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Course: DJJ 2003, Fall 2009School: Harvard
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AEROSOL BACKGROUND IN THE UNITED STATES: NATURAL SOURCES AND TRANSBOUNDARY POLLUTION Daniel J. Jacob and Rokjin J. Park with support from EPRI, EPA/OAQPS How good are the "default estimated natural PM concentrations" proposed by EPA as 2064 endpoint for application of the Regional Haze Rule? To what extent does transboundary pollution compromise achievability of natural PM concentrations?...
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AEROSOL BACKGROUND IN THE UNITED STATES: NATURAL SOURCES AND TRANSBOUNDARY POLLUTION Daniel J. Jacob and Rokjin J. Park
with support from EPRI, EPA/OAQPS How good are the "default estimated natural PM concentrations" proposed by EPA as 2064 endpoint for application of the Regional Haze Rule? To what extent does transboundary pollution compromise achievability of natural PM concentrations?
2004-2018 EMISSION REDUCTIONS FOR THE RHR ARE STRONGLY SENSITIVE TO CHOICE OF 2064 ENDPOINT
Conceptual calculation for mean western U.S. conditions, assuming linear relationship between emissions and bext Desired trend in visibility
dv = 10 ln
bext ,natural + bext ,anthrop 10
Phase 1 48% 30%
Required % decrease of U.S. anthropogenic emissions
STRATEGY FOR QUANTIFYING BACKGROUND PM CONCENTRATIONS IN UNITED STATES
Start from best a priori estimates of natural and anthropogenic PM sources Simulate PM concentrations with GEOS-CHEM global model Improved emission estimates
Evaluate with observations from IMPROVE, CASTNET, other networks
Conduct sensitivity simulations Quantify natural aerosol concentrations Quantify transboundary pollution
GEOS-CHEM GLOBAL CHEMICAL TRANSPORT MODEL (http://www-as.harvard.edu/chemistry/trop/geos) Driven by NASA/GEOS-3 assimilated meteorological data with 2ox2.5o horizontal resolution, 48 levels in vertical Carbonaceous aerosol simulation (OC, EC) for 1998
Park, R.J., D.J. Jacob, M. Chin, and R.V. Martin, Sources of carbonaceous aerosols over the United States: implications for natural visibility, J. Geophys. Res.., 108, 4355, 2003.
Coupled oxidant sulfate-nitrate-ammonium simulation for 2001 (also 1998)
Park, R.J., D.J. Jacob, et al., Natural and transboundary influences on ammonium-sulfate-nitrate aerosols in the United States: implications for visibility, J. Geophys. Res., manuscript in preparation
CARBONACEOUS AEROSOL SIMULATION Best a priori sources (1998)
ORGANIC CARBON (OC) ELEMENTAL CARBON (EC)
GLOBAL
130 Tg yr-1
22 Tg yr-1
UNITED STATES 0.66 Tg yr-1
2.7 Tg yr-1
BIOMASS BURNING EMISSIONS IN GEOS-CHEM:
Climatology from Duncan, Logan, et al. [JGR 2002] scaled to 1998 using TOMS and ATSR satellite data Interannual variability derived from TOMS Aerosol Index [Duncan et al., 2002]
1998 fires from ATSR satellite data: Apr-May fires in Mexico Jul-Sep fires in U.S/Canada
SEASONAL VARIATION OF OC AND EC
Constrain OC/EC sources using simulation of monthly mean IMPROVE observations and model tracers of individual source types. IMPROVE model biomass burning vegetation fossil fuel biofuel
model tracers (additive)
LEAST-SQUARES FIT OF MODEL TO MONTHLY MEAN OC/EC OBSERVATIONS AT 45 IMPROVE SITES YIELDS OPTIMIZED A POSTERIORI SOURCES Fossil fuel 15% Biofuel 65% Biomass burning 17% Biogenic 11%
CARBONACEOUS AEROSOL IN THE U.S.:
contributions from natural sources and transboundary pollution
Annual regional means from GEOS-CHEM standard and sensitivity simulations OC (g m-3 as OMC) West East (1998) Baseline Background (no U.S. anthrop. emissions, climatological fires) Natural (no anthrop. emissions globally) Transboundary pollution enhancements Canada and Mexico Asia EPA default estimated natural concentrations 2.0 1.3 1.2 0.05 0.013 0.5 3.2 1.2 1.1 0.05 0.007 1.4 EC (g m-3 ) West 0.30 0.06 0.04 0.02 0.005 0.02 East 0.68 0.04 0.02 0.02 0.003 0.02
EPA default natural concentrations for OC are OK in eastern U.S., a factor of 23 too low in western U.S. quantifying fire influences is critical Transboundary pollution influences are relatively small
H2SO4-HNO3-NH3-H2O AEROSOL SIMULATION GEOS-CHEM emissions (2001)
GLOBAL UNITED STATES
78
Sulfur, Tg S yr-1
8.3
55
Ammonia, Tg N yr-1
2.8
43
NOx, Tg N yr-1
7.4
ANNUAL MEAN SULFATE (2001): GEOS-CHEM vs. IMPROVE (141 sites)
Highest concentrations in industrial Midwest (coal-fired power plants)
SULFATE AT IMPROVE, CASTNET, NADP (deposition) SITES: model vs. observed for different seasons
High correlation, no significant model bias except 25-30% negative bias in summer (we attribute it to excessive scavenging of SO2 in convective updrafts)
ANNUAL MEAN AMMONIUM (2001): GEOS-CHEM vs. CASTNET (79 sites)
(no ammonium data at IMPROVE sites)
Highest concentrations in upper Midwest (livestock)
ANNUAL MEAN NITRATE (2001): GEOS-CHEM vs. CASTNET (79 sites)
Highest concentrations in upper Midwest (NH4NO3 formation limited by ammonia availability)
Ammonium
Nitrate
Nitrate
AMMONIUM AND NITRATE AT CASTNET AND IMPROVE SITES: model vs. observed for different seasons
High bias for NH4+ in fall: excessive seasonal livestock emissions High bias for NO3-, esp. in summer/fall, results from bias on [SO42-]-2[NH4+]
SULFATE-NITRATE-AMMONIUM AEROSOL IN THE U.S.:
contributions from natural sources and tra...
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