Characterization of Air Pollutant and Greenhouse Gas Emissions from Energy Use and Energy Production Processes in United States

Air pollutants and greenhouse gases are two groups of important trace components in the earth’s atmosphere that can affect local air quality, be detrimental to the human health and ecosystem, and cause climate change. Human activities, especially the energy use and energy production processes, are responsible for a significant share of air pollutants and greenhouse gases in the atmosphere. In this work, I specifically focused on characterizing air pollutants and greenhouse gas emissions from the on-road gasoline and diesel vehicles, which is an important energy use process that largely contributes to the urban air pollutions, and from the natural gas production systems, which is a major energy production process that has increased dramatically in recent years and is expected to have a long-lasting impact in the future. We conducted multi-seasonal measurements in the Fort Pitt Tunnel in Pittsburgh, PA to update the on-road vehicle emission factors, to measure the size distribution of vehicle emitted particulate matter (PM), and to quantify the volatility distributions of the vehicle emitter primary organic aerosol (POA). We also conducted mobile measurements in the Denver-Julesburg Basin, the Uintah Basin, and the Marcellus Shale to quantify facility-level VOC emission from natural gas production facilities, and I constructed a gridded (0.1° × 0.1°) methane emission inventory of natural gas production and distribution over the contiguous US. I found that the stricter emission standards were effective on regulating NOx and PM emissions of diesel vehicles and the NOx, CO and organic carbon (OC) emissions of gasoline vehicles, while the elemental carbon (EC) emissions of gasoline vehicles did not change too much over the past three decades. Vehicle-emitted particles may be largely externally mixed, and a large fraction of vehicle-emitted particles may be purely composed of volatile component. Vehicle-emitted smaller particles (10– 60 nm) are dominantly (over 75%) composed of volatile component. The size-resolved particles and particles emission factors for both gasoline and diesel vehicles are also reported in this work. I also found that the POA volatility distribution measured in the dynamometer studies can be applied to describe gas-particle partitioning of ambient POA emissions. The POA volatility distribution measured in the tunnel does not have significant diurnal or seasonal variations, which indicate that a single volatility distribution is adequate to describe the gas-particle partitioning of vehicle emitted POA in the urban environment. The facility-level VOC emission rates measured at gas production facilities in all three gas production fields are highly variable and cross a range of ~2-3 order of magnitudes. It suggests that a single VOC emission profile may not be able to characterize VOC emissions from all natural gas production facilities. My gridded methane emission inventory over the contiguous US show higher methane emissions over major natural gas production fields compared with the Environmental Protection Agency Inventory of US Greenhouse Gas Emission and Sinks (EPA GHGI) and the Emission Database for Global Atmospheric Research, version 4.2 (Edgar v4.2). The total methane emissions of the natural gas production and distribution sector estimated by my inventory are 74% and 20% higher than the Edgar v4.2 and EPA GHGI, respectively. I also run the GEOS-Chem methane simulation with my inventory and EPA GHGI and compare with the GOSAT satellite data, and results show that my inventory can improve the model and satellite comparison, but the improvement is very limited. The size-resolved emission factors of vehicle emitted particles and POA volatility distribution reported in this work can be applied by the chemical transport models to better quantify the contribution of vehicle emissions to the PM in the atmosphere. Since our measurement of VOC emissions of natural gas production facilities were conducted before EPA started to regulate VOC emissions from the O&NG production facilities in 2016, the facility-level VOC emission rates reported in this work can serve as the basis for future studies to test the effectiveness of the regulatory policies. The spatially resolved methane emission inventory of natural gas production and distribution constructed in this work can be applied to update the current default methane emission inventory of GEOS-Chem, and the updated methane emission inventory can be used as a better a priori emission field for top-down studies that inversely estimate methane emissions from atmospheric methane observation.