 39.4/4.1 59.1/6.3 95.5/10.2
Exhaust gas throughput (kg/s)/% 615.2/100 533.6/86.7 352.2/42.7 234.7/38.2
Exhaust gas temperature (8C) 120.7 119.8 119.1 118.4
Exhaust gas molecular weight (kg/kmol) 28.4 29 29.2 29.5
Steam turbine extraction rate (kg/s) 54.1 54.5 54.5 55.3
BOLLAND and MATHIEU: COMPARISON OF TWO CO2 REMOVAL OPTIONS 1659

Fig. 5. Sensitivity on plant performance from the energy requirement in the stripper column reboiler.

Consequently it clearly appears that the objective of recirculating a part of the ¯ue gas is not
the increase of the performance but rather the decrease of the gas throughput as well as the
increase of the CO2 concentration at the CO2 scrubber inlet. This latter is then operating closer
to its design point so that its size and hence its cost decrease with the treated mass ¯ow rate.
In Fig. 5 the sensitivity on plant performance of the energy requirement in the stripper col-
umn reboiler is shown. In the present work a value of 4000 kJ/kg CO2 removed corresponding
to approximately 1.7 kg steam/kg CO2 removed was selected. Eciency and power output
decrease almost linearly when the heat consumption of the reboiler and consequently the steam
mass ¯ow rate bled from the steam turbine increase.
This shows how interesting it would be to minimise the steam consumption in the reboiler
complying with the constraints of the absorption and stripping processes using MEA. For
example, a reduction of the consumption from 4 to 3 MJ/kg extracted CO2 would give a gain of
2% points eciency and of 2.4% power output. An optimization of the CO2 scrubber inte-
gration into the Rankine cycle is still to be carried out.

Semi-closed CO2/O2-based CC
The optimal CC pressure ratio was found to be approximately 30 based on a sensitivity analy-
sis including both oxygen production and CO2 compression and is depicted in Fig. 6. For a
``classical'' air based gas turbine the ratio R/Cp is about 0.23 while for the CO2 cycle the R/Cp
is approximately 0.15.
This di€erence results in higher exhaust temperatures for the CO2 semi-closed cycle compared
to a standard air gas turbine cycle, and moves the optimal pressure ratio upwards. Most large
industrial gas turbines on the market today have a pressure ratio in the range 10±16, but the
aeroderivative gas turbine RR Trent and LM6000 from General Electric have a pressure ratio
of 30±35.
Approximately 93% of the exhaust gas is recirculated back to the GT compressor whilst the
excess CO2 produced in the combustion process is extracted behind the GT compressor and
1660 BOLLAND and MATHIEU: COMPARISON OF TWO CO2 REMOVAL OPTIONS

feeds to the CO2 compressor. The gas turbine exit temperature is approximately 6708C for a
pressure ratio of 30, which is good news for the Rankine cycle eciency.
For the energy consumption in the ASU, a sensitivity analysis was carried out and the results
are shown in Fig. 7. The plant power output and the eciency decrease linearly with the ASU
electricity consumption. An increase of this latter by 0.1 kWh/kg O2 gives rise to an eciency
drop of 3% points and a power decrease of about 7%. In the present study a value of 0.25
kWh/kg O2 was chosen. Additionally, compressor work is required to feed the oxygen to the
GT combustor. The total energy consumption is then 0.39 kWh/kg O2 for a GT pressure ratio
of 30.
The results show the following trends. As expected, the eciency and power output of the
GT increase with the pressure ratio. However, with CO2, the optimal values are obtained for
very high pressure ratios. When this latter is 40, it is observed that the power output and the
eciency are already very close to their maximal values. The stream cycle power output
decreases with the GT pressure ratio due to a lowering of the GT exhaust temperature. The con-
sumption of auxiliaries and of CO2 compressors are independent of the pressure ratio whilst the
ASU and the oxygen compression, which are the biggest consumers, have a consumption

Fig. 6. Eciency and power output versus gas turbine pressure ratio for the oxygen ®red combined
cycle.
BOLLAND and MATHIEU: COMPARISON OF TWO CO2 REMOVAL OPTIONS 1661

Fig. 7. Sensitivity on plant performance from ASU energy consumption for production of atmospheric
O2.

slightly increasing with the GT pressure ratio. As far as the CC is concerned, the CC eciency
has an optimum in the range of 25±30 and a decreasing power output with GT pressure ratio.

SUMMARY OF THE RESULTS


The main results are summarized in Table 3.
A comparison of the performances of a CC plant without CO2 removal on the one hand and
with 40% recirculation and CO2 removal on the other hand shows a drop of the power output
by 16% and of the eciency by 8% points. For the eciency this drop remains almost the
same whatever the recirculation rate. This is the energy cost of CO2 scrubbing. The results also
show that the eciency of a CC with recirculation is always higher than that of a semi-closed

Table 3. Summary of plant performance


Combined cycle with 40%
Standard combined recirculationÐremoval2 of Semi-closed combined
cycleÐno removal of CO2 CO2 cycle4
Generator terminals output MW 350.6 100% 320.2 91.3%3 76.0 100%
Air separation unit MW Ð Ð Ð Ð 14.45 18.9%
CO2 compressor MW Ð Ð 15.31 4.4%3 3.1 4.1%
Power plant auxiliaries MW 7.1 2% 9.3 2.7%3 1.3 1.7%
Net plant power output MW 343.5 98% 295.6 84.3%3 57.2 75.3%
Net plant eciency % 55.2 47.1 44.9
1
Equivalent to 0.12 kWh/kg CO2.
2
Related to the generator terminals output (350.6 MW) of the standard CC without removal of CO2.
3
It is assumed that 90% of produced CO2 is removed in the amine absorption process.
4
The size of this plant is given by a compressor inlet ¯ow rate of 100 kg/s.
5
Equivalent to 0.25 kWh/kg O2 for production of atmospheric oxygen. Additionally comes the compression work for
feeding the oxygen to the gas turbine. The number (14.4 MW) comprises both oxygen production and compression.
1662 BOLLAND and MATHIEU: COMPARISON OF TWO CO2 REMOVAL OPTIONS

CO2-based CC, whatever the recirculation rate. When this latter is 40%, the eciency di€erence
is about 2% points.
The analysis shows that the recirculation rate has only a slight positive in¯uence on eciency
and output. Its in¯uence is mainly on the size and hence on the cost of the CO2 scrubber. On
the other hand, as CO2 is used as the working ¯uid (heavier and less compressible than air), the
semi-closed CC, although optimized, will never overcome the CC with recirculation from the
performance point of view. Also the weight of the use of an ASU on the eciency penalty is
high and is not o€set by the weight of the MEA scrubber used here.

CONCLUSIONS
The cross-check of the results obtained by both the Norwegian and the Belgian research
teams using their own models and programmes in the same conditions show a very close agree-
ment of the calculated results. This gives us a full trust in the ®gures used for a comparison of
the two considered CO2 removal options, namely the semi-closed Brayton cycle and the use of
partial recirculation of the ¯ue gas. The results clearly show that the second option is the best
one either from the performance point of view or for the technical feasibility. Indeed, in the ®rst
option the development of a CO2-based gas turbine is necessary. Although such machines do
not exist on the market, a big manufacturer would however only need 5 years to build them.
Although the recirculation technique does not bring a signi®cant eciency improvement when
compared to a plant equipped with a CO2 scrubber without recirculation it provides better oper-
ating conditions for the scrubber performance and lower costs thanks to a reduction of the inlet
throughput and an increase of the CO2 concentration in the ¯ue gas.
On its side, the second option, in addition of being 2 or 3% points more ecient than the
®rst one, is feasible in a short future as all the components belong to proven and mature tech-
nologies.
However, if zero emission is the decision criterion, the ®rst option is then required. It has to
be beared in mind that other CO2-based cycles with zero emissions are as ecient as if not
more than the one considered here and should be taken into consideration in a broader
analysis [11].
So the conclusion of this analysis is only valid for the semi-closed cycle which has been
selected here because, unlike others, it only comprises a one-shaft gas turbine.

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