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Study of a Rich/Lean Staged Combustion Concept for Hydrogen at Gas Turbine


Relevant Conditions

Conference Paper · June 2013


DOI: 10.1115/GT2013-94420

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Proceedings of ASME Turbo Expo 2013: Turbine Technical Conference and Exposition
GT2013
June 3-7, 2013, San Antonio, Texas, USA

GT2013-94420

STUDY OF A RICH/LEAN STAGED COMBUSTION CONCEPT FOR HYDROGEN AT GAS


TURBINE RELEVANT CONDITIONS

Felipe Bolaños, Dieter Winkler, Felipe Piringer, Timothy Griffin*


Institute for Thermo- and Fluid Engineering, University of Applied Sciences Northwestern Switzerland
(FHNW) 5210 Windisch, Switzerland

Rolf Bombach, John Mantzaras


Paul Scherrer Institute, Combustion Research, 5232 Villigen-PSI, Switzerland

*Corresponding Author: timothy.griffin@fhnw.ch

ABSTRACT
In the realized R/L concept the products of the first rich stage,
The combustion of hydrogen-rich fuels (> 80 % vol. H2), which is ignited by a Pt/Pd catalyst (under a laminar flow,
relevant for gas turbine cycles with "pre-combustion" carbon Re ≈ 1900) are combusted in a diffusion-flame-like lean stage
capture, creates great challenges in the application of standard (turbulent flow Re ≈ 18500) without any flashback risk. The
lean premix combustion technology. The significant higher optical accessibility of the reactor has allowed insight into the
flame speed and drastically reduced auto-ignition delay time of combustion processes of both stages. Applying OH-LIF and
hydrogen compared to those of natural gas, which is normally OH*-chemiluminescence optical techniques, it was shown that
burned in gas turbines, increase the risk of higher NOX mainly homogeneous reactions at rich conditions take place in
emissions and material damage due to flashback. Combustion the first stage, questioning the importance of a catalyst in the
concepts for gas turbines operating on hydrogen fuel need to be system, and opening a wide range of optimization possibilities.
adapted to assure safe and low-emission combustion.
The promising results obtained in this study suggest that such a
A rich/lean (R/L) combustion concept with integrated heat rich/lean staged burner with integrated heat transfer could help
transfer that addresses the challenges of hydrogen combustion to develop a new generation of gas turbine burners for safe and
has been investigated. A sub-scale, staged burner with full clean combustion of H2-rich fuels.
optical access has been designed and tested at gas turbine
relevant conditions (flame temperature of 1750 K, preheat
temperature of 400 °C and a pressure of 8 bar).

Results of the burner tests have confirmed the capability of the


rich/lean staged concept to reduce the NOx emissions for
undiluted hydrogen fuel. The NOx emissions were reduced from
165 ppm measured without staging (fuel pre-conversion) to
23 ppm for an R/L design having a fuel-rich hydrogen pre-
conversion of 50 % at a constant power of 8.7 kW.

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INTRODUCTION
− Avoidance of super adiabatic temperatures; hydrogen's
Electricity generation with a low CO2 footprint produced by a
lower than unity Lewis number LeH2 < 1 causes super
combination of highly energy efficient, gas turbine combined
adiabatic temperatures at the catalyst surface under lean
cycles with additional carbon capture steps will play an
conditions. This can be avoided with fuel-rich operation
important role in the future. During the last decades carbon
by making the less diffusive oxygen (LeO2 ≈ 2.1) the
dioxide concentration in the atmosphere has increased
limiting reactant.
approximately 20 %; carbon dioxide is a greenhouse gas which
participates in the global warming process and all the natural
To be able to apply this concept in gas turbines, a better
and social consequences that this phenomenon implies. “Pre-
understanding of the heterogeneous and homogeneous
combustion carbon capture” is a recent technology under
combustion processes is required. In this work an experimental
intense investigation, which essentially removes carbon from
and numerical study using a visually accessible rich/lean burner
the fossil fuels (e.g. natural gas or coal) resulting in hydrogen-
module is proposed to understand the combustion processes in
rich fuels. In this context, the combustion properties of
the heterogeneous and homogeneous reaction stages.
hydrogen lead to much higher flame speeds and reactivity, as
well as drastically reduced auto-ignition delay times compared
This module allows the investigation of the progress of reaction
to natural gas fuels that are normally burned in gas turbines.
and its location inside the catalytic stage (e.g. determination of
This in turn requires an adaptation of the combustion concept to
potential homogeneous combustion within the catalytic section).
assure safe and low-emission (NOX) combustion [1].
The study of the second stage lean flame further facilitates the
understanding of the NOX formation and flame stabilization
Over the last years many research groups and gas turbine
mechanisms.
producers have been studying hydrogen combustion
fundamentals and related practical issues, seeking concepts and
To investigate gas turbine relevant conditions the operating
engineering solutions for this new technology [2-7]. One
conditions for the experiments were chosen as follows: A flame
promising concept to reduce NOX emissions is rich/lean
temperature of 1750 K, a pressure of 8 bar and a preheat
combustion (Figure 1). This concept consists of staged
temperature of 673 K.
combustion with a first fuel-rich section and a second lean
burnout stage; its capability for NOX emissions reduction has
been demonstrated by different researchers for hydrocarbon
fuels [8-10] and for hydrogen [11-14].

Previously a staged R/L burner has been developed and tested


with success, achieving low NOX emissions and demonstrating
stable combustion [14]. The design of this burner presents a
variation of the R/L concept, which is not well understood. This
burner includes a heterogeneously catalyzed rich stage, which is
advantageous when working with H2-rich fuels, as described
below.

The concept of this burner is to reduce the reactivity of the H2-


rich fuel by distributing part of its enthalpy to a bypassing air
stream via heat transfer in the rich combustion stage. Not only
the reduction of the amount of fuel being injected into the Figure 1: R/L staged combustion concept, where λ is the air
homogenous lean stage but also the presence of diluents and excess ratio (λ=1/φ).
products of combustion (in the hydrogen case, nitrogen and
steam) would reduce the reactivity of the mixture, thus allowing OPTICALLY ACCESIBLE R/L STAGED BURNER
for safe, clean and stable combustion
The adopted burner is a simplification of the design investigated
The use of a catalyst in a fuel-rich hydrogen combustion stage by Piringer et al. [14]. Herein, the rich stage comprises only one
presents a number of advantages: catalytic tube (rather than the tube bundle used in [14]). Both,
− Low ignition temperatures the catalytic rich and the homogeneous lean stages, are optically
− No igniter necessary accessible.
The first stage (catalytic) has a length of 430 mm (Figure 2) and
− Very low NOX emissions is composed of three concentric cylindrical tubes; the two outer

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ones are made of quartz glass and the inner one is a nickel- and their temperatures were monitored with thermocouples.
based alloy tube. The inner tube is coated with a Pt/Pd catalyst Three different mass flow controllers were employed; one for
only in its outer surface. the bypass air, one for the air of the rich combustion stage, and
a third one for the hydrogen flow. Having two different mass
The three tubes define two annular gaps. Rich combustion takes flow controllers for the bypassing air and the rich stage air
place in the inner annular gap. Air for the rich stage is delivered allowed the variation of the fuel/air ratio in the rich stage (λRich;
from the outer annular gap through an arrangement of holes in air excess ratio in the rich stage). This in turn facilitated the
the inner quartz tube. On the other hand, the bypass air required investigation of different levels of fuel pre-conversion (from 0
for lean combustion flows inside the metal catalytic tube, thus to 50 % fuel pre-conversion in the rich stage), while keeping a
cooling the rich stage and distributing the released heat constant overall flame temperature and thus a constant
throughout the system. At the end of the rich stage, both flows equivalence ratio. An oil-free compressor supplied the
(the bypassed air and the rich combustion products H2, N2 and necessary air, while hydrogen was supplied by pressurized gas
water steam) are discharged in the follow-up lean stage module cylinders. The experimental conditions are presented in Table 1.
(not shown in Figure 2). This module is also fully optically
accessible. Pressure [bar] 8
Preheat temperature Tox [K] 673
Flame temperature Tad [K] 1750
λOverall 2.37
λRich 0.0 - 0.5
ReRich ≈1900
ReLean ≈18500
Table 1: Experimental conditions

To study the combustion processes, planar OH-LIF, OH*-


chemiluminescence and exhaust gas analysis measurement
techniques were employed. The exhaust gas composition (O2,
NOX) was measured at the end of the burnout zone using a
cooled gas probe and an MRU MGA5+ gas analyzing system.
For the laser diagnostics the pressure vessel was equipped with
two 350 mm long, 50 mm high and 35 mm thick quartz
windows, aligned with respect to the R/L reactor; the entire lean
combustion section and most of the rich section (2/3 of the rich
stage length) could thus be visualized. An additional window in
the rear flange of the vessel (at the reactor exhaust) provided a
counterflow optical access for the LIF laser sheet.

For the OH-LIF laser measurements a Nd:YAG pulsed laser


(Quantel YG981E) pumped a tunable dye laser (TDL90 NBP2).
The frequency-doubled radiation of the dye laser (285 nm) had
a pulse energy of 5 mJ, low enough to avoid saturation of the
A(v’ = 1) ←X(v″ = 0) transition at 8 bar. The 285 nm beam was
transformed into a light sheet using a cylindrical lens telescope
and a 1 mm slit mask, which propagated counterflow along the
x–y symmetry plane (Figure 3). The fluorescence from both
Figure 2: Rich stage module description and geometry (not (1-1) and (0–0) OH transitions at 308 and 314 nm, respectively,
drawn to scale) was collected at 90° through the reactor and tank side-windows
with an ICCD camera (LaVision Imager Compact HiRes-IRO,
1392 x 1024 pixels). After a 2:2 binning, a 110 mm x 35 mm
EXPERIMENTAL SETUP
area was recorded onto 696 x 220 pixels of the ICCD chip,
providing sufficient intensity for single exposure LIF and OH*-
The R/L staged burner was mounted inside a 1.8 m long
chemiluminescence images. The camera was traversed axially
cylindrical vessel providing the desired pressurization
to map both rich and lean stages of the burner.
(Figure 3). The air flows were preheated electrically. All flows
entering the burner were controlled with mass flow controllers

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y

Figure 3: Experimental setup and measuring system of the high pressure test rig

RESULTS NOX vs. λRich


T ad=1750 K, P=8 bar, Fuel: XH2=1
The above presented burner and experimental setup allowed 180

investigating the rich stage independently of the lean stage and 160
vice versa. Results for the overall burner performance are 140
presented below. 120
NOX [ppm]

100
Burner Overall NOX Emission Performance
80
60
The NOX emissions for different pre-conversion values are
presented in Figure 4. 40
20

The measured NOx emissions presented in Figure 4 (not 0


normalized) illustrate the beneficial effect of fuel pre- 0 0.1 0.2 0.3 0.4 0.5

conversion in the rich stage. It can be clearly noticed that the λRich [-]
NOX emissions drop by a factor of eight, from ≈165 ppm
without pre-conversion to ≈23 ppm with a fuel pre-conversion Figure 4: Measured NOX emissions vs. fuel pre-conversion
rate of 50 % (full oxygen conversion in the rich stage is always
assumed).
Lean Homogeneous Stage Performance

The optical access to the lean stage permitted the observation of


the lean burnout flame. An OH-LIF averaged image of the
flame is presented in Figure 5.

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From Figure 5 it can be determined that the flame established in Nonetheless a different behavior was observed in the
the lean stage is a diffusion type flame. The flame is attached to experiments. Combustion did not occur on the catalyst surface
the rich module outlet being stabilized by the hot product (heterogeneous combustion) but in a mainly homogeneous
recirculation zone. Two different reaction zones, indicated by reaction zone. Figure 6 shows a flame stabilized at one of the
the OH-LIF signal were observed (Figure 5). A more intense rich air delivery holes.
OH zone in the inner side of the annular flame and a weaker
zone in the outer side were observed. This difference is due to
the reduced concentration of oxygen coming from the
recirculated reaction products of the lean stage (13.3 % vol. O2)
compared to the bypass air flow (21 % vol. O2).

The stoichiometric reacting zone of the established diffusion


flame is well known for its high flame temperatures resulting in
high NOX production. However, the results show that the R/L
concept is capable of combusting undiluted hydrogen with very
low NOX emissions (<25 ppm), while eliminating any flashback
risk, due to the inherent characteristic of a diffusion flame.
These results reveal an even further NOX reduction potential.

Figure 6: Visible light and OH*-chemiluminescence around


the rich catalytic stage air distribution hole
Not only the observed visible light, but mainly the high OH*-
chemiluminescence signal measured at the air holes, confirming
that combustion occurred primarily homogeneously (the OH
signal in a pure catalytic process is too low to monitor with LIF
[15]). The immediate reaction after the air injection in the
annular gap did not allow for a fully premixed combustion, thus
λRich = 0.5 conditions close to stoichiometry were present along the
reaction zone and a diffusion type flame was formed in the fuel-
Figure 5: Averaged (A) and instantaneous (B) 2D OH-LIF
rich section.
image of the flame. 1) Bypass air core, 2) Annular
fuel injection (burner outlet), 3) Recirculation
To better understand the process in Figure 6, Figure 7 presents a
zone, 4) Outer zone of appreciable OH-LIF signal,
diagram depicting the flow in a cross section view.
5) Inner zone of OH-LIF with maximum signal.

Rich Catalytic Stage Performance

The rich stage can be tested independently from the lean stage
by using nitrogen as bypass "air". In this way the rich stage
NOX emission and the fuel conversion effectiveness can be
studied. The novel optical access to the rich stage annular gap
reaction zone also facilitated the study of the rich combustion
process characteristics.

The preheated air for the rich stage was designed to flow
through the hole arrangement from the outer into the inner
annular gap (where the catalytic coating was located). In the
inner annular gap the air would mix with the hydrogen and start Figure 7: Diagram depicting the section view of an air
reacting on the catalyst surface controlled by oxygen diffusion injection zone (hole injection) in the inner annular
(thus avoiding super adiabatic flame temperatures). After the gap (rich stage combustion zone).
rich catalytic section, the combustion products (hydrogen,
nitrogen and water-steam) flow into the lean stage. Figure 6 refers to λRich = 0.2. With this degree of pre-conversion
and taking into account the bypass cooling effect (assuming
ideal heat transfer) a rich stage flow temperature of ≈580 °C

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was expected, however the cooling effect was not perfect and hydrogen's high reactivity and high flame speed allowed for the
occurred slowly, permitting higher local temperatures. Maestri upstream propagation of lean stage flame through the annular
et al. have also measured homogeneous ignition in an annular gap. This is a kind of "flashback", however, the presence of a
catalytic reactor at atmospheric conditions over temperatures of reaction zone in this region was intentional; this behavior can be
650 °C [16, 17]. Also Schultze et al. [18] have shown that under described as a "flashback ignition" of the rich stage.
fuel-rich conditions homogeneous ignition over a catalyst
occurs easier than at lean conditions due to the low molecular Although it has been observed that the rich stage contained
transport of the limiting O2 reactant that negates large catalytic fuel-rich diffusion flames, no NOX production was detected
consumption over the gas-phase induction zone. On the other coming from this stage. It is likely that the highly reactive
hand, at lean conditions, the large diffusivity of the limiting H2 hydrogen consumes most of the oxygen before NOx can be
reactant allows for considerable catalytic conversion, which in formed. NOX emissions from the rich stage were measured by
turn deprives H2 from the homogeneous reaction pathway suppressing the lean combustion via flowing nitrogen instead of
air in the bypass tube (a minimal flow in the bypass tube was
This result is very important since it demonstrates that a pure required to cool the rich stage and ensure mechanical integrity
catalytic combustion process is not feasible under the examined of the burner).
conditions (high preheat temperatures and pressures) and
questions the necessity and importance of a catalyst in the rich
stage.

To assess the role that the catalyst is playing in the stabilization


of the flame it was decided to test the system without any
catalytic coating. To this end, a polished non-catalytic metal
tube was used (Figure 8).

Figure 9: OH-chemiluminescence of the homogeneous


reaction in the rich stage, with catalyst (upper)
without catalytic coating (lower)
Figure 8: Catalytic and inert bypass tubes
This test has shown that the catalytic coating is not required to NOX Modeling
stabilize the flame in the rich stage. Figure 9 shows the OH*-
chemiluminescence in both cases. It is clear that the reaction To understand the NOX production two zero-dimensional
zone stabilizes at the air holes in the same way without any models of the combustion concept were proposed using the
apparent influence of the catalytic coating. However, it is open source software Cantera [19] and the GRI 3.0 gas-phase
stressed that it was not possible to ignite the system without an reaction mechanism [20]. The first model is presented in
external ignition source (the catalyst acted as igniter); for this Figure 10.
reason, an external source of ignition (heated coil) was placed
in the lean section. The fact that a stable reaction was observed
at the rich stage without the presence of a catalyst indicated that

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condition). For this purpose, the model presented in Figure 12
was proposed.

Figure 10: PFR model for NOX production


In this model the air of the rich section and the fuel are mixed in
a first step and then enter a reactor under fuel-rich conditions. Figure 12: Model for stoichiometric flame temperatures
In this reactor the mixture equilibrium is calculated without
In this model instead of employing a PFR to calculate the NOX
nitrogen oxide products (assumption based on measurement
production, the maximum combustion temperatures were
results). Downstream of the rich reactor the rich combustion
calculated. This was done by mixing only the required amount
products exchange energy with the bypass air, cooling them
of bypass air with the remaining fuel (function of λRich) coming
down and afterwards are mixed and brought into the lean
from the rich combustion so as to achieve stoichiometric
reactor. The lean reactor was modeled as a plug flow reactor,
conditions in the second reactor. Before splitting and mixing the
PFR, so as to understand the effect of pre-conversion on the
fuel, an ideal heat transfer between both flows was assumed
NOX chemical kinetics. Figure 11 shows calculated NOX
(modeling the cooling of the rich stage with the bypass air).
production as a function of fuel pre-conversion.
The results for the stoichiometric temperatures of the diffusion
NOX vs. Pre-conversion flame as a function of the fuel pre-conversion in the rich stage
Tad = 1750 K, P=8 bar, Tin = 673.15 K
3 are presented in Figure 13.
PFR
2.5
Stoichiometric flame temperature vs.
Pre-conversion
2 Tad = 1750 K, P=8 bar
NOX [ppm]

2800
1.5
Temperature [K]

2600
1

0.5 2400

0
2200
0 0.1 0.2 0.3 0.4 0.5 0.6
λRich [-]
2000
0 0.1 0.2 0.3 0.4 0.5 0.6
Figure 11: NOX production for different λRich calculated λRich [-]
using a PFR model.
Figure 13: Flame temperature (λ=1) vs. pre-conversion
From Figure 11 it can be concluded that a staged combustion
rate (diffusion flame max. temperature)
concept is irrelevant if perfect mixing could be attained. Perfect
mixing is difficult to achieve when employing highly reactive
H2-rich fuels because of the associated flashback risk. The The results show a significant reduction of the flame peak
results in Figure 11 do not capture in any way the NOX temperature. The temperature change achieved with a 50 % pre-
production observed in the experiments (Figure 4) since the conversion of the fuel in the rich stage was approximately
assumed perfect mixture does not represent the physics of a ΔT = 400 K. To better assess the effect of such a ΔT on the
diffusion flame. nitrogen oxides production, the NOX emissions for different
flame temperatures over a temperature change of 400 K were
However, capturing NOX emissions in a diffusion flame with a calculated (using a PFR).
zero-dimensional model is a very difficult task. To assess the
fuel pre-conversion effect on the diffusion flame, it was decided
to model the highest possible flame temperature (stoichiometric

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NOX vs. Flame Temperature
former was investigated using an external ignition source); this
P=8 bar Tox=673.15 K comparison showed that the only apparent function of the
catalyst was to ignite the fuel-rich gaseous flame in the first
100
stage.
47.4
NOX/NOX,min [-]

17.4 After analyzing the experimental data, the key features reducing
10 the NOx emissions were identified:
7.2

2.8 1. Less amount of hydrogen being injected into the lean


1 1 stage:
0 100 200 300 400 500 Pre-converting hydrogen in the rich stage (without
ΔT [K]
noticeable NOX production) reduced the amount of fuel
that had to be injected and mixed in the lean stage. This
Figure 14: Calculated normalized NOX emission vs. relative
reduced the hot spots in the lean flame, lowering at the
flame temperature using a PFR in a
same time the NOX production.
temperature range between 1600 and 2000 K
which is relevant for lean premix gas turbine
2. Heat transfer in the rich stage:
technology.
The heat transfer to the bypass air helps to distribute the
Figure 14 shows the normalized NOX production (normalized to heat release over the total flow through the burner, thus
the minimal. calculated value) as a function of the relative reducing the forming of hot spots. It was shown that this
temperature (interval between Tad = 1600 and 2000 K, flame process reduces NOX formation in the following lean stage.
temperatures relevant for gas turbine combustion). Results in
Figure 14 present the well-known exponential effect of 3. Self-dilution:
temperature on NOX production. By comparing these results Fuel pre-conversion also helped to reduce the NOX
with the experimental ones, which exhibit a nearly exponential production by providing self-dilution. Cooled combustion
dependency on λRich, it can be concluded that NOX production is products from the rich stage served as thermal ballast; this
reduced mainly due to this temperature reduction effect. thermal ballast dropped the peak temperatures in the
unmixed flame and reduced its NOX formation.

CONCLUSIONS The combination of these factors was responsible for reducing


the NOX production and attaining low emissions with a
The search for clean and efficient energy sources has posed new diffusion flame.
challenges to the power generation sector. The utilization of
hydrogen-rich fuels is one such key issue. In this work a The rich/lean combustion concept has proven to be a very
rich/lean optically accessible staged combustion system for promising possibility to combust hydrogen-rich fuels cleanly
hydrogen was designed and tested under gas turbine relevant and safely at gas turbine conditions.
conditions. This novel quartz glass design permitted optical
measurements (OH-LIF and OH*-chemiluminescence) that
helped to understand the combustion processes in both rich and ACKNOWLEDGEMENTS
lean stages.
The authors thank the financial support of this research by
It has been shown that the R/L concept is capable of reducing CCEM/CCES, swisselectric research and the Swiss Federal
the NOX emissions significantly to low values (≈23 ppm at Office of Energy (BFE) under project "CARMA" (Carbon
Tad = 1750 K, P = 8 bar, Tox = 673 K) using 100 % hydrogen Management in Power Generation).
(no external dilution) while eliminating the flashback risk. The
optically accessible sub-scale burner showed that diffusion For their technical support the authors thank Ueli Andrist
flames in both stages (rich and lean) were present, which (FHNW), Daniel Erne (PSI) and the late René Kaufmann (PSI).
eliminates any further flashback risk.

Optical measurement techniques also revealed that


homogeneous combustion also occurred in the rich stage,
suggesting that a catalyst is not required in the system for steady
operation. Furthermore, it was shown that without catalytic
coating homogeneous combustion could still be stabilized in the
rich stage nearly in the same way as with catalyst coating (the

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