Source apportionment of size and time resolved trace elements and organic aerosols from an urban courtyard site in Switzerland

Time and size resolved data of trace elements were obtained from measurements with a rotating drum impactor (RDI) and subsequent X-ray fluorescence spectrometry. Trace elements can act as indicators for the identification of sources of particulate matter <10 μm (PM10) in ambient air. Receptor modeling was performed with positive matrix factorization (PMF) for trace element data from an urban background site in Zürich, Switzerland. Eight different sources were identified for the three examined size ranges (PM1-0.1, PM2.5-1 and PM 10-2.5): secondary sulfate, wood combustion, fire works, road traffic, mineral dust, de-icing salt, industrial and local anthropogenic activities. The major component was secondary sulfate for the smallest size range; the road traffic factor was found in all three size ranges. This trace element analysis is complemented with data from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (AMS), assessing the PM1 fraction of organic aerosols. A separate PMF analysis revealed three factors related to three of the sources found with the RDI: oxygenated organic aerosol (OOA, related to inorganic secondary sulfate), hydrocarbon-like organic aerosol (HOA, related to road traffic) and biomass burning organic aerosol (BBOA), explaining 60 %, 22 % and 17 % of total measured organics, respectively. Since different compounds are used for the source classification, a higher percentage of the ambient PM10 mass concentration can be apportioned to sources by the combination of both methods. © 2011 Author(s)

Evaluation of the Particle Measurement Programme (PMP) Protocol to Remove the Vehicles-Exhaust Aerosol Volatile Phase

European regulation for Euro 5/6 light duty emissions introduced the particle number concentration measurement of non-volatile particles with electrical mobility diameter >23 nm. The volatile phase is removed by using a heated dilution stage (150 °C) and a heated tube (at 300-400 °C). We investigated experimentally the volatile removal efficiency of the specific protocol by conducting measurements with two Euro 3 diesel light duty vehicles, a Euro 2 moped, and a Euro III heavy duty vehicle with the system¿s heaters on and off. The particle number distributions were measured with a Scanning Mobility Particle Sizer (SMPS) and a Fast Mobility Particle Sizer (FMPS). An Aerosol Mass Spectrometer (AMS) was used to identify the non-refractory chemical composition of the particles. A Multi-Angle Absorption Photometer (MAAP) was used to measure the black carbon concentration. The results showed that the condensed material on the accumulation mode (i.e. particles in the range of 50-500 nm) was efficiently removed (50-90%). The (volatile) nucleation mode was also completely evaporated or was decreased to sizes <23 nm; thus these particles wouldn¿t be counted from the particle counter, indicating the robustness of the protocol.JRC.F.8-Sustainable Transport (Ispra

Wintertime aerosol chemical composition and source apportionment of the organic fraction in the metropolitan area of Paris

The effect of a post-industrial megacity on local and regional air quality was assessed via a month-long field measurement campaign in the Paris metropolitan area during winter 2010. Here we present source apportionment results from three aerosol mass spectrometers and two aethalometers deployed at three measurement stations within the Paris region. Submicron aerosol composition is dominated by the organic fraction (30–36%) and nitrate (28–29%), with lower contributions from sulfate (14–16%), ammonium (12–14%) and black carbon (7–13%). Organic source apportionment was performed using positive matrix factorization, resulting in a set of organic factors corresponding both to primary emission sources and secondary production. The dominant primary sources are traffic (11–15% of organic mass), biomass burning (13–15%) and cooking (up to 35% during meal hours). Secondary organic aerosol contributes more than 50% to the total organic mass and includes a highly oxidized factor from indeterminate and/or diverse sources and a less oxidized factor related to wood burning emissions. Black carbon was apportioned to traffic and wood burning sources using a model based on wavelength-dependent light absorption of these two combustion sources. The time series of organic and black carbon factors from related sources were strongly correlated. The similarities in aerosol composition, total mass and temporal variation between the three sites suggest that particulate pollution in Paris is dominated by regional factors, and that the emissions from Paris itself have a relatively low impact on its surroundings

Online characterization of regulated and unregulated gaseous and particulate exhaust emissions from two-stroke mopeds: A chemometric approach

Two-stroke mopeds are a popular and convenient mean of transport in particular in the highly populated cities. These vehicles can emit potentially toxic gaseous and aerosol pollutants due to their engine technology. The legislative measurements of moped emissions are based on offline methods; however, the online characterization of gas and particulate phases offers great possibilities to understand aerosol formation mechanism and to adapt future emission standards. The purpose of this work was to study the emission behavior of two mopeds complying with different European emission standards (EURO-1 and EURO-2). A sophisticated set of online analyzers was applied to simultaneously monitor the gas phase and particulate phase of exhaust on a real time basis. The gaseous emission was analyzed with a high resolution Fourier transform infrared spectrometer (FTIR; nitrogen species) and a resonance-enhanced multiphoton ionization time-of-flight mass spectrometer (REMPI-ToF-MS; polycyclic aromatic hydrocarbons: PAH), whereas the particulate phase was chemically characterized by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS; organic, nitrate and chloride aerosol) and a multiangle absorption photometer (MAAP; black carbon). The physical characterization of the aerosol was carried out with a condensation particle counter (CPC; particle number concentration) and a fast mobility particle sizer (FMPS; size distribution in real time). In order to extract underlying correlation between gas and solid emissions, principal component analysis was applied to the comprehensive online dataset. Multivariate analysis highlighted the considerable effect of the exhaust temperature on the particles and heavy PAH emissions. The results showed that the after-treatment used to comply with the latest EURO-2 emission standard may be responsible for the production of more potentially harmful particles compared to the EURO-1 moped emissions

Primary and secondary organic aerosol origin by combined gas-particle phase source apportionment

Secondary organic aerosol (SOA), a prominent fraction of particulate organic mass (OA), remains poorly constrained. Its formation involves several unknown precursors, formation and evolution pathways and multiple natural and anthropogenic sources. Here a combined gas-particle phase source apportionment is applied to wintertime and summertime data collected in the megacity of Paris in order to investigate SOA origin during both seasons. This was possible by combining the information provided by an aerosol mass spectrometer (AMS) and a proton transfer reaction mass spectrometer (PTR-MS). A better constrained apportionment of primary OA (POA) sources is also achieved using this methodology, making use of gas-phase tracers. These tracers made possible the discrimination between biogenic and continental/anthropogenic sources of SOA. We found that continental SOA was dominant during both seasons (24–50% of total OA), while contributions from photochemistry-driven SOA (9% of total OA) and marine emissions (13% of total OA) were also observed during summertime. A semi-volatile nighttime component was also identified (up to 18% of total OA during wintertime). This approach was successfully applied here and implemented in a new source apportionment toolkit

Application of modern online instrumentation for chemical analysis of gas and particulate phases of exhaust at the European Commission heavy-duty vehicle emission laboratory.

The European Commission recently established a novel test facility for heavy-duty vehicles to enhance more sustainable transport. The facility enables the study of energy efficiency of various fuels/scenarios as well as the chemical composition of evolved exhaust emissions. Sophisticated instrumentation for real-time analysis of the gas and particulate phases of exhaust has been implemented. Thereby, gas-phase characterization was carried out by a Fourier transform infrared spectrometer (FT-IR; carbonyls, nitrogen-containing species, small hydrocarbons) and a resonance-enhanced multiphoton ionization time-of-flight mass spectrometer (REMPI-TOFMS; monocyclic and polycyclic aromatic hydrocarbons). For analysis of the particulate phase, a high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS; organic matter, chloride, nitrate), a condensation particle counter (CPC; particle number), and a multiangle absorption photometer (MAAP; black carbon) were applied. In this paper, the first application of the new facility in combination with the described instruments is presented, whereby a medium-size truck was investigated by applying different driving cycles. The goal was simultaneous chemical characterization of a great variety of gaseous compounds and particulate matter in exhaust on a real-time basis. The time-resolved data allowed new approaches to view the results; for example, emission factors were normalized to time-resolved consumption of fuel and were related to emission factors evolved during high speeds. Compounds could be identified that followed the fuel consumption, others showed very different behavior. In particular, engine cold start, engine ignition (unburned fuel), and high-speed events resulted in unique emission patterns

Emissions of organic aerosol mass, black carbon, particle number, and regulated and unregulated gases from scooters and light and heavy duty vehicles with different fuels

A sampling campaign with seven different types of vehicles was conducted in 2009 at the vehicle test facilities of the Joint Research Centre (JRC) in Ispra (Italy). The vehicles chosen were representative of some categories circulating in Europe and were 5 fueled either with standard gasoline or diesel and some with blends of rapeseed methyl ester biodiesel. The aim of this work was to improve the knowledge about the emission factors of gas phase and particle-associated regulated and unregulated species from vehicle exhaust. Unregulated species such as black carbon (BC), primary organic aerosol (OA) content, particle number (PN), monocyclic and polycyclic aromatic 10 hydrocarbons (PAHs) and a selection of unregulated gaseous compounds, including nitrous acid (N2O), ammonia (NH3), hydrogen cyanide (HCN), formaldehyde (HCHO), acetaldehyde (CH3CHO), sulfur dioxide (SO2), and methane (CH4), were measured in real time with a suite of instruments including a high-resolution aerosol time-of-flight mass spectrometer, a resonance enhanced multi-photon ionization time-of-flight mass 15 spectrometer, and a high resolution Fourier transform infrared spectrometer. Diesel vehicles, without particle filters, featured the highest values for particle number, followed by gasoline vehicles and scooters. The particles from diesel and gasoline vehicles were mostly made of BC with a low fraction of OA, while the particles from the scooters were mainly composed of OA. Scooters were characterized by super high emissions 20 factors for OA, which were orders of magnitude higher than for the other vehicles. The heavy duty diesel vehicle (HDDV) featured the highest nitrogen oxides (NOx) emissions, while the scooters had the highest emissions for total hydrocarbons and aromatic compounds due to the unburned and partially burned gasoline and lubricant oil mixture. Generally, vehicles fuelled with biodiesel blends showed lower emission 25 factors of OA and total aromatics than those from the standard fuels. The scooters were the main emitters of aromatic compounds, followed by the gasoline vehicle, the diesel vehicles and the HDDV.JRC.C.4-Sustainable Transpor

Application of Modern On-line Instrumentation for Chemical Analysis of Gas Phase and Particulate Phases of Exhaust at the European Commission Heavy-Duty Vehicle Emission Laboratory

The European Commission recently established a novel test facility for heavy duty vehicles to enhance more sustainable transport. The facility enables to study the energy efficiency of various fuels/scenarios as well as the chemical composition of evolved exhaust emissions. Sophisticated instrumentation for real-time analysis of the gas phase and the particulate phase of exhaust has been implemented. Thereby, gas phase characterization was carried out by a Fourier-transformation infrared spectrometer (FTIR: carbonyls, nitrogen-containing species, small hydrocarbons) and a resonance-enhanced multiphoton ionization time-of-flight mass spectrometer (REMPI-TOFMS: monocyclic and polycyclic aromatic hydrocarbons). For the analysis of the particulate phase a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS: organic matter, chloride, nitrate), a condensation particle counter (CPC: particle number), and a multi-angle absorption photometer (MAAP: black carbon) were applied. In this paper, the first application of the new facility in combination with the described instruments is presented, whereby a medium size truck was investigated by applying different driving cycles. Goal was the simultaneous chemical characterization of a great variety of gaseous compounds and particulate matter in exhaust on a real-time basis. The time-resolved data allowed new approaches to view the results e.g. emission factors were normalized to time-resolved consumption of fuel as well as related to emission factors evolved during high speeds. Compounds could be identified, which follow the fuel consumption, others showing a very different behavior. In particular, engine cold start, engine ignition (unburned fuel) and high speed events resulted in unique emission patterns.JRC.DDG.F.9-Sustainable Transport (Ispra