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Purdue University
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Development Of All-Solid-State Sensors for Measurement of Nitric Oxide and Ammonia Concentrations by Optical
Absorption in Particulate-laden Combustion Exhaust Streams
Development Of All-Solid-State Sensors for Measurement of Nitric Oxide and Ammonia Concentrations by Optical
Absorption in Particulate-laden Combustion Exhaust Streams
Robert P. LuchtSchool of Mechanical Engineering, Purdue
University, West Lafayette, IN
University Coal Research Contractors Review Conference
Pittsburgh, PA June 9, 2004
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Acknowledgements Acknowledgements
• This research was supported by the U. S. Department of Energy through the University Coal Research Program under Grant #DE-FG26-02NT41535.
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ParticipantsParticipants
• Rodolfo Barron-Jimenez, Soyuz Priyadarson, Senthilvasan Arumugam, Jerry Caton, Kalyan Annamalai (Texas A&M University)
• Thomas Anderson, Robert Lucht (Purdue University)
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Outline of the Presentation Outline of the Presentation
• Introduction and Motivation• Diode-Lased-Based Sensors • Laboratory Gas Cell Measurements• Field Demonstrations:
-APU Gas Turbine at Honeywell -Coal Combustor at Texas A&M
• Conclusions and Future Work
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Motivation for the Work Motivation for the Work • Optical absorption sensors have the
capability of in-situ, real-time measurements of NO and NH3, potential for incorporation into combustor control systems
• NO absorption band in ultraviolet at 226 nm, fundamental NH3 band at 3 microns are very strong, sub-ppm sensitivity achievable for high-resolution absorption measurements.
• Recent advances in laser technology make development of high-resolution ultraviolet sensor systems feasible, much development also in mid-infrared.
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NO Infrared Absorption NO Infrared Absorption
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NO Ultraviolet Absorption NO Ultraviolet Absorption
226 nm
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NO Sensor SystemNO Sensor System
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NO Sensor SystemNO Sensor System
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Signal and Reference Beams:100 ppm NO in Gas Cell
Signal and Reference Beams:100 ppm NO in Gas Cell
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Theory vs. Experiment:100 ppm NO, 2.4 kPa in Gas Cell
Theory vs. Experiment:100 ppm NO, 2.4 kPa in Gas Cell
1 23
No. Line
1 P2(4) andPQ12(4)
2 P2(3) andPQ12(3)
3 P2(5) andPQ12(5)
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Field Demonstration: Honeywell Gas Turbine Engine
Field Demonstration: Honeywell Gas Turbine Engine
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Field Demonstration: Honeywell Gas Turbine Engine
Field Demonstration: Honeywell Gas Turbine Engine
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Field Demonstration: Honeywell Gas Turbine Engine
Field Demonstration: Honeywell Gas Turbine Engine
• Sensor system operated remotely because of high level of noise and vibrations in test cell
• Compared results with chemiluminescent analyzer
• Tuned laser to probe P2(10) and PQ12(10) transition of NO
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Gas Turbine Measurements:High Load Condition
Gas Turbine Measurements:High Load Condition
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Gas Turbine Measurements:Low Load Condition
Gas Turbine Measurements:Low Load Condition
0
0.01
0.02
0.03
0.04
0.05
-20 -10 0 10 20
Absorption 1Absorption 2Theory
Nor
mal
ized
Abs
orpt
ion
Frequency Detuning (GHz)
Absorption Results: X
NO = 14.4 ppm
Temp = 610 K
2γ = 0.6 cm-1/atm
∆νd = 0.14 cm-1
Probe Results: X
NO = 8.1 ppm
Temp = 586-599 K
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Modified Boiler Burner FacilityModified Boiler Burner FacilitySecondaryAir Blower
Fuel Hopper
Venturi
Primary Air Temperature Ports
Propane Ignition Torch
FlexibleExhaust Duct Laser
Apparatus
Optical Table
Water Spray ExhaustParticulate Trap
Laser Beam
Alternate Optional WaterSpray Particulate Trap
Exhaust Fan
To Atmosphere
SCHEMATIC SKETCH OF TAMU 30 kWt (100,000 Btu/hr) BOILERBURNER FACILITY MODIFIED FOR LASER MEASUREMENTS
Gas SamplingPorts
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LaserApparatus
Optical Table
Water Spray ExhaustParticulate Trap
Laser Beam
Alternate Optional WaterSpray Particulate Trap
Exhaust Fan
To Atmosphere
Gas SamplingPorts
Modified Boiler Burner FacilityModified Boiler Burner Facility
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NO Measurements in Particle-LadenExhaust Flow from Coal CombustorNO Measurements in Particle-LadenExhaust Flow from Coal Combustor
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NO Measurements in Particle-LadenExhaust Flow from Coal CombustorNO Measurements in Particle-LadenExhaust Flow from Coal Combustor
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NO Measurements in Particle-LadenExhaust Flow from Coal CombustorNO Measurements in Particle-LadenExhaust Flow from Coal Combustor
05
10152025303540
02468101214
-0.05 0 0.05 0.1 0.15
Sign
al, R
ef. I
nten
sitie
s (a
rb. u
nits
) Etalon, E
CD
L Ram
p (arb. units)
Time (sec)
Reference
Signal x 9.97Ramp Etalon
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NO Measurements in Particle-LadenExhaust Flow from Coal CombustorNO Measurements in Particle-LadenExhaust Flow from Coal Combustor
0.1
0.2
0.3
0.4
0.5
-15 -10 -5 0 5 10 15
Absorption 1Absorption 2Theory
Abso
rptio
n
Frequency Detuning (GHz)
AbsorptionMeasurements: x
NO = 108 ppm
∆νc = 0.6 cm-1/atm
Path length = 0.610 m Scaling Factor = 4.61
Probe and Thermocouple: Exhaust Temp = 157 F (center) x
NO = 154 ppm (center)
xNO
= 112 ppm (path-averaged)
SingleSweep
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NO Measurements in Particle-LadenExhaust Flow from Coal CombustorNO Measurements in Particle-LadenExhaust Flow from Coal Combustor
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0.1
0.2
0.3
0.4
0.5
-15 -10 -5 0 5 10 15
Absorption 1Absorption 2Theory
Abso
rptio
n
Frequency Detuning (GHz)
Probe and Thermocouple: Exhaust Temp = 157 F (center) x
NO = 154 ppm (center)
xNO
= 112 ppm (path-averaged)
AbsorptionMeasurements: x
NO = 102 ppm
∆νc = 0.57 cm-1/atm
Path length = 0.610 m Scaling Factor = 9.97
8 Sweeps
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NO Measurements in Particle-LadenExhaust Flow from Coal CombustorNO Measurements in Particle-LadenExhaust Flow from Coal Combustor
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0.1
0.2
0.3
0.4
0.5
-15 -10 -5 0 5 10 15
Absorption 1Absorption 2Theory
Abso
rptio
n
Frequency Detuning (GHz)
Probe and Thermocouple: Exhaust Temp = 157 F (center) x
NO = 154 ppm (center)
xNO
= 112 ppm (path-averaged)
AbsorptionMeasurements: x
NO = 93 ppm
∆νc = 0.59 cm-1/atm
Path length = 0.610 m Scaling Factor = 4.11
32 Sweeps
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Spatial Profile of NO Concentration in Particle-Laden Exhaust Flow
Spatial Profile of NO Concentration in Particle-Laden Exhaust Flow
-50
0
50
100
150
200
-0.2 -0.15 -0.1 -0.05 0 0.05 0.1 0.15 0.2
NO Concentration Gradient
NO
Con
cent
ratio
n, P
robe
(ppm
)
Distance x Along Absorption Path Length (m)
Win
dow
Win
dow
Win
dow
Pu
rge
Ape
rture
Win
dow
Pur
ge
Aper
ture
CNO
= 163 - 1846.5 x2 - 2.2182e+05 x4
NO measured by probe sampling and electrochemicalcell analysis at five different spatial locationsalong absorptionbeam path.
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ConclusionsConclusions
• New Sensor for NO Applied in TAMU Boiler Burner Facility
- Measurements were performed successfully even with severe (> 1% transmission) attenuation of the ultraviolet beam
- NO ultraviolet absorption measurements were in good agreement with probe measurements
- Single-sweep, 0.1 sec measurements demonstrated, data rate limited by mechanical tuning of the ECDL
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Future Work Future Work
• Increase Tuning Range and Tuning Rate of Sensors –Second Set of NO Sensor Measurements in Progress- Incorporate new ECDL from Sacher Laser with 90
GHz mode-hop-free tuning range
• Develop Mid-Infrared Sensor for NH3 for Optimization and Control of Thermal DeNox Process- Mid-infrared NH3 sensor will be very similar to
mid-infrared CO sensor that we have developed
• Decrease Total Acquisition Time by Improving Processing and Acquisition Routines
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Second Set of NO Measurements Second Set of NO Measurements
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Second Set of NO Measurements Second Set of NO Measurements
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ECDL with Extended Mode-Hop-Free TuningECDL with Extended Mode-Hop-Free Tuning
-1
-0.5
0
0.5
1
1.5
0
0.02
0.04
0.06
0.08
0.1
0.12
0.14
0 0.001 0.002 0.003 0.004 0.005
Ram
p Vo
ltage
to G
ratin
g Pi
ezo Etalon O
utput (2 GH
z FSR
)
Time (sec)
New 395-nmECDL with mode-hop-free tuning range up to 90 GHz, can be scanned at rates up to 1 kHz.
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NO Absorption in Gas Cell with New ECDLNO Absorption in Gas Cell with New ECDL
0
0.05
0.1
0.15
0.2
-50 0 50
15 Hz Scan Rate, Q2(10) Line at 44127.49 cm -1
AbsorptionTheory
Abs
orpt
ion
Frequency Detuning (GHz)
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NH3 Sensor System1064-nm telescope
785-nm ECDL
550 mW 1064-nm Crystalaser
Reference InSb Detector
50-50 Beam Splitter
PPLN crystal (oven)
Faraday IsolatorSpectrum Analyzer
Dichroic mirrorOptical Chopper
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NH3 Sensor SystemPPLN crystal and oven
785-nm ECDL
550 mW 1064-nm Crystalaser
ECDL Drive Electronics
DigitalOscilloscope
PC
CombustorExhaust
Faraday Isolator
Mirror
Long Wave Pass Filter
Reference InSb Detector
Spectrum Analyzer
Optical Chopper
1064-nm telescope
Half- Wave plates
Dichroic mirror 50-50 Beam Splitter
LensSignal InSb Detector
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Theoretical NH3 SpectrumTheoretical NH3 Spectrum
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0.03
0.04
3.06 3.065 3.07 3.075 3.08 3.085 3.09 3.095
Theo
retic
al A
bsor
ptio
n
Wavelength [µm]
Temp = 300 K Pressure = 101.3 kPaX
NH3 = 1000 ppm Pathlength = 0.32 m
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CO Sensor SystemCO Sensor System
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CO Sensor SystemCO Sensor System
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CO Sensor SystemCO Sensor System
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Laboratory Gas Cell Measurements:1000 ppm CO at 13.35 kPa
Laboratory Gas Cell Measurements:1000 ppm CO at 13.35 kPa
R(24) Transitionat 2227.639 cm-1
