Project Final Review · 2015-09-18 · Project Final Review A Coupled Measurement-Modeling Approach...
Transcript of Project Final Review · 2015-09-18 · Project Final Review A Coupled Measurement-Modeling Approach...
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Project Final Review
A Coupled Measurement-Modeling Approach to Improve Biogenic Emission Estimates:
Application to Future Air Quality Assessments
Huiting Mao, Ming Chen, Barkley Sive, Robert Talbot, Ruth Varner and Robert GriffinUniversity of New Hampshire
RTP, NCOctober 28, 2008
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Objectives
• To predict changes in climate that influence biogenic emissions and air quality.
• To quantify the impact of climate change on plant ecosystem composition.
• To estimate the impact of a changing plant ecosystem on biogenic emissions.
• To estimate the impact of changes in regional climate and plant ecosystem on aerosol loading, O3, NOx, hydrocarbons, and the oxidative capacity of the atmosphere.
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Ring 1Ambient CO2
Ring 2Elevated CO2
(Ambient+200 ppmv)
TRACK I: CO2 ENRICHMENT RESEARCH –Measurements at the Duke Forest FACTS-I site
Measurements at Duke Forest
NMHCsHalocarbonsAlkyl NitratesOVOCsO3NOCO2H2O
SOA & POA – number density, size distribution and composition (AMS, CN, filters)Black CarbonMet Data
3 Field Campaigns
1. Canopy: September 2004
2. Vegetation and Soil: June 2005
3. Soil: September 2005
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EDT9/15/04 9/17/04 9/19/04 9/21/04 9/23/04 9/25/04 9/27/04
Mix
ing
Rat
io (p
ptv)
0
1000
2000
3000
4000
5000
6000
Ring 1 ethane (ambient CO2)Ring 2 ethane (elevated CO2)
EDT9/15/04 9/17/04 9/19/04 9/21/04 9/23/04 9/25/04 9/27/04 9/29/04
Mix
ing
Rat
io (p
ptv)
0
50
100
150
200
250
300
C2Cl4 Ring 1 (ambient CO2)C2Cl4 Ring 2 (elevated CO2)
0
50
100
150
200
250
0 50 100 150 200 250
Ring 1 (pptv)
Slope = 1.02
r2=0.99
C2Cl4
0
50
100
150
200
250
0 50 100 150 200 250
Ring 1 (pptv)
Slope = 1.02
r2=0.99
C2Cl4
0
1000
2000
3000
4000
5000
6000
0 1000 2000 3000 4000 5000 6000
Ring 1 (pptv)
Slope = 0.99
r2=1.00
Ethane
0
1000
2000
3000
4000
5000
6000
0 1000 2000 3000 4000 5000 6000
Ring 1 (pptv)
Slope = 0.99
r2=1.00
Ethane
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EDT9/15/04 9/17/04 9/19/04 9/21/04 9/23/04 9/25/04 9/27/04
Mix
ing
Rat
io (p
ptv)
0
1000
2000
3000
4000
5000
6000
Ring 1 α-pinene (ambient CO2)Ring 2 α-pinene (elevated CO2)
EDT9/15/04 9/17/04 9/19/04 9/21/04 9/23/04 9/25/04 9/27/04 9/29/04
Mix
ing
Rat
io (p
ptv)
0
1000
2000
5000
6000
7000
Ring 1 isoprene (ambient CO2)Ring 2 isoprene (elevated CO2)
R2:R1 = 1.08
α-pinene: R2:R1 = 0.77β-pinene:R2:R1= 0.80
0
1000
2000
3000
4000
5000
6000
7000
0 1000 2000 3000 4000 5000
Ring 1 (pptv)
Slope = 1.08
r2=0.90
Isoprene
0
1000
2000
3000
4000
5000
6000
7000
0 1000 2000 3000 4000 5000
Ring 1 (pptv)
Slope = 1.08
r2=0.90
Isoprene
0
1000
2000
3000
4000
5000
0 1000 2000 3000 4000 5000 6000
Ring 1 (pptv)
Slope = 0.76
r2=0.83
α-pinene
0
1000
2000
3000
4000
5000
0 1000 2000 3000 4000 5000 6000
Ring 1 (pptv)
Slope = 0.76
r2=0.83
α-pinene
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Isoprene9/23/04
11am-6pm AverageMixing Ratio (pptv)
9/24/0411am-6pm Average Mixing Ratio (pptv)
Ring 1Ambient CO2 657 (± 80) 880 (± 79)Ring 2Elevated CO2 960 (± 135) 1112 (± 96)
Ring 2/Ring1 1.46 1.26
EDT9/23/04 9/24/04 9/25/04 9/26/04
Mix
ing
Rat
io (p
ptv)
0
500
1000
1500
2000Ring 1 isoprene (ambient CO2)Ring 2 isoprene (elevated CO2)
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Mixing Ratio (pptv)
0 2000 4000 6000 8000 10000 12000 14000
Hei
ght (
m)
0
5
10
15
20 Ring 2 (Elevated)Ring 3 (Elevated)Ring 4 (Elevated)Ring 1 (Ambient)Ring 5 (Ambient)Ring 6 (Ambient)
Mixing Ratio (pptv)
-2000 0 2000 4000 6000 8000 10000
Hei
ght (
m)
0
5
10
15
20
Elevated-Ambient (Ring 2-1)Elevated-Ambient (Ring 3-5)Elevated-Ambient (Ring 4-6)
June 5, 2005 16:00 (EDT)Isoprene
Comprehensive vertical profiles Rings 1-6 confirm elevated isoprene in elevated CO2 environment.
Difference betw Rings: 1 & 2, 3 & 5, and 4 & 6. All rings exhibit similar differencesRules out that: 1) vegetation distributions betw rings biasing results2) results are fortuitous.
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2.5
2.0
1.5
1.0
0.5
0.09/11/2004 9/16/2004 9/21/2004 9/26/2004
2.5
2.0
1.5
1.0
0.5
0.09/11/2004 9/16/2004 9/21/2004 9/26/2004
• Ring 1 (ambient CO2 )
• Ring 2 (elevated CO2 )M
ixin
g R
atio
(ppb
v)M
ixin
g R
atio
(ppb
v)20 m
16 m
PTR-MS MVK + MACR
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• Below-canopy profiles of a suite of VOCs measured.
• Source of reactive alkenes in the lower forest canopy/soil in the elevated CO2 ring.
• Some uptake of isoprene near the surface.
Propene (pptv)0 100 200 300 400
0
5
10
15
20
Ethene (pptv)0 200 400 600 800 1000
Hei
ght (
m)
0
5
10
15
20
Isoprene (pptv)0 200 400 600 800 1000 1200 1400
0
5
10
15
20
1-butene (pptv)0 10 20 30 40 50 60
Hei
ght (
m)
0
5
10
15
20 Ring 1Ring 2
β-pinene (pptv)
0 50 100 150 200 250 300 350
0
5
10
15
20
α-pinene (pptv)
0 200 400 600 800 1000
Hei
ght (
m)
0
5
10
15
20
Ring 1Ring 2
Ring 1Ring 2
Ring 1Ring 2
Ring 1Ring 2
Ring 1Ring 2
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Hour of Day (EDT) 00:00 04:00 08:00 12:00 16:00 20:00
Flux
(ug
g-1
h-1 )
0
1
2
3
4
5Ring 1Ring 2
Loblolly Pineα-pinene
Hour of Day (EDT) 00:00 04:00 08:00 12:00 16:00 20:00
Flux
(ug
g-1
h-1 )
0
20
40
60
80
100
120Ring 1Ring 2
isoprene
Sweetgum
Emission Fluxes
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a-Pinene b-Pinene
Emis
sion
Flu
x, u
g m
-2 d
-1
0
2000
4000
6000
8000
10000
12000
14000
16000
377 ppmv CO2600 ppmv CO2
Camphene Limonene
Emis
sion
Flu
x, u
g m
-2 d
-1
0
100
200
300
400
500
600
Duke Forest - Loblolly Pine
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Net CO2 Flux(mmol m-2 d-1)
-600 -300 0 300 600
Net
OC
S F
lux
(nm
ol m
-2 d
-1)
-300
-200
-100
0
100
PAR > 10 μmol m-2 s-1
PAR < 10 μmol m-2 s-1
High Respiration
Ring 2: Sweetgum
R2 = 0.70
Ambient OCS
0 150 300 450
Net
OC
S F
lux
(nm
ol m
-2 d
-1)
-450
-300
-150
0
150
PAR > 10 μmol m-2 s-1
PAR < 10 μmol m-2 s-1
Ring 2: Loblolly Pine
R2 = 0.66
OCS uptake is tree species-dependent: ambient OCS level for Loblolly pine and net CO2 flux for sweetgum. White et al., 2008, ACPD, in review
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ng C
H3I
m-2
d-1
40
60
80
100
120
140
160
180
ug Isoprene m-2 d
-1
0
5000
10000
15000
20000
25000Loblolly PineSweetgumSweetgum (Isoprene)
Local Time (EDT)
00:00 04:00 08:00 12:00 16:00 20:00 00:00
PAR
, umol m
-2 s-1
0
200
400
600
800
1000
1200
1400
umol
CO
2 m
-2 s
-1
-1
0
1
2
3
PARLoblolly PineSweetgum
a)
b)
Emissions of CH3I from the two tree species were comparable, but with a distinct diurnal cycle from Loblolly Pine and none from Sweetgum (emission not stomatally driven).
The average CH3I flux from mid-latitude vegetation and soils similar in magnitude to previous estimates of the oceanic source strength.
Sive et al. [2007], GRL
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Biogenic Emissions ares a Significant Source of Summertime Atmospheric Toluene
15 20 25 30 35 40
-2000
200400600800
100012001400
6/4/2005 12:00 6/5/2005 12:00 6/6/2005 12:00-200
0
200
400
600
800
1000
1200
0.0
3.0x105
6.0x105
9.0x105
1.2x106
1.5x106
tolu
ene
flux
(nm
ol m
-2 d
-1)
enclosure temperature (oC)
y = -600 +40xR2 = 0.73
b)
tolu
ene
flux
(nm
ol m
-2 d
-1)
local time (UTC-4:00)
net Toluene Flux
a)
α-p
inen
e flu
x (n
mol
m-2 d
-1)
net α-pinene Flux
1/1/2004 7/1/2004 1/1/2005 7/1/2005 1/1/2006 7/1/2006 1/1/20070.1
1
10
ethy
ne/C
O (p
ptv/
ppbv
)to
luen
e/be
nzen
e (p
ptv/
pptv
)
local date and time
ethyne/CO 15 day ethyne/CO ave. toluene/benzene 15 day toluene/benzene ave.
White et al., 2008, ACP
Toluene from
Fuel Evaporation Toluene from Crop
Plant Emissions Toluene from Pine
Tree Emissions Summer Toluene
Enhancement Year (pptv d-1) (pptv d-1) (pptv d-1) (pptv d-1) 2004 22 ±7 5 ±0.3 12 ±7 21 ±6 2005 16 ±6 5 ±0.3 12 ±7 43 ±9 2006 30 ±10 5 ±0.3 12 ±7 50 ±10
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Days in September
R2-R1:
6.4±5.5 ppbv
O3, NO
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MM Simulated O3 Mixing Ratios
1. Box model results show that O3 levels in Ring 2 were increased by 2.4 ppbv±2.0 ppbv on average.
2. Ozone uptake by vegetation was increased in Ring 2 by 0.5±0.3 ppbv hr-1
on average compared to Ring 1 using the sap flux measurements.3. Overall, model only captured 37% of the observed O3 increases in Ring 2.
Compounds are missing from our VOC measurements that likely contributed to O3 production. Mao et al., 2008, to be submitted to ACP
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TRACK II – Regional Climate and Air Quality Assessment
For a future climate with doubled CO2:
1. More convective precipitation with higher intensity across the U.S.
2. Heavy precipitation events should become more frequent, and be distributed over fewer days with larger daily amounts.
3. The mean length of the drying period should increase from 1.78 days at present to 1.92 days, and the domain-wide maximum extended from 34 to 40 days.
4. The probability of flooding and droughts should increase in the future.
Chen et al. [2005], GRL
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CMAQ OA Module Improvement
Species Data points
Mean observation
(μg m-3)
Mean prediction (μg m-3)
Mean normalized gross error (MNGE)
Mean normalized bias (MNB)
CACM/MPMPO
CB4/SORGA
M
CACM/MPMPO
CB4/SORGA
M
CACM/MPMPO
CB4/SORGA
M
PM2.5 45 16.70 13.70 14.10 0.33 0.36 -0.17 -0.15
Sulfate 44 7.13 7.98 8.55 0.52 0.60 0.32 0.39
Nitrate 44 0.28 0.19 0.18 1.34 1.23 -0.06 -0.03
Ammonium 15 2.73 2.74 2.71 0.14 0.15 0.03 0.02
EC 44 0.80 0.39 0.39 0.52 0.52 -0.45 -0.45
OC 44 3.82 1.26 1.18 0.66 0.69 -0.66 -0.69
Chen et al. [2006], JGR
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2000 – 2004 Summertime Air QualityMap Types - Sea Level Pressure (mb)
Mean Daily Maximum O3
Hegarty et al., 2007, JGR
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Interannual Variability Reconstruction
r = - 0.94
CII (hPa)
Map Type III
Regression Analysis
Reconstruction of summer O3 level based on map type frequency and intensity reproduced 46% of interannual variability
O3k - mean per map type k
ΔO3km - O3 perturbation from CII
Fkm - Frequency per map type k per year m
( ) kmk
kmkmm FOOO ∑=
Δ+=5
1333
Hegarty et al., 200750
52
54
56
58
60
62
64
66
68
2000 2001 2002 2003 2004
Year
O3 (
ppbv
)
Obs. All Days
Obs. Class. Days
Rec. MT Freq.
Rec. MT Freq. +CII
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Surface 1h (a,b) and 8h (c,d) O3 Daily Maximums Averaged over 2001-2005
1-hr
8-hr
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Comparison of Domain Averaged Observed and Modeled 1h-O3 Daily Maxima
8h-O3 Daily Maxima Sample # MODOBS − ±σ OBS MOD RMSE AINDEX R
2001 55718 1.8±14 55 53 14 73 0.58 2002 56223 3.4±16 58 54 16 69 0.56 2003 57300 -0.3±14 52 52 14 69 0.52 2004 55984 -4.7±13 46 51 13 65 0.51 2005 56505 -3.2±14 52 55 14 73 0.57 Total 282371 -0.6±14 52 53 14 71 0.54
Sample # MODOBS − ±σ OBS MOD RMSE AINDEX R 2001 55718 2.3±17 62 60 17 68 0.48 2002 56223 5.5±18 65 60 19 66 0.53 2003 57300 1.7±15 59 57 15 70 0.52 2004 55984 -3.6±15 52 56 15 64 0.46 2005 56505 -2.5±17 58 61 17 71 0.51 Total 282371 0.7±17 59 59 17 69 0.51
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Cumulative Distribution of Frequency (%)0 10 20 30 40 50 60 70 80 90 100
O3 (
ppbv
)
0
30
60
90
120
150
180
1hO3 Obs1hO3 Mod8hO3 Obs8hO3 Mod
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Example:IONS Ozonesonde
vs. Model
O3 (ppbv)0 50 100 150 200 250
Alti
tude
(km
)
0
2
4
6
8
10
ModObs
Average over all sites
a.) Beltsville, MD
0 50 100 150 200 250
Altit
ude
(km
)0
2
4
6
8
10
12
obsmod
b.) Hunstville, AL
0 50 100 150 200 2500
2
4
6
8
10
12
obsmod
c.) Narragansett, RI
0 50 100 150 200 2500
2
4
6
8
10
12
obsmod
e.) Ron Brown
O3 (ppbv)0 50 100 150 200 250
0
2
4
6
8
10
12
obs mod
f.) Wallops Island, VA
O3 (ppbv)0 50 100 150 200 250
0
2
4
6
8
10
12
obsmod
d.) Pellston, MI
O3 (ppbv)0 50 100 150 200 250
Alti
tude
(km
)
0
2
4
6
8
10
12
obsmod
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Future Projection of Global and US Anthropogenic Emissions
IPCC A2 2000 2090 Change (%)VOCs (Tg yr-1) 141 309 120NOx (Tg(N) yr-1) 32 98 207
VOCs (OECD90) 40 52 29
NOx (OECD90) 13 18 38
Case Scenarios
Future Climate Change and Its Impact on Air Quality
Present (Case 1)
Future (Case 2)
Future (Case 3)
Future (Case 4)
Future (Case 5)
Climate P F P F F Emissions P F F P-Einv, F-Bio P BC P P P P P
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IsoprenePresent
TerpenesPresent
TerpenesFuture-Present
IsopreneFuture-Present
moles s-1
Biogenic Emissions
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Daily Maximum 1h- and 8h-O3
O3 (ppbv) 0 10 20 30 40 50 60 70 80 90 100
Cum
ulat
ive
Dis
tribu
tion
of F
requ
ency
(%)
0
10
20
30
40
50
60
70
80
90
100
1hO3 Baseline1hO3 FClim_FEinv1hO3 CClim_FEmis1hO3 FClimž_CEinv1hO3 FClim_CEmis8hO3 Baseline8hO3 FClim_FEinv8hO3 CClim_FEmis8hO3 FClimž_CEinv8hO3 FClim_CEmis
Present (Case 1)
Future (Case 2)
Future (Case 3)
Future (Case 4)
Future (Case 5)
Median 31/60 25/66 28/67 30/64 29/62 4th highest 41/91 40/99 41/101 40/93 40/89
2.5th 13/44 9/46 9/45 14/45 14/45 25th 25/54 19/58 21/59 24/56 24/55 75th 37/71 33/79 37/78 36/75 36/71
97.5th 41/96 40/103 41/108 40/99 40/93
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Seasonal Mean Daily Maximum 8h-O3 Levels
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Average Mean Temperature and Surface Pressure Levels
The area of largest increases in O3 coincides with that of positive pressure changes in spite of uniform increases in anthropogenic O3precursors.
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Publications• Chen, M., H. Mao, and R. Talbot (2005), Changes in precipitation
characteristics over North America for doubled CO2, Geophys. Res. Lett., 32, L19716, doi:10.1029/ 2005GL024535.
• Mao, R. Talbot, D. Troop, B. Moore, R. Johnson, S. Businger, and A. M. Thompson (2006), Smart Balloon Observations over the North Atlantic: Part II – O3 Data Analysis and Modeling, J. Geophys. Res., 111, D23S56, doi:10.1029/2005JD006507.
• Hegarty, J., H. Mao, and R. Talbot (2007), Relationships between circulations patterns and surface ozone over the northeastern United States,J. Geophys. Res., 112, D14306, doi:10.1029/2006JD008170.
• Chen, J., H. Mao, R.W. Talbot, and R.J. Griffin (2006), Application of the CACM and MPMPO modules using the CMAQ model for the Eastern United States, J. Geophys. Res.,111, D23S25, doi:10.1029/2006JD007603.
• Sive, B. C., R. K. Varner, H. Mao, D. R. Blake, O. W. Wingenter, and R. Talbot (2007), A large terrestrial source of methyl iodide, Geophys. Res. Lett., 34, L17808, doi:10.1029/2007GL030528.
• Sive, B. C., R. K. Varner, L. C. Nielsen, R. S. Russo, Y. Zhou, M. L. White, A. Csakai, P. Beckman, J. Ambrose, O. W. Wingenter, H. Mao and R. Talbot (2006), Isoprene and monoterpene emissions in ambient and future CO2 environments, in preparation for submission to Atmos. Chem. Phys.
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Continued
• White, M. L., B. C. Sive, R. K. Varner, R. S. Russo, Y. Zhou, A. Csakai, P. Beckman, J. Ambrose, O. W. Wingenter, H. Mao and R. Talbot (2008a), Methyl halides and OCS exchange with soil and trees at the Duke Forest FACE site, Chapel Hill, NC, ACPD, in review.
• White, M. L., et al. (2008b): Are Biogenic Emissions a Significant Source in Summertime Toluene Enhancements in the Rural Northeast? ACPD, in review.
• Chen, M. et al., (2008), Characteristics Climate Change Patterns over Regions of Upwind Pollutants Sources and Their Impact on Regional Air Quality over New England, in preparation for submission to J. Geophys. Res.
• Mao, H., R. Talbot, B. Sive, R. Varner, M. Chen, R. Oren, and H.-S. Kim (2008a), Enhanced O3 in an elevated CO2 environment, in preparation for submission to Atmos. Chem. Phys.
• Mao, H., M. Chen, and R. Talbot (2008b), Air quality assessment for the northeastern United States, in preparation for submission to Atmos. Chem. Phys.
• Mao, H., M. Chen, and R. Talbot (2008c), Present and future air quality assessment for the northeastern United States, in preparation for submission to Atmos. Chem. Phys.
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Acknowledgement
• Laura Cottrell• Pieter Beckman• Tod Hagan• All graduate students and technicians from
Climate Change Research Center who participated in the project.