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Flue Gas Recirculation in Gas Turbine
Flue Gas Recirculation in Gas Turbine
GT2009-59221
τ
increase of CO emission due to incomplete combustion, (ii) the tHR_reactivity relative t HR reactivity: tHR / tHR_ref
Da = turb
τ HR
shift of the lean blow out (LBO) margin limit, (iii) the changes Damköhler number
in the thermo acoustic response of the combustor, (iv) the
change of flame volume and location leading to variations of SENKIN~PFR Chemkin plug flow reactor module
wall heat load, and (v) the change of flame luminosity and flow PREMIX Chemkin laminar flame speed module
radiation properties.
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purposes only and is subject to change without notice. No representation or warranty is given or to be implied as to the
completeness of information or fitness for any particular purpose.
2
PDF probability density function (PDF) was computed using CHEMKIN II modules [15]. For the first
n=
m combustor (EV), also representing a single combustion engine,
mole number [mole], mass and molar mass the computational module PREMIX for laminar flame speed
M was used, whereas for the sequential combustor (SEV), the
ex in
n NOx , n NOx NOx mole number at exhaust, inlet SENKIN module (plug flow reactor for ignition times) was
χ NO =
ex employed. The study is therefore made both for a generic gas
ex nNO turbine lean premix burner and also for a reheat burner similar
exhaust mole fraction
n ex to the reheat burner used in the ALSTOM GT26 engines. The
network model used for the numerical study is shown in Figure
χ net combustor net NOx production
equivalence ratios φ according to a distribution that can also be
NOx 2. In this a number of similar reactors are run at different
χ fuel =
n fuel
n fuel + nair
molar fuel fraction
derived from CFD and water channel tests.
χ NOx
EV-flame SEV-flame
Air , d
seeding NOx content of recirculated air TAT1
SK
TSEV-flame
PR TEV-flame
PR SK
2. REPRESENTATIVE OXIDIZER COMPOSITION Air
Flame HP- SEV LP-
The inlet composition of the GT is determined by the FGR front SK SK
Turbine burner
Flame front SK Turbine
N Premix N Senkin
ratio and the overall O2 consumption of the engine. The latter is reactors
Post flame reactors
Post
flame
Fuel–EV parallel zone parallel
driven by the overall air to fuel Ratio (AFR). The practical limit reactors
serial
Fuel–EV zone
PR SK
of the engine FGR ratio is determined by the technical limit of
combustor and the cooling within the GT. When the exhaust Figure 2. Schematic of the network reactor model using
gas is recirculated not only CO2, but also NOx is accumulated parallel and serial reactors made of PREMIX (PR) and plug
in the flue gas leading also to altered inlet conditions. An flow (SK-SENKIN) modules.
explicit analytical function giving the recirculated gas
composition (including NOx) directly as a function of AFR and The dependency of the NOx formation primarily on the
FGR ratio is used but not further described here. Note however mixing rates has been shown by Vranos [16] to be of
that the gas composition depends to high accuracy only on importance in the pollutants formation for diffusion and
these two parameters. partially premixed flames. Further investigations made by
Adding NO to the air flow at the combustor inlet can result Biagioli and Güthe [17] show the sensitivity to fuel-oxidiser
in negative net emission values if more NOx is consumed than unmixedness of the prompt and post flame contributions to the
produced in the combustor. This “reburn chemistry” is known NOx formation, with a strong effect of pressure. Therefore, it is
[11, 12] to play an important role near stoichiometric of primary importance for practical application to study the
conditions and intermediate temperatures. The effect on laminar NOx formation sensitivity to the unmixedness for FGR
flame speed and NOx formation and destruction has recently combustion operation.
been addressed [13] highlighting the differences of lean and
rich combustion regimes. 3.2. Probability Density Function (PDF) of fuel mixing
The case of recirculating NOx is studied here in an analysis fraction
of the reburn effect. To study the impact of recirculated NOx in In the numerical tool descried above, fuel–air unmixedness
the combustion process and emissions in the GT a parametric is addressed by running parts of the flame at different
study using a high but still moderate value of 100 ppm (mole ~ equivalence ratios in several parallel reactors according to a
volume) NOx [13] at the inlet was conducted for both probability density function (PDF) as shown later in Figure 4.
combustors of the reheat engine. This value is relatively high The PDF models the distribution of fuel mixture fraction. The
but not too far from realistic values at high FGR ratio. The flame is treated like a collection of single flamelets and is
comparison between the NOx-polluted-flue-gas and the non- simulated by running in parallel all the individual reactors
polluted-flue-gas results would explain the chemical effects of followed by a single PFR reactor to model the post flame
the NOx-vitiation in the oxidizer. The influence of CO2 is also region. Each reactor has its individual mean equivalence ratio
investigated in order to verify its influence at realistic levels of and altered mixing temperature distribution according to the
FGR conditions. individual fuel mole fraction xfuel given by the PDF. This means
that parts of the flame will actually sample fuel rich conditions
3. DESCRIPTION OF THE INVESTIGATION METHODS even at overall lean combustor settings. The PDF was chosen as
a Gaußian distribution calibrated with water channel and
3.1. Numerical methods computational fluid dynamics (CFD) simulations data obtained
Following the study of the conventional operation of the at typical engine operation levels is chosen.
reheat engine [14], the kinetic model of the combustion process
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purposes only and is subject to change without notice. No representation or warranty is given or to be implied as to the
completeness of information or fitness for any particular purpose.
3
a large portion of the equivalence ratios φ is covered. This
The width of that function is relatively broad to ensure that is determined by Equation 2 in terms of relative mole (volume)
− n NOx
fraction:
χ NOx ≡
approach has been developed and validated for lean conditions ex in
net n NOx
without recirculation and shown to predict NOx emission well.
n ex
to change with φ such approach will be useful enabling to
Especially for FGR cases where the NOx chemistry is expected
Equation 2
χ NOx
account for mixing and running the problem with detailed The doping is realised by adding a fixed amount of NO
chemistry. If other effects like turbulent mixing and flow fields Air , d
to the air flow resulting in the NOx mole fraction at
remain unchanged, the problem can be described with the same
χ NOx
unmixedness parameter and changes in chemistry are thereby in inlet of the flame after mixing with the fuel (Equation 3).
χ NOx = =
in Air , d
(1 + χ fuel )
focus. In extension to this approach also CO emissions could be in n NOx
modelled if some further refinements were done.
In a technical mixer for a given power the mixing quality is
n in
dependent on geometrical constraints only and not changing Equation 3
with other operating parameters. The width of unmixedness Combining these equations the net NOx production to be
distribution can also be related to experimental or modelling studied with respect to the reburn capability leads to Equation
results to be used as burner design criterion. The fuel mixture 4:
(1 + χ fuel ) M
net ex in ex
straightforward as for non-FGR cases and some alternative
definitions have been proposed [5] there seems to be some need M in
for clarification. In an actual FGR engine not only CO2, but Equation 5
χ NOx =
ex
ex n NOx outcome of a joint KW21 research project of DLR, Alstom and
EnBW (Energie Baden-Württemberg) and will be described in
n ex detail elsewhere. It contains a C2 chemistry including peroxide
Equation 1 chemistry and updated nitrogen chemistry starting from a
flames reactivity (flame speeds sl, ignition times τign and heat
The seeding of NOx at inlet can have an impact on a) the version of the work of Glarborg et al. [12] with some
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purposes only and is subject to change without notice. No representation or warranty is given or to be implied as to the
completeness of information or fitness for any particular purpose.
4
first observed by Fenimore [20] some of these species are the burner inlet from 850 to 1000°C. A wide range of flame
strongly linked to chemistry occurring in the heat release zone temperatures was tested at 8 and 16 bar pressure in the
while others appear to depend on the temperature only. The combustion chamber. For the current experiments, no
different chemical routes can be separated after the N2-reaction pollutants, such as NO or CO, were added to the synthetic
partner into three contributions: oxidizer mixture.
N 2 + O ↔ N + NO Reaction 1
H2
N 2 + O (+ M) ↔ N 2 O (+ M)
CO Throttle
Electric Combustion
N2 Catalytic N2
Reaction 3 O2
Preheater
Preheater
Chamber
N2 + H ↔ N 2H
CO2
View Port
Reaction 4
N 2 + H(+M) ↔ N 2 H (+ M)
Burner
Reaction 5 Mixture of
N2 , O2 , CO2, H2 O Gas Probe
max 1000 °C
3.5. Experimental method defines a limit of operation since beyond that value combustion
In Figure 3 a schematic drawing of the experimental setup cannot be completed. Note that the same mean Tflame for
increasing FGR ratio the richer parts of the flame do not result the combustion zone with the FGR as well as the slow down of
in higher Tflame as in the standard case the combustion process going along with a decrease of
Since NOx production increases exponentially with reactivity as can be expressed by the Damköhler number Da.
temperature for each flame-let the overall NOx production for Assuming the turbulence levels to be unchanged by the gas
increasing FGR decreases due to reduced magnitude of the inlet composition the decreased reactivity due to FGR defined
local temperature peaks within the flame brush. This fact by the reaction time tHR leads to a decrease of Da. consequently
already substantiates a first argument why in technical mixtures the flame-let approximation valid for Da>>1 [25] might
FGR would produce less NOx compared to the standard case. become less accurate and combustor designed on this
assumption might be problematic. Note the reactivity decrease
4.2. EV- Heat release time scale τHR when following the mean operation line in Figure 5 and Figure
These changes in temperature and equivalence ratio have a 6. A similar argumentation supports this based on the sl directly
direct impact on the chemical time scale of the combustion for the EV or for tHR in SEV combustion but are omitted here
process, or combustion reactivity. This is represented by the for brevity.
τign/τign_ref
6 GRI:O2_GT_inlet=no FGR
GRI:O2_GT_inlet=high FGR
GRI:O2_GT_inlet+NO=no FGR
5 GRI:O2_GT_inlet+NO=high FGR
RD:O2_GT_inlet=no FGR
RD:O2_GT_inlet=high FGR
RD:O2_GT_inlet+NO=no FGR
4
RD:O2_GT_inlet+NO=high FGR
ΔNO
FGR
3
GRI
2
1
lean rich RD06_NO
Figure 6: Map of ignition time reactivity τign_reactivity as a
no FGR
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purposes only and is subject to change without notice. No representation or warranty is given or to be implied as to the
completeness of information or fitness for any particular purpose.
7
conditions. For the EV conditions the effects of NOx on tHR and
15 Overall NOx Production EV-combustor
laminar flame speed sl are negligible for GRI and RD06_NO
5. NOX EMISSION 5
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purposes only and is subject to change without notice. No representation or warranty is given or to be implied as to the
completeness of information or fitness for any particular purpose.
8
The NOx formation is best understood by investigating the
8 Overall NOx Production SEV NO profiles of the SEV flamelets of the different cases as
7
shown in Figure 11 and for the EV conditions in Figure 12. The
SEV tech mix cal no seed NO formation profile is determined by the reaction of the
6 SEV tech mix cal seed
SEV perf mix _cal no seed
reactants concentration (N2, O, CH, H, etc.) as well as the
NOx abs. normalised
5
SEV tech mix cal seed reaction rates k(T, p). The NO formed at a given residence time
4 0 therefore depend on the reactant species concentrations,
3 temperature and competition of the different chemical
2 pathways.
RD: no EGR
1 RD: EGR_case2
RD: EGR_case3
NO
0
RD: EGR_case4
-1 RD: EGR_case5
RD: EGR_case6
-2 RD: EGR_case5 phi=1.45
decreasing [O2]_inlet
NO abs
Figure 9: Net SEV-NOx emissions ( χ net NOx
) on absolute
scale normalised to “no FGR perfect mixing” for technical
mixer (solid lines) and perfectly mixed case (dashed lines) with
(squares) and without (triangles) seeding of NO at p ~16 bar
using RD06_NO.
In Figure 10, the fact that NOx can increase with the very
- 0.10 0.20 0.30 0.40 0.50 0.60 0.70 0.80 0.90 1.00
small amount O2 inlet concentration is at first sight puzzling time/ tres
since FGR is usually thought to decrease NOx emission. This
could be expected from the reduced concentration of O Figure 11: NO time profiles for reference Tflame and
radicals, reducing the formation of NOx via Reactions 1-2. different FGR ratios form SEV model with RD06_NO. For the
However the numerical finding in Figure 8 seem to be low O2 content of 12.7 % (at GT inlet) also profile at increased
confirmed by experimental data. The nature of this important xfuel (φ=1.45) is plotted. Cases 2 to 6 refer to the FGR ratios as
observation will further be analyzed in the next section. plotted in Figure 4, Figure 5 and Figure 8.
2.0 Overall NOx Production MHD vs. SEV- model
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purposes only and is subject to change without notice. No representation or warranty is given or to be implied as to the
completeness of information or fitness for any particular purpose.
9
GRI: no EGR
The profiles of NO and intermediates for the EV and SEV
x_mole
GRI: EGR_case7 NO model appear to be similar and are displayed for the EV case
GRI: EGR_case8
GRI: EGR_case9 using the RD06_NO in Figure 12. The cases 7 to 10 refer to the
GRI: EGR_case10
GRI: EGR_case5phi1.72
FGR ratios as plotted in Figure 6, Figure 9 and Figure 13.
The NO profile is plotted over the full reactor residence
time while the intermediates are plotted just around the heat
release time scale showing the super-equilibrium concentration
close to the heat release to explain the radical (O, CH, H)
overshoot responsible for the prompt NOx formation.
With increasing FGR the O radical peak becomes less
-10% 0% 10% 20% 30% 40% 50% 60% 70% 80% 90%
time /100%
tres importnat resulting in less importance for the reaction 1 and 2
x_mole
GRI: EGR_case10
formation consider the work of Dagaut et al. [28]. While it is
6.E-09
reasonable to separate [17] the NOx formation into a part
4.E-09 coupled to heat release (prompt, or fast) and a part occurring in
post flame regions (thermal, or slow), the chemical reaction
2.E-09 paths (in terms of intermediates and reaction steps) can be
studied by the following simulations. Since the NOx formation
0.E+00
1.E-04 chemistry is described well in the GRI this mechanism
x_mole
O GRI: no EGR (compared to the RD06_NO) can serve as base for the
1.E-04
GRI: EGR_case7 following study on the NOx formation pathways- at least for the
1.E-04 GRI: EGR_case8 EV case studied here: Each of the reactions has been turned off
8.E-05 GRI: EGR_case9 in the GRI mechanism as described earlier. For the SEV
6.E-05
GRI: EGR_case10 simulations analogue modification can be done.
Turning off the N2O reactions (reaction 2) reduces most of
4.E-05
the NO formed promptly in both cases having little impact on
2.E-05 the post flame slope for thermal NOx, which is changed only if
0.E+00
the Zeldovich path (reaction 1) is turned off. The thermal NOx
3.E-07 GRI: no EGR rate depends strongly on temperature and pressure while the
x_mole
HCN GRI: EGR_case7 N2O (also from N2 and O) has little dependency on temperature
GRI: EGR_case8 and pressure and is more sensitive to reactant concentration [O]
2.E-07 GRI: EGR_case9 at super equilibrium. In the FGR case, the thermal NOx rate is
GRI: EGR_case10 clearly reduced due to reduced reactant concentration of [O]
with prompt formation playing the bigger role. Clearly at richer
1.E-07 conditions also the Fenimore (via CHn species) and NNH paths
play a role complementing the N2O path.
Assuming that the coupling is not large, each path can be
0.E+00 assigned a relative value of relevance for the NOx contribution
1.E-04
x_mole
GRI: no EGR
H GRI: EGR_case7
for different selected O2 conditions, as shown in Figure 13. The
8.E-05
individual contribution of a reaction path is given as the
GRI: EGR_case8
difference obtained using the truncated mechanisms and the full
6.E-05
GRI: EGR_case9
GRI. Summing up all contributions leaves a remaining portion
GRI: EGR_case10 of less than 18 %. These relative contributions are plotted
4.E-05 stacked-up to sum up to 100% for the full SEV model in Figure
13. Note that the absolute NOx formation is at the same time
2.E-05
reduced as displayed by the full line and circles. The remaining
18% probably result from other paths not resolved in this study
0.E+00
-1% 0% 1% 2% 3% 4% 5% 6% 7% 8% time
9%/ tres or from coupling between the mechanisms. Within the GRI this
Figure 12: Profiles of key intermediates and trace species include the reactions of N2 with OH, HO2, H, H2, H2O, CO,
from EV model (PREMIX runs using GRI30) at different FGR. CO2, HCO. The degree of decoupling is however remarkable
which is prerequisite for a display as stack-up plot.
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purposes only and is subject to change without notice. No representation or warranty is given or to be implied as to the
completeness of information or fitness for any particular purpose.
10
SEV Tref: technical mixer participation in further heat release driving reactions.
NOx_abs/ppm
100%
Furthermore, the role of CO2 is observed in Figure 14. CO2 is
90%
in fact acting through the removal of the highly reactive
80%
radicals like H via reactions such as OH + CO ú H + CO2 [6]
70% revealing that CO2 cannot be treated as a fully inert diluent. The
60% influence of CO2 is turned off by replacing the CO2 by a less
NOx [%]
50% Fenimore reactive inert, namely N2, and leaving all other effects of FGR
40% HNN turned on. It is found that when reaching the lowest O2
30% N2O concentration level, the decrease of laminar flame speed is 27%
20% Zeldovich lower when CO2 is not considered (64.7 % of the reference
10% Else case). Thus, CO2 has a significant share in the overall decrease
0% Absolute Nox of reactivity, keeping in mind that in engine operation such
no EGR EGR 1 EGR 2 EGR 3 EGR 4 effect would have to be compensated by other operating
decreasing O2 _inlet [mol] conditions. The main effect however seems to be due to the
Figure 13: Relative contribution displayed as stack-up for reduced O2 and O radicals content.
110%
SEV model with versions of GRI as described in the text for the CO2 effect on reactivity
technical mixer.
3E-06
As a conclusion, the FGR reveals a new energy technology
2E-06 beneficial not only for CO2 capture but also the reduction of
pollutant emissions in the combustion process. The benefits for
1E-06 FGR can be utilised at all existing ALSTOM GTs but especially
the prospect for the reheat engines GT24 and GT26 look
0E+00 promising:
0.0 0.2 0.4 0.6 0.8 1.0 1. Higher AFR requires less recirculation rate to reach low
non-dim. residence time [-]
O2 and high CO2.
Figure 15: NO time profiles for perfectly mixed cases non 2. The increased operational flexibility to compensate
FGR (green curves) and FGR (brown curves) at p = ~16 bar reactivity variations with temperature of the first
(solid lines) and at 2p = ~32 bar (dashed lines). combustor at minimal impact on power according to the
reheat concept allows flexible operation over the full
range of reactivities.
CONCLUSION 3. Technically the SEV combustion range at FGR conditions
The investigations presented in this paper point to the use is ideal to utilize the benefit of reburn chemistry effects to
of the FGR not only as a way of cost reduction and efficiency achieve low NOx emissions.
rise in a combined cycle plant with a CO2 capture unit, but also 4. Running the first combustor at FGR condition the main
as an effective technique for pollutant emissions reduction. A benefit is obtained at high engine pressure ratio in the first
reactor network model described for the first time has been combustor where the post flame NOx is reduced without
applied to predict the effect on NOx emission for FGR for real altering the EV reactivity too much, while the second
engines and technical mixers using detailed chemistry. An combustor runs at low O2 content.
extension to predict CO emission using this approach is also
possible. The two different kinetic schemes used (the GRI and ACKNOWLEDGMENTS
RD06_NO) show different trends for reactivities especially in Dieter Winkler, Tim Griffin University of Applied Sciences
presence of NO, while their NOx predictions seem to agree. The Northwestern Switzerland are acknowledged for providing first
analysing the contribution of the different reaction pathways 1 Griffin T., Buecker D., Pfeffer A., “Technology Options
as a function of FGR ratio. The main NOx pathway for for Gas Turbine Power Generation With Reduced CO2
“non-FGR” gas turbines is the thermal NOx following the Emission”, ASME Journal of Engineering for Gas Turbines and
Zeldovich path. The N2O pathway is most important for Power, 130, 041801 (2008).
prompt NOx in the lean regime. The NNH and Fenimore via 2 Bolland O., Mathieu P., “Comparison of Two CO2
CHn are becoming important only for prompt formation Removal Options in Combined Cycle Power Plants”, Journal of
under rich conditions or in unmixed region for FGR. The Energy Conversion and Management, Vol. 39, No. 16-18, pp.
residence time where NOx are analyzed plays a major role 1653-1663 (1998).
© ALSTOM 2009. All rights reserved. Information contained in this document is provided without liability for information
purposes only and is subject to change without notice. No representation or warranty is given or to be implied as to the
completeness of information or fitness for any particular purpose.
12
4 Benajes, J., Molina, S., Novella R., and DeRudder K. 18 Gregory P. Smith, David M. Golden, Michael Frenklach,
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© ALSTOM 2009. All rights reserved. Information contained in this document is provided without liability for information
purposes only and is subject to change without notice. No representation or warranty is given or to be implied as to the
completeness of information or fitness for any particular purpose.
13
© ALSTOM 2009. All rights reserved. Information contained in this document is provided without liability for information
purposes only and is subject to change without notice. No representation or warranty is given or to be implied as to the
completeness of information or fitness for any particular purpose.
14