euphore chamber in spain (204m 3` x 2) swiss indoor chamber (27m 3 )
DESCRIPTION
New Indoor and Outdoor Smog Chambers Costs, advantages/disadvantages and types of things one can study. EUPHORE Chamber in Spain (204m 3` x 2) Swiss Indoor Chamber (27m 3 ) Caltech indoor chamber (28m3 EPA-RTP indoor chamber indoor (14.5m 3 ) UNC -outdoor chamber (135m 3 x2) - PowerPoint PPT PresentationTRANSCRIPT
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New Indoor and Outdoor Smog Chambers
Costs, advantages/disadvantages and types of things one can study
• EUPHORE Chamber in Spain (204m3`x 2)• Swiss Indoor Chamber (27m3)• Caltech indoor chamber (28m3• EPA-RTP indoor chamber indoor (14.5m3)• UNC-outdoor chamber (135m3x2)• UCR-CERT indoor (90m3x2)
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The European PhotoreactorEUPHORE (1996)
• Largest outdoor chamber (204 m3)• FEP film with a thickness of 0.127 mm (80%
transmission)• Positive pressure (100-200 Pa)• State of the art instrumentation
DOAS (O3, NO2, HCHO, HONO) , long-path FT-IRTDL (tunable diode laser)
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This image shows one of the two chambers of EUPHOR
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The European PhotoreactorEUPHORE (1996)
• K.H. Becker / Project Co-cordinator [email protected]
• J. Hjorth [email protected] • G. Laverdet [email protected] • M.M. Millán [email protected] • U. Platt [email protected]
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Caltech new Indoor chambers(Cocker and Seinfeld et al, ES&T 35, 2594,2001)
• Two 28m3 meters• 2 ml FEP Teflon wall• Controlled aerosol injection system• Indoor lights
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William Carter aerosol chambers
• two collapsible 90m3 FEP Teflon film reactors inside an outer enclosure.
• Solar radiation is simulated with either a 200kW Argon arc lamp or multiple black lamps.
• Collapsible system, positive 5 pa, Outer enclosure flushed with clean air to reduce input of dirty air from outside; temp controlled from 5-45oC
• mechanism evaluation data for experiments with NOx levels as low as 2 ppb
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New UNC outdoor aerosol dual chamber
• Quonset Hut design; 270 m3 FEP Teflon film chambers.
• Natural sunlight • Exchange rate with outside air 0.5 to 1.5%/hour• Particle half-live of 17 hours• Design permits chamber walls to be easily washed
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Dual 270m3 chamber fine particle t 1/2 >17 h
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New UNC aerosol smog chamber
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Major costs for any chamber system
• NOx, O3 $24,000• 4 GC and GCMSs 200,000• 6 nm to 900 nm particles 85,000• 0.3 to 5 um particles 25,000• Data system 3,500• Light and Dew point 6,000• Flow meters, etc 10,000• 6 place balance 12,000• Clean air generator 20,000• Denuders and filter holders 10,000• Total = ~$ 400,000• Build a new chamber ~50,000-100,000
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Need an analytical and an modeling group
•
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Research Issues that can be studied in Environmental Chambers
• Chemical mechanisms• Product studies• Effects of light, temperature and
water vapor• Generate data for modeling studies
– Simple compounds – Complex mixtures
• Gases and particle interactions
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Problems with Environmental Chambers
• Wall effects
• Care is needed to extend results to the atmosphere.
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• Wall effectsAldehydes, HONO can off gas from the walls
wet walls adsorb more aldehydes and NOX
outer sheath of clean air
purchase a “clean batch” of Teflon film
have a chamber design that permits cleaning
run characterization tests before and after cleaning (O3 decay)
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What are some historical uses for Environmental Chambers
• Test and develop gas phase chemical mechanisms
• Develop product information and yields
• Reactivity
• Evaluate aerosol formation– Aerosol products– Aerosol kinetic mechanisms
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The Chamber had two sides
Or Darkness 300 m3 chamber
Teflon Film walls
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The Chamber had two sides
Or Darkness
Formaldehyde
propylene
300 m3 chamber
Teflon Film walls
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The Chamber had two sides
Or Darkness
Formaldehyde
propylene
300 m3 chamber
Teflon Film walls
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The Chamber had two sides
Or Darkness
Formaldehyde
propylene
300 m3 chamber
Teflon Film walls
NO &NO2
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Example experiment with the following chamber concentrations:
• NO = 0.47 • NO2 = 0.11 ppm• Propylene = 0.99 ppmV• temp = 15 to 21oC
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Solar Radiation Profile
-0.2
0
0.2
0.4
0.6
0.8
1
1.2
cal c
m-2
min
-1
6 8 10 12 14 16 time in hours
TSR
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Example Mechanism NO2+ hNO + O. k1 keyed to sunlight
O. + O2 --> O3 k2
O3 +NO2 --> NO + O3 k3
H2C=O + h --> .HC=O + H. k4 keyed to sunlight
H. +O2 --> HO2. k5
HO2. + NO --> NO2+OH. k6 (fast) OH.+ C=C ---> H2C=O + HO2
+ H2COO. k7
• dNO2/dt = -k1[NO2]; NO2=-k1 [NO2] t
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Photochemical System
0
0.1
0.2
0.3
0.4
0.5
0.6 pp
m
10 11 12 13 14 15 time in hours
NO-data O3-mod NO2-data
O3-data NO-mod NO2-mod
NOx-O3: model vs. data
PAN
NO2O3
NO
NO2
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Photochemical System
0
0.2
0.4
0.6
0.8
1
1.2
ppm
V
10 11 12 13 14 15 Time in hours
Propylene: data vs. model
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Studying AEROSOLS IN Chambers
• Ambient data often guides experiments
• Our understanding of aerosol formation is ~20 years behind gas phase chemistry
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PM10 Chemical Characterization in Beijing Xiao-Feng, Min Hua, Ling-Yan Hea, Xiao-Yan
Tang, Atmos. Environ. 39 (2005) 2819–2827
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Characteristics of carbonaceous aerosols in Beijing, ChinaYele Suna, Guoshun Zhuang, Ying Wang, Lihui Han, Jinghua Guo, Mo Dan, Wenjie Zhang, Zifa Wang, Zhengping Hao, Atmos, Environ. 38 (2004) 5991–6004
• coal burning, traffic exhaust, and dust from the long-range transport, were the major sources of the aerosol pollution in Beijing.
• Mineral aerosol from outside Beijing accounted for 79% of the total PM10 minerals and 37% of the PM2.5 in winter. It was 19% and 20% in summer
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Characteristics of carbonaceous aerosols in Beijing, ChinaFengkui Duan, Kebin He, Yongliang Ma, Yingtao Jia,Fumo Yang, Yu Lei, S. Tanaka, T. Okuta, Chemosphere 60 (2005) 355–364
• OC/EC ratio (on a 1.5 basis showed that SOC accounted more than 50% for the total organic carbon. In winter, the SOC contribution to OC was also significant, and as high as 40%.
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Characteristics of carbonaceous aerosols in Beijing, ChinaYele Suna, Guoshun Zhuang, Ying Wang, Lihui Han, Jinghua Guo, Mo Dan, Wenjie Zhang, Zifa Wang, Zhengping Hao, Atmos, Environ. 38 (2004) 5991–6004
• PM2.5/PM10 ratios were 0.45–0.48 in summer and 0.52–0.73 in winter
• in winter. SO4 , NO3, NH4, OC,crustal matter, and EC were the six dominant species
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Can we chemically and kinetically model Secondary Organic Aerosol Formation???
• Numerical fitting• Semi-explicit
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From a modeling perspective Equilibrium Organic Gas-particle partitioning provides a context for addressing SOA formation
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Gas/Particle Partitioning
particleand particleChemical nature of gasTemperature
Humidity
gas
Thermodynamic Equilibrium?
TSPCC
Kgas
partp
Cgas +surf Cpart
Kp will vary with 1/Po
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Odum-Seinfeld Model SOA model
Y= MY= Moo / / HC HC
Y Y MK
K Mii
oi om i
om i oi
,
,( )1
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- pinene- NOx experiments by OdumY Mo(g/m3)
1 0.012 1
2 0.028 8
3 0.056 22
4 0.067 34
5 0.081 38
6 0.116 83
7 0.122 94
Y MK
K M MK
K Moom
om oo
om
om o
1 1
1
2 2
21 1,
,
,
,( ) ( )
Y = M= Moo / / HC HC
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-pinene
Y MK
K M MK
K Moom
om oo
om
om o
1 1
1
2 2
21 1,
,
,
,( ) ( )
How is this done?
1 = 0.038, Kom1= 0.17
2 = 0.326, Kom2 = 0.004
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Overall kinetic Mechanism
• links gas and particle phase rate expressions
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gas phase reactions min-1 or ppm-1 min-1
1-pinene + O3 .4 Criegee1 + .6 Criegee2 1.492 exp-732/T2. Criegee1 .3 pinacidgas + .15 stabcrieg1 + .8 OH + .5 HO2 + .3 pinaldgas + .25 oxy-pinaldgas + .3 CO 1x106
3. Criegee2 .35 crgprod2 + .5 oxy-pinaldgas +.35 HCHO + .15 stabcrieg2 +.8 OH + .5 HO2 1x106
4. stabcrieg1 + H2O pinacidgas 6x10-3
10. oxy-prepinacid +HO2 oxy-pinacid 677 exp1040/T16. pinacidgas {walls} 4x10-7 exp2445/T
partitioning reactions22. stabcrieg1 + pinaldgas seed1 29.5,25. pinacidgas + seed1 seed1 + pinacidpart 29.8,34. diacidgas + pinacidpart --> pinacidpart + diacidpart 68,35. diacidpart diacidgas 3.73x1014 exp-10285/T44. diacidpart {walls} 0.0008,
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Particle Phase reactions
particle
C=OO
cis-pinonaldhyde
C=OO
polymers
Gas phase reactions
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Particle Phase reactions
particle
C=OO
cis-pinonaldhyde
C=OO
polymers
Gas phase reactions
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Particle Phase reactions
C=OO
cis-pinonaldhyde
C=OO
polymers
Gas phase reactions
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Chemical System
-pinene
+ NOx+ sunlight + ozone----> aerosols
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0
0.2
0.4
0.6
0.8
1
ppm
V
9 9.2 9.4 9.6 9.8 10 Time in hours
Gas Phase -pinene and O3data and model
-pinene
MODEL
Warm high concentration experiment
MODEL
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Warm high concentration experiment
0
1
2
3
4
5
9 10 11 12 13 time in hours
A
model
Filter Data
Reacted -pinene
mg /
m3
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Other Temperature Conditions
0.82 ppmv -pinene + 0.60 ppm O3(295K)
0.60 ppmv -pinene + 0.65 ppm O3 (284K)
0.35 ppmv -pinene + 0.25 ppm O3 (295K)
0.88 ppmv -pinene + 0.47 ppm O3(269K)
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Daytime systems
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0.95 ppm -pinene + 0. 44ppm NOx
O3NO
NO2
NO2
model
data
Time in hours EST
ppm
V
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Gas phase pinonaldehdye
OO
mg/
m3
Time in hours EST
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Particle phase
model TSP
mg/
m3
Particle phase
model TSP
mg/
m3
Measured particle mass vs. model
data
Time in hours EST
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Indoor vs. Outdoor chambers: Advantages and disadvantages• Indoor chambers
– More controlled conditions– It is possible to change temperatures– Conduct more experiments– Difficult to maintain constant light conditions– Need a large building for a large chamber– Can be used in a dynamic mode to generate large
samples for product analysis
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Indoor vs. Outdoor chambers: Advantages and disadvantages
• Outdoor chambers – Can not control temperature– Temperature changes during the day– Conduct fewer experiments– Uses real sunlight – Large chambers can be used for longer
simulations