A gap in emission inventories of urban volatile organic compound (VOC) sources, which contribute to regional ozone and aerosol burdens, has increased as transportation emissions in the United States and Europe have declined rapidly. A detailed mass balance demonstrates that the use of volatile chemical products (VCPs)-including pesticides, coatings, printing inks, adhesives, cleaning agents, and personal care products-now constitutes half of fossil fuel VOC emissions in industrialized cities. The high fraction of VCP emissions is consistent with observed urban outdoor and indoor air measurements. We show that human exposure to carbonaceous aerosols of fossil origin is transitioning away from transportation-related sources and toward VCPs. Existing U.S. regulations on VCPs emphasize mitigating ozone and air toxics, but they currently exempt many chemicals that lead to secondary organic aerosols.
Several different inventories of global and regional anthropogenic and biomass burning emissions are assessed for the 1980-2010 period. The species considered in this study are carbon monoxide, nitrogen oxides, sulfur dioxide and black carbon. The inventories considered include the ACCMIP historical emissions developed in support of the simulations for the IPCC AR5 assessment. Emissions for 2005 and 2010 from the Representative Concentration Pathways (RCPs) are also included. Large discrepancies between the global and
Abstract. The mandate of the Task Force Hemispheric Transport of Air Pollution (TF HTAP) under the Convention on Long-Range Transboundary Air Pollution (CLRTAP) is to improve the scientific understanding of the intercontinental air pollution transport, to quantify impacts on human health, vegetation and climate, to identify emission mitigation options across the regions of the Northern Hemisphere, and to guide future policies on these aspects. The harmonization and improvement of regional emission inventories is imperative to obtain consolidated estimates on the formation of global-scale air pollution. An emissions data set has been constructed using regional emission grid maps (annual and monthly) for SO2, NOx, CO, NMVOC, NH3, PM10, PM2.5, BC and OC for the years 2008 and 2010, with the purpose of providing consistent information to global and regional scale modelling efforts. This compilation of different regional gridded inventories – including that of the Environmental Protection Agency (EPA) for USA, the EPA and Environment Canada (for Canada), the European Monitoring and Evaluation Programme (EMEP) and Netherlands Organisation for Applied Scientific Research (TNO) for Europe, and the Model Inter-comparison Study for Asia (MICS-Asia III) for China, India and other Asian countries – was gap-filled with the emission grid maps of the Emissions Database for Global Atmospheric Research (EDGARv4.3) for the rest of the world (mainly South America, Africa, Russia and Oceania). Emissions from seven main categories of human activities (power, industry, residential, agriculture, ground transport, aviation and shipping) were estimated and spatially distributed on a common grid of 0.1° × 0.1° longitude-latitude, to yield monthly, global, sector-specific grid maps for each substance and year. The HTAP_v2.2 air pollutant grid maps are considered to combine latest available regional information within a complete global data set. The disaggregation by sectors, high spatial and temporal resolution and detailed information on the data sources and references used will provide the user the required transparency. Because HTAP_v2.2 contains primarily official and/or widely used regional emission grid maps, it can be recommended as a global baseline emission inventory, which is regionally accepted as a reference and from which different scenarios assessing emission reduction policies at a global scale could start. An analysis of country-specific implied emission factors shows a large difference between industrialised countries and developing countries for acidifying gaseous air pollutant emissions (SO2 and NOx) from the energy and industry sectors. This is not observed for the particulate matter emissions (PM10, PM2.5), which show large differences between countries in the residential sector instead. The per capita emissions of all world countries, classified from low to high income, reveal an increase in level and in variation for gaseous acidifying pollutants, but not for aerosols. For aerosols, an opposite trend is apparent with higher per capita emissions of particulate matter for low income countries.
The multispecies analysis of daily air samples collected at the NOAA Boulder Atmospheric Observatory (BAO) in Weld County in northeastern Colorado since 2007 shows highly correlated alkane enhancements caused by a regionally distributed mix of sources in the Denver‐Julesburg Basin. To further characterize the emissions of methane and non‐methane hydrocarbons (propane, n‐butane, i‐pentane, n‐pentane and benzene) around BAO, a pilot study involving automobile‐based surveys was carried out during the summer of 2008. A mix of venting emissions (leaks) of raw natural gas and flashing emissions from condensate storage tanks can explain the alkane ratios we observe in air masses impacted by oil and gas operations in northeastern Colorado. Using the WRAP Phase III inventory of total volatile organic compound (VOC) emissions from oil and gas exploration, production and processing, together with flashing and venting emission speciation profiles provided by State agencies or the oil and gas industry, we derive a range of bottom‐up speciated emissions for Weld County in 2008. We use the observed ambient molar ratios and flashing and venting emissions data to calculate top‐down scenarios for the amount of natural gas leaked to the atmosphere and the associated methane and non‐methane emissions. Our analysis suggests that the emissions of the species we measured are most likely underestimated in current inventories and that the uncertainties attached to these estimates can be as high as a factor of two.
Methane (CH4) emissions from natural gas production are not well quantified and have the potential to offset the climate benefits of natural gas over other fossil fuels. We use atmospheric measurements in a mass balance approach to estimate CH4 emissions of 55 ± 15 × 103 kg h−1 from a natural gas and oil production field in Uintah County, Utah, on 1 day: 3 February 2012. This emission rate corresponds to 6.2%–11.7% (1σ) of average hourly natural gas production in Uintah County in the month of February. This study demonstrates the mass balance technique as a valuable tool for estimating emissions from oil and gas production regions and illustrates the need for further atmospheric measurements to determine the representativeness of our single‐day estimate and to better assess inventories of CH4 emissions.
[1] In situ measurements of the mass, mixing state, and optical size of individual black-carbon (BC) particles in the fine mode (90 -600 nm) have been made in fresh emissions from urban and biomass burning sources with an airborne single-particle soot photometer. Contrasts between the two sources are significant and consistent. Urban BC tends to smaller sizes, fewer coated particles, thinner coatings, and less absorption per unit mass than biomass-burning BC. This suggests that urban BC may have a longer lifetime in the atmosphere and a different impact on BC radiative forcing in the first indirect effect than biomass-burning BC. These measurements bound the likely variability in the microphysical state of BC emissions from typical continental processes, and provide direct measurements of the size distribution and coating state of fine-mode BC for use in constraining climate and aerosol models. These results highlight the need for the integration of sourcespecific information into such models. Citation: Schwarz, J. P., et al. (2008), Measurement of the mixing state, mass, and optical size of individual black carbon particles in urban and biomass burning emissions, Geophys. Res. Lett., 35, L13810,
While the formation pathways and thermodynamic properties of inorganic species (e.g., sulphate) in atmospheric aerosols are well understood, many more uncertainties exist about organics. In the present study we present oxidation pathways of organic gas phase species that lead to low volatility organic compounds (C2‐C6 dicarboxylic acids, pyruvic acid) in both the aqueous and gas phases. This mechanism is implemented in a cloud parcel model initialized with pure (NH4)2SO4 particles in 10 discrete sizes. Under clean continental conditions a few cloud processing cycles produce a total organic mass addition of ∼150 ng m−3. Individual resuspended aerosol size classes contain significant organic fractions, sometimes higher than 50%. These are likely upper bound estimates of organic mass production. In a polluted, i.e., SO2‐rich scenario, about 400 ng m−3 organic material is produced after about eight cloud cycles. Since the initial conditions in this latter case favor significant production of sulphate, the organic fraction of the aerosol mass after cloud processing represents a much lower percentage of the total aerosol mass. Oxalic, glutaric, adipic, and pyruvic acids are the main contributors to the organic fraction in both cases. In agreement with observations, the oxalate fraction in processed particles exceeds the fractions of other dicarboxylic acids since it represents an end product in the oxidation of several organic gas phase species. The study suggests that cloud processing may act as a significant source of small dicarboxylic acids, some fraction of which can be retained in the aerosol phase upon drop evaporation.
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