PNNL

Abstract

The 2000 and 2006 Texas Air Quality Study (TexAQS 2000 and 2006) field campaigns took place in eastern Texas in August-October of 2000 and 2006. Several flights of the National Oceanic and Atmospheric Administration (NOAA) and National Center for Atmospheric Research (NCAR) research aircraft were dedicated to characterizing anthropogenic emissions over Houston. Houston is known for having serious problems with non-attainment of air quality standards. We present a method that uses three models and aircraft observations to assess and improve existing emission inventories using an inverse modeling technique. We used 3-dimensional and 4-dimensional variational (3D-VAR and 4D-VAR) inverse modeling techniques based on a least-squares method to improve the spatial and temporal distribution of CO, NOy (sum of all reactive nitrogen compounds), and SO2 emissions predicted by the 4-km-resolution U.S. Environmental Protection Agency (EPA) National Emission Inventory (NEI) for 2005. Differences between the prior and posterior inventories are discussed in detail. We found that in 2006 the prior daytime emissions in the urban area of Houston have to be reduced by 40%±12% for CO and 7%±13% for NOy. Over the Houston Ship Channel, where industrial emissions are predominant, the prior emissions have to be reduced by 41%±15% for CO and 51%±9% for NOy. Major ports around Houston have their NOy emissions reduced as well, probably due to uncertainties in near-shore ship emissions in the EPA NEI inventory. Using the measurements from the two field campaigns, we assessed the interannual emission variability between 2000 and 2006. Daytime CO emissions from the Houston urban area have been reduced by 8%±20%, while the NOy emissions have increased by 20%±12% from 2000 to 2006. In the Houston Ship Channel, the daytime NOy emissions have increased by 13%±17%. Our results show qualitative consistencies with known changes in Houston emissions sources.