ABSTRACT
The SAE International has published Aerospace Information Report (AIR) 6241 which outlined the design and operation of a standardized measurement system for measuring non-volatile particulate matter (nvPM) mass and number emissions from commercial aircraft engines. Prior to this research, evaluation of this system by various investigators revealed differences in nvPM mass emissions measurement on the order of 15-30% both within a single sampling system and between two systems operating in parallel and measuring nvPM mass emissions from the same source. To investigate this issue, the U. S. Environmental Protection Agency in collaboration with the U. S. Air Force's Arnold Engineering Development Complex initiated the VAriable Response In Aircraft nvPM Testing (VARIAnT) research program to compare nvPM measurements within and between AIR-compliant sampling systems used for measuring combustion aerosols generated both by a 5201 Mini-CAST soot generator and a J85-GE-5 turbojet engine burning multiple fuels. The VARIAnT research program has conducted four test campaigns to date. The first campaign (VARIAnT 1) compared two essentially identical commercial versions of the sampling system while the second campaign (VARIAnT 2) compared a commercial system to the custom-designed Missouri University of Science and Technology's North American Reference System (NARS) built to the same specifications. Comparisons of nvPM particle mass (i.e., black carbon), number, and size were conducted in both campaigns. Additionally, the sensitivity to variation in system operational parameters was evaluated in VARIAnT 1. Results from both campaigns revealed agreement of about 12% between the two sampling systems, irrespective of manufacturer, in all aspects except for black carbon determination. The major source of measurement differences (20-70%) was due to low BC mass measurements made by the Artium Technologies LII-300 as compared to the AVL 483 Micro-Soot Sensor, the Aerodyne Cavity Attenuated Phase Shift (CAPS PMSSA) monitor, and the thermal-optical reference method for elemental carbon (EC) determination, which was used as the BC reference.
ABSTRACT
Secondary organic aerosol (SOA) constitutes a substantial fraction of fine particulate matter and has important impacts on climate and human health. The extent to which human activities alter SOA formation from biogenic emissions in the atmosphere is largely undetermined. Here, we present direct observational evidence on the magnitude of anthropogenic influence on biogenic SOA formation based on comprehensive ambient measurements in the southeastern United States (US). Multiple high-time-resolution mass spectrometry organic aerosol measurements were made during different seasons at various locations, including urban and rural sites in the greater Atlanta area and Centreville in rural Alabama. Our results provide a quantitative understanding of the roles of anthropogenic SO2 and NOx in ambient SOA formation. We show that isoprene-derived SOA is directly mediated by the abundance of sulfate, instead of the particle water content and/or particle acidity as suggested by prior laboratory studies. Anthropogenic NOx is shown to enhance nighttime SOA formation via nitrate radical oxidation of monoterpenes, resulting in the formation of condensable organic nitrates. Together, anthropogenic sulfate and NOx can mediate 43-70% of total measured organic aerosol (29-49% of submicron particulate matter, PM1) in the southeastern US during summer. These measurements imply that future reduction in SO2 and NOx emissions can considerably reduce the SOA burden in the southeastern US. Updating current modeling frameworks with these observational constraints will also lead to more accurate treatment of aerosol formation for regions with substantial anthropogenic-biogenic interactions and consequently improve air quality and climate simulations.
ABSTRACT
Cloud droplet formation depends on the condensation of water vapor on ambient aerosols, the rate of which is strongly affected by the kinetics of water uptake as expressed by the condensation (or mass accommodation) coefficient, αc. Estimates of αc for droplet growth from activation of ambient particles vary considerably and represent a critical source of uncertainty in estimates of global cloud droplet distributions and the aerosol indirect forcing of climate. We present an analysis of 10 globally relevant data sets of cloud condensation nuclei to constrain the value of αc for ambient aerosol. We find that rapid activation kinetics (αc > 0.1) is uniformly prevalent. This finding resolves a long-standing issue in cloud physics, as the uncertainty in water vapor accommodation on droplets is considerably less than previously thought.
ABSTRACT
Atmospheric emissions of gas and particulate matter from a large ocean-going container vessel were sampled as it slowed and switched from high-sulfur to low-sulfur fuel as it transited into regulated coastal waters of California. Reduction in emission factors (EFs) of sulfur dioxide (SO2), particulate matter, particulate sulfate and cloud condensation nuclei were substantial (≥ 90%). EFs for particulate organic matter decreased by 70%. Black carbon (BC) EFs were reduced by 41%. When the measured emission reductions, brought about by compliance with the California fuel quality regulation and participation in the vessel speed reduction (VSR) program, are placed in a broader context, warming from reductions in the indirect effect of SO4 would dominate any radiative changes due to the emissions changes. Within regulated waters absolute emission reductions exceed 88% for almost all measured gas and particle phase species. The analysis presented provides direct estimations of the emissions reductions that can be realized by California fuel quality regulation and VSR program, in addition to providing new information relevant to potential health and climate impact of reduced fuel sulfur content, fuel quality and vessel speed reductions.
