A new inversion method to calculate emission inventories without a prior at mesoscale: Application to the anthropogenic CO_2 emission from Houston, Texas

摘要

We developed a new inversion method to calculate an emission inventory for an anthropogenic pollutant without a prior emission estimate at mesoscale. This method employs slopes between mixing ratio enhancements of a given pollutant (CO_2, for instance) with other co-emitted tracers in conjunction with the emission inventories of those tracers (CO, NOy, and SO_2 are used in this example). The current application of this method employed in situ measurements onboard the NOAA WP-3 research aircraft during the 2006 Texas Air Quality Study (TexAQS 2006). We used 3 different transport models to estimate the uncertainties introduced by the transport models in the inversion. We demonstrated the validity of the new inversion method by calculating a 4 x 4 km~2 emission inventory of anthropogenic CO_2 in the Houston area in Texas, and comparing it to the 10 x 10 km2 Vulcan emission inventory for the same region. The calculated anthropogenic CO2 inventory for the Houston Ship Channel, home to numerous major industrial and port emission sources, showed excellent agreement with Vulcan. The daytime CO2 average flux from the Ship Channel is the largest urban CO_2 flux reported in the literature. Compared to Vulcan, the daytime urban area CO_2 emissions were higher by 37% ± 6%. Those differences can be explained by uncertainties in emission factors in Vulcan and by increased emissions from point sources and on-road emitters between 2002, the reference year in Vulcan, and 2006, the year that the TexAQS observations were made.