Improved estimate of the policy-relevant background ozone in the United States using the GEOS-Chem global model with 1/2° x 2/3° horizontal resolution over North America

摘要

The policy-relevant background (PRB) ozone is defined by the US Environmental Protection Agency (EPA) as the surface ozone concentration that would be present over the US in the absence of North American anthropogenic emissions. It is intended to provide a baseline for risk and exposure assessments used in setting the National Ambient Air Quality Standard (NAAQS). We present here three-year statistics (2006-2008) of PRB ozone over the US calculated using the GEOS-Chem global 3-D model of atmospheric composition with 1/2° ×2/3° horizontal resolution over North America and adjacent oceans (2°×2.5° for the rest of the world). We also provide estimates of the US background (no anthropogenic US emissions) and natural background (no anthropogenic emissions worldwide and pre-industrial methane). Our work improves on previous GEOS-Chem PRB estimates through the use of higher model resolution, 3-year statistics, better representation of stratospheric influence, and updated emissions. PRB is particularly high in the intermountain West due to high elevation, arid terrain, and large-scale subsidence. We present for this region a detailed model evaluation showing that the model is successful in reproducing ozone exceedances up to 70 ppbv. However, the model cannot reproduce PRB-relevant exceptional events associated with wildfires or stratospheric intrusions. The mean PRB estimates for spring-summer are 27±8 ppbv at low-altitude sites and 40±7 ppbv at high-altitude sites. Differences between the PRB simulation and the natural simulation indicate a mean enhancement from intercontinental pollution and anthropogenic methane of 9 ppbv at low-altitude sites and 13 ppbv at high-altitude sites. The PRB is higher than average when ozone exceeds 60 ppbv, particularly in the intermountain West. Our PRB estimates are on average 4 ppbv higher than previous GEOS-Chem studies and we attribute this to higher lighting, increasing Asian emissions, and improved model resolution. Whereas previous studies found no occurrences of PRB exceeding 60 ppbv, we find here some occurrences in the intermountain West. The annual 4th-highest PRB values in the intermountain West are typically 50-60 ppbv, as compared to 35-45 ppbv in the East or on the West Coast. Such high PRB values in the intermountain West suggest that special consideration of this region may be needed if the ozone NAAQS is decreased to a value in the 60-70 ppbv range.