scholarly journals Chamber simulation on the formation of secondary organic aerosols (SOA) from diesel vehicle exhaust in China

2016 ◽  
Author(s):  
Wei Deng ◽  
Qihou Hu ◽  
Tengyu Liu ◽  
Xinming Wang ◽  
Yanli Zhang ◽  
...  
Keyword(s):  
Secondary Organic Aerosols ◽  
Organic Aerosols ◽  
Vehicle Exhaust ◽  
Chemical Aging ◽  
Aerosol Mass Spectrometer ◽  
Particulate Matter Emission ◽  
Photo Oxidation ◽  
Diesel Vehicles ◽  
Aerosol Mass ◽  
Production Factors

Abstract. In China primary particulate matter emission from on-road vehicles is predominantly coming from diesels, yet secondary organic aerosols (SOA) formed from diesel emission may be also of greater significance due to more intermediate volatile organic compounds (IVOC) in the exhaust. Here we introduced exhaust from in-use diesel vehicles under warm idling condition directly into an indoor smog chamber with a 30 m3 Teflon reactor, and investigated the SOA formation as well as chemical aging of organic aerosols during photo-oxidation. The emission factors of primary organic aerosol (POA) and black carbon (BC) for the three typical Chinese diesel vehicles ranged 0.18–0.91 and 0.15–0.51 g kg-fuel−1, respectively; and the SOA production factors ranged 0.50–1.8 g kg-fuel−1 with an average SOA/POA ratio of 1.6. Aromatic hydrocarbons could only explain less than 3 % of SOA formed during aging, and IVOC and oxygenated VOC might contribute substantially to SOA formation. High resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) resolved that POA dominated by CH classes (alkanes, cycloalkanes and alkenes) with high abundances of the CnH2n+1 and CnH2n-1 fragments, and after photo-oxidation the fraction of CH classes and the H/C ratios decreased, while the fraction of CHO, as well as the ratios of O/C and of organic matter to organic carbon (OM/OC), all increased. The plot of f44 (ratio of m/z 44 to the total signal in a mass spectrum) versus f43 indicated that diesel SOA were semi-volatile oxygenated organic aerosols (SV-OOA). The slopes of O:C versus H:C element ratios in the Van Krevelen diagram ranged from −0.47 to −0.68, suggesting a combination of carboxylic acid and alcohols/peroxides formed during the aging of diesel exhaust.

scholarly journals Characterization of particulate matter emissions from on-road gasoline and diesel vehicles using a soot particle aerosol mass spectrometer

2014 ◽  
Vol 14 (3) ◽  
pp. 4007-4049 ◽  
Author(s):  
T. R. Dallmann ◽  
T. B. Onasch ◽  
T. W. Kirchstetter ◽  
D. R. Worton ◽  
E. C. Fortner ◽  
...  
Keyword(s):  
Trace Elements ◽  
Particulate Matter ◽  
Soot Particle ◽  
Organic Aerosol ◽  
Lubricating Oil ◽  
Vehicle Exhaust ◽  
Aerosol Mass Spectrometer ◽  
Diesel Vehicles ◽  
Aerosol Mass ◽  
Exhaust Plumes

Abstract. Particulate matter (PM) emissions were measured in July 2010 from on-road motor vehicles driving through a highway tunnel in the San Francisco Bay area. A soot particle aerosol mass spectrometer (SP-AMS) was used to measure the chemical composition of PM emitted by gasoline and diesel vehicles at high time resolution. Organic aerosol (OA) and black carbon (BC) concentrations were measured during various time periods that had different levels of diesel influence, as well as directly in the exhaust plumes of individual heavy-duty (HD) diesel trucks. BC emission factor distributions for HD trucks were more skewed than OA distributions, with the highest 10% of trucks accounting for 56 and 42% of total measured BC and OA emissions, respectively. A comparison of measured OA and BC mass spectra across various sampling periods revealed a high degree of similarity in BC and OA emitted by gasoline and diesel engines. Cycloalkanes predominate in exhaust OA emissions relative to saturated alkanes (i.e., normal and iso-paraffins), suggesting that lubricating oil rather than fuel is the dominant source of primary organic aerosol (POA) emissions in diesel vehicle exhaust. This finding is supported by the detection of trace elements such as zinc and phosphorus in the exhaust plumes of individual trucks. Trace elements were emitted relative to total OA at levels that are consistent with typical weight fractions of commonly used additives present in lubricating oil. The presence of trace elements in vehicle exhaust raises the concern that ash deposits may accumulate over time in diesel particle filter systems, and may eventually lead to performance problems that require servicing.

scholarly journals Collection Efficiency of the Aerosol Mass Spectrometer for Chamber-Generated Secondary Organic Aerosols

2012 ◽  
Vol 47 (3) ◽  
pp. 294-309 ◽  
Author(s):  
Kenneth S. Docherty ◽  
Mohammed Jaoui ◽  
Eric Corse ◽  
Jose L. Jimenez ◽  
John H. Offenberg ◽  
...  
Keyword(s):  
Mass Spectrometer ◽  
Secondary Organic Aerosols ◽  
Collection Efficiency ◽  
Organic Aerosols ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass

scholarly journals Formation and evolution of secondary organic aerosols derived from urban-lifestyle sources: vehicle exhaust and cooking emissions

2021 ◽  
Vol 21 (19) ◽  
pp. 15221-15237
Author(s):  
Zirui Zhang ◽  
Wenfei Zhu ◽  
Min Hu ◽  
Kefan Liu ◽  
Hui Wang ◽  
...  
Keyword(s):  
Urban Areas ◽  
Secondary Organic Aerosols ◽  
Organic Aerosols ◽  
Growth Potential ◽  
Vehicle Group ◽  
Acid Oxidation ◽  
Vehicle Exhaust ◽  
Oxidation Pathway ◽  
Aerosol Mass ◽  
Photochemical Age

Abstract. Vehicle exhaust and cooking emissions are closely related to the daily life of city dwellers. Here, we defined the secondary organic aerosols (SOAs) derived from vehicle exhaust and cooking emissions as “urban-lifestyle SOAs” and simulated their formation using a Gothenburg potential aerosol mass reactor (Go:PAM). The vehicle exhaust and cooking emissions were separately simulated, and their samples were defined as “vehicle group” and “cooking group”, respectively. After samples had been aged under 0.3–5.5 d of equivalent photochemical age, these two urban-lifestyle SOAs showed markedly distinct features in the SOA mass growth potential, oxidation pathways, and mass spectra. The SOA/POA (primary organic aerosol) mass ratios of vehicle groups (107) were 44 times larger than those of cooking groups (2.38) at about 2 d of equivalent photochemical age, according to the measurement of scanning mobility particle sizer (SMPS). A high-resolution time-of-flight aerosol mass spectrometer was used to perform a deeper analysis. It revealed that organics from the vehicle may undergo the alcohol and/or peroxide and carboxylic acid oxidation pathway to produce abundant less and more oxidized oxygenated OAs (LO-OOAs and MO-OOAs), and only a few primary hydrocarbon-like organic aerosols (HOAs) remain unaged. In contrast, organics from cooking may undergo the alcohol and/or peroxide oxidation pathway to produce moderate LO-OOAs, and comparable primary cooking organic aerosols (COAs) remain unaged. Our findings provide an insight into atmospheric contributions and chemical evolutions for urban-lifestyle SOAs, which could greatly influence the air quality and health risk assessments in urban areas.

scholarly journals Aerosol chemical and optical properties over the Paris area within ESQUIF project

2006 ◽  
Vol 6 (11) ◽  
pp. 3257-3280 ◽  
Author(s):  
A. Hodzic ◽  
R. Vautard ◽  
P. Chazette ◽  
L. Menut ◽  
B. Bessagnet
Keyword(s):  
Optical Properties ◽  
Secondary Organic Aerosols ◽  
Organic Aerosols ◽  
Dust Particles ◽  
Aerosol Size Distribution ◽  
Aerosol Composition ◽  
Aerosol Mass ◽  
Coarse Mode ◽  
Paris Area ◽  
Flight Trajectories

Abstract. Aerosol chemical and optical properties are extensively investigated for the first time over the Paris Basin in July 2000 within the ESQUIF project. The measurement campaign offers an exceptional framework to evaluate the performances of the chemistry-transport model CHIMERE in simulating concentrations of gaseous and aerosol pollutants, as well as the aerosol-size distribution and composition in polluted urban environments against ground-based and airborne measurements. A detailed comparison of measured and simulated variables during the second half of July with particular focus on 19 and 31 pollution episodes reveals an overall good agreement for gas-species and aerosol components both at the ground level and along flight trajectories, and the absence of systematic biases in simulated meteorological variables such as wind speed, relative humidity and boundary layer height as computed by the MM5 model. A good consistency in ozone and NO concentrations demonstrates the ability of the model to reproduce the plume structure and location fairly well both on 19 and 31 July, despite an underestimation of the amplitude of ozone concentrations on 31 July. The spatial and vertical aerosol distributions are also examined by comparing simulated and observed lidar vertical profiles along flight trajectories on 31 July and confirm the model capacity to simulate the plume characteristics. The comparison of observed and modeled aerosol components in the southwest suburb of Paris during the second half of July indicates that the aerosol composition is rather correctly reproduced, although the total aerosol mass is underestimated by about 20%. The simulated Parisian aerosol is dominated by primary particulate matter that accounts for anthropogenic and biogenic primary particles (40%), and inorganic aerosol fraction (40%) including nitrate (8%), sulfate (22%) and ammonium (10%). The secondary organic aerosols (SOA) represent 12% of the total aerosol mass, while the mineral dust accounts for 8%. The comparison demonstrates the absence of systematic errors in the simulated sulfate, ammonium and nitrates total concentrations. However, for nitrates the observed partition between fine and coarse mode is not reproduced. In CHIMERE there is a clear lack of coarse-mode nitrates. This calls for additional parameterizations in order to account for the heterogeneous formation of nitrate onto dust particles. Larger discrepancies are obtained for the secondary organic aerosols due to both inconsistencies in the SOA formation processes in the model leading to an underestimation of their mass and large uncertainties in the determination of the measured aerosol organic fraction. The observed mass distribution of aerosols is not well reproduced, although no clear explanation can be given.

scholarly journals Towards a better understanding of the origins, chemical composition and aging of oxygenated organic aerosols: case study of a Mediterranean industrialized environment, Marseille

2013 ◽  
Vol 13 (15) ◽  
pp. 7875-7894 ◽  
Author(s):  
I. El Haddad ◽  
B. D'Anna ◽  
B. Temime-Roussel ◽  
M. Nicolas ◽  
A. Boreave ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Organic Aerosols ◽  
Industrial Emissions ◽  
Aerosol Mass Spectrometer ◽  
Statistical Confidence ◽  
Aerosol Mass ◽  
Novel Approach ◽  
Organic Markers ◽  
The Impact ◽  
First Time

Abstract. As part of the FORMES summer 2008 experiment, an Aerodyne compact time-of-flight aerosol mass spectrometer (cToF-AMS) was deployed at an urban background site in Marseille to investigate the sources and aging of organic aerosols (OA). France's second largest city and the largest port in the Mediterranean, Marseille, provides a locale that is influenced by significant urban industrialized emissions and an active photochemistry with very high ozone concentrations. Particle mass spectra were analyzed by positive matrix factorization (PMF2) and the results were in very good agreement with previous apportionments obtained using a chemical mass balance (CMB) approach coupled to organic markers and metals (El Haddad et al., 2011a). AMS/PMF2 was able to identify for the first time, to the best of our knowledge, the organic aerosol emitted by industrial processes. Even with significant industries in the region, industrial OA was estimated to contribute only ~ 5% of the total OA mass. Both source apportionment techniques suggest that oxygenated OA (OOA) constitutes the major fraction, contributing ~ 80% of OA mass. A novel approach combining AMS/PMF2 data with 14C measurements was applied to identify and quantify the fossil and non-fossil precursors of this fraction and to explicitly assess the related uncertainties. Results show with high statistical confidence that, despite extensive urban and industrial emissions, OOA is overwhelmingly non-fossil, formed via the oxidation of biogenic precursors, including monoterpenes. AMS/PMF2 results strongly suggest that the variability observed in the OOA chemical composition is mainly driven in our case by the aerosol photochemical age. This paper presents the impact of photochemistry on the increase of OOA oxygenation levels, formation of humic-like substances (HULIS) and the evolution of α-pinene SOA (secondary OA) components.

scholarly journals Aerosol chemical and optical properties over the Paris area within ESQUIF project

2006 ◽  
Vol 6 (1) ◽  
pp. 401-454 ◽  
Author(s):  
A. Hodzic ◽  
R. Vautard ◽  
P. Chazette ◽  
L. Menut ◽  
B. Bessagnet
Keyword(s):  
Optical Properties ◽  
Secondary Organic Aerosols ◽  
Organic Aerosols ◽  
Dust Particles ◽  
Aerosol Size Distribution ◽  
Aerosol Composition ◽  
Aerosol Mass ◽  
Coarse Mode ◽  
Paris Area ◽  
Flight Trajectories

Abstract. Aerosol chemical and optical properties are extensively investigated for the first time over the Paris Basin in July 2000 within the ESQUIF project. The measurement campaign offers an exceptional framework to evaluate the performances of the chemistry-transport model CHIMERE in simulating concentrations of gaseous and aerosol pollutants, as well as the aerosol-size distribution and composition in polluted urban environment against ground-based and airborne measurements. A detailed comparison of measured and simulated variables during the second half of July with particular focus on 19 and 31 pollution episodes reveals an overall good agreement for gas-species and aerosol components both at the ground level and along flight trajectories, and the absence of systematic biases in simulated meteorological variables such as wind speed, relative humidity and boundary layer height as computed by the MM5 model. A good consistency in ozone and NO concentrations demonstrates the ability of the model to reproduce fairly well the plume structure and location both on 19 and 31 July, despite an underestimation of the amplitude of ozone concentrations on 31 July. The spatial and vertical aerosol distributions are also examined by comparing simulated and observed lidar vertical profiles along flight trajectories on 31 July and confirmed the model capacity to simulate the plume characteristics. The comparison of observed and modeled aerosol components in the southwest suburb of Paris during the second half of July indicated that the aerosol composition is rather correctly reproduced, although the total aerosol mass is underestimated of about 20%. The simulated Parisian aerosol is dominated by primary particulate matter that accounts for anthropogenic and biogenic primary particles (40%) and inorganic aerosol fraction (40%) including nitrate (8%), sulfate (22%) and ammonium (10%). The secondary organic aerosols (SOA) represent 12% of the total aerosol mass, while the mineral dust accounts for 8%. The comparison demonstrated the absence of systematic errors in the simulated sulfate, ammonium and nitrates total concentrations. However for nitrates the observed partition between fine and coarse mode is not reproduced. In CHIMERE there is a clear lack of coarse-mode nitrates. This calls for additional parameterizations in order to account for the heterogeneous formation of nitrate onto dust particles. Larger discrepancies are obtained for the secondary organic aerosols due to both inconsistencies in the SOA formation processes in the model leading to an underestimation of their mass and large uncertainties in the determination of the measured aerosol organic fraction. The observed mass distribution of aerosols is not well reproduced, although no clear explanation can be given.

Characterization of organic aerosols in Beijing using an aerodyne high-resolution aerosol mass spectrometer

2015 ◽  
Vol 32 (6) ◽  
pp. 877-888 ◽  
Author(s):  
Junke Zhang ◽  
Yuesi Wang ◽  
Xiaojuan Huang ◽  
Zirui Liu ◽  
Dongsheng Ji ◽  
...  
Keyword(s):  
High Resolution ◽  
Mass Spectrometer ◽  
Organic Aerosols ◽  
Aerosol Mass Spectrometer ◽  
Aerosol Mass

scholarly journals Overview of the field measurement campaign in Hyytiälä, August 2001 in the framework of the EU project OSOA

2004 ◽  
Vol 4 (3) ◽  
pp. 657-678 ◽  
Author(s):  
M. Boy ◽  
T. Petäjä ◽  
M. Dal Maso ◽  
Ü. Rannik ◽  
J. Rinne ◽  
...  
Keyword(s):  
Solar Irradiance ◽  
Secondary Organic Aerosols ◽  
Organic Aerosols ◽  
Ground Level ◽  
Oxidation Products ◽  
Particle Phase ◽  
Average Growth ◽  
Photo Oxidation ◽  
Nucleation Mode ◽  
Condensation Sink

Abstract. As part of the OSOA (Origin and formation of Secondary Organic Aerosols) project, two intensive field campaigns were conducted in Melpitz, Germany and Hyytiälä, Finland. This paper gives an overview of the measurements made during the Hyytiälä campaign, which was held between 1 and 16 August 2001. Various instrumental techniques were used to achieve physical and chemical characterisation of aerosols and to investigate possible precursor gases. During the OSOA campaign in Hyytiälä, particle formation was observed on three consecutive days at the beginning of the campaign (1 to 3 August 2001) and on three days later on. The investigation of the meteorological situation divided the campaign into two parts. During the first three days of August, relatively cold and clean air masses from northwest passed over the station (condensation sink – CS: <0.002 s-1, NOx: <0.5 ppb). Daily particle bursts of one fraction of the nucleation mode aerosols (3–10 nm) with number concentrations between 600–1200 particles cm-3 were observed. After this period, warmer and more polluted air from south-west to south-east arrived at the station (CS: 0.002–0.01 s-1, NOx: 0.5–4 ppb) and during these 13 days only three events were observed. These events were not as apparent as those that occurred during the earlier period of the campaign. The chemical analyses from different institutes of PM2, PM2.5 and PM10 particles confirmed the assumption that organic matter from the oxidation of various terpenes contributed to the formation of secondary organic aerosols (SOA). Concerning these conclusions among others, the ratio between formic (oxidation product of isoprene and monoterpenes by ozone) and acetic acid (increased by anthropogenic emissions) (ratio=1 to 1.5) and concentration of different carboxylic acids (up to 62 ngm-3) were investigated. Gas/particle partitioning of five photo-oxidation products from α- and β-pinene resulted in higher concentrations of pinonic, nor pinonic and pinic acids in the particle phase than in the gas phase, which indicates a preference to the particle phase for these compounds. The average growth factors (GF) from 100 nm particles in water vapour gave a diurnal pattern with a maximum during daytime and values between 1.2 and 1.7. On average, the amount of secondary organic carbon reached values around 19% of the sampled aerosols and we speculate that formation of SOA with the influence of photo-oxidation products from terpenes was the reason for the observed particle bursts during the campaign. However, correlations between the precursor gases or the favourable condensing species with the monitored nucleation mode particles were not found. For the investigated time period other factors like the condensation sink of newly formed particles to the pre-existing aerosols, temperature and solar irradiance seem to be more important steering parameters for the production of new aerosols. Another open question concerns the vertical distribution of the formation of SOA. For this reason measurements were conducted at different altitudes using a tethered balloon platform with particle sampling and particle counting equipment. They were incorporated with eddy covariance (EC) flux measurements made at 23 m above ground level. The results give first indications that production of new aerosols happens throughout the planetary boundary layer (PBL), whereby different parameters e.g. temperature, CS, solar irradiance or concentration of monoterpenes are responsible for the location of the vertical maximum.

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