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1.
  • Bilde, M., et al. (författare)
  • Saturation Vapor Pressures and Transition Enthalpies of Low-Volatility Organic Molecules of Atmospheric Relevance: From Dicarboxylic Acids to Complex Mixtures
  • 2015
  • Ingår i: Chemical Reviews. - : The American Chemical Society (ACS). - 0009-2665 .- 1520-6890. ; 115:10, s. 4115-4156
  • Tidskriftsartikel (refereegranskat)abstract
    • There are a number of techniques that can be used that differ in terms of whether they fundamentally probe the equilibrium and the temperature range over which they can be applied. The series of homologous, straight-chain dicarboxylic acids have received much attention over the past decade given their atmospheric relevance, commercial availability, and low saturation vapor pressures, thus making them ideal test compounds. Uncertainties in the solid-state saturation vapor pressures obtained from individual methodologies are typically on the order of 50-100%, but the differences between saturation vapor pressures obtained with different methods are approximately 1-4 orders of magnitude, with the spread tending to increase as the saturation vapor pressure decreases. Some of the dicarboxylic acids can exist with multiple solid-state structures that have distinct saturation vapor pressures. Furthermore, the samples on which measurements are performed may actually exist as amorphous subcooled liquids rather than solid crystalline compounds, again with consequences for the measured saturation vapor pressures, since the subcooled liquid phase will have a higher saturation vapor pressure than the crystalline solid phase. Compounds with equilibrium vapor pressures in this range will exhibit the greatest sensitivities in terms of their gas to particle partitioning to uncertainties in their saturation vapor pressures, with consequent impacts on the ability of explicit and semiexplicit chemical models to simulate secondary organic aerosol formation.
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2.
  • Emanuelsson, Eva U., et al. (författare)
  • Parameterization of Thermal Properties of Aging Secondary Organic Aerosol Produced by Photo-Oxidation of Selected Terpene Mixtures
  • 2014
  • Ingår i: Environmental Science and Technology. - : The American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 48:11, s. 6168-6176
  • Tidskriftsartikel (refereegranskat)abstract
    • Formation and evolution of secondary organic aerosols (SOA) from biogenic VOCs influences the Earth's radiative balance. We have examined the photo-oxidation and aging of boreal terpene mixtures in the SAPHIR simulation chamber. Changes in thermal properties and chemical composition, deduced from mass spectrometric measurements, were providing information on the aging of biogenic SOA produced under ambient solar conditions. Effects of precursor mixture, concentration, and photochemical oxidation levels (OH exposure) were evaluated. OH exposure was found to be the major driver in the long term photochemical transformations, i.e., reaction times of several hours up to days, of SOA and its thermal properties, whereas the initial concentrations and terpenoid mixtures had only minor influence. The volatility distributions were parametrized using a sigmoidal function to determine T-VFR0.5 (the temperature yielding a 50% particle volume fraction remaining) and the steepness of the volatility distribution. T-VFR0.5 increased by 0.3 +/- 0.1% (ca. 1 K), while the steepness increased by 0.9 +/- 0.3% per hour of 1 x 10(6) cm(-3) OH exposure. Thus, aging reduces volatility and increases homogeneity of the vapor pressure distribution, presumably because highly volatile fractions become increasingly susceptible to gas phase oxidation, while less volatile fractions are less reactive with gas phase OH.
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3.
  • Flores, J. M., et al. (författare)
  • Evolution of the complex refractive index in the UV spectral region in ageing secondary organic aerosol
  • 2014
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus Gesellschaft mbH. - 1680-7316 .- 1680-7324. ; 14:11, s. 5793-5806
  • Tidskriftsartikel (refereegranskat)abstract
    • The chemical and physical properties of secondary organic aerosol (SOA) formed by the photochemical degradation of biogenic and anthropogenic volatile organic compounds (VOC) are as yet still poorly constrained. The evolution of the complex refractive index (RI) of SOA, formed from purely biogenic VOC and mixtures of biogenic and anthropogenic VOC, was studied over a diurnal cycle in the SAPHIR photochemical outdoor chamber in Julich, Germany. The correlation of RI with SOA chemical and physical properties such as oxidation level and volatility was examined. The RI was retrieved by a newly developed broadband cavity-enhanced spectrometer for aerosol optical extinction measurements in the UV spectral region (360 to 420 nm). Chemical composition and volatility of the particles were monitored by a high-resolution time-of-flight aerosol mass spectrometer, and a volatility tandem differential mobility analyzer. SOA was formed by ozonolysis of either (i) a mixture of biogenic VOC (alpha-pinene and limonene), (ii) biogenic VOC mixture with subsequent addition of an anthropogenic VOC (p-xylene-d(10)), or (iii) a mixture of biogenic and anthropogenic VOC. The SOA aged by ozone/OH reactions up to 29.5 h was found to be non-absorbing in all cases. The SOA with p-xylene-d(10) showed an increase of the scattering component of the RI correlated with an increase of the O / C ratio and with an increase in the SOA density. There was a greater increase in the scattering component of the RI when the SOA was produced from the mixture of biogenic VOCs and anthropogenic VOC than from the sequential addition of the VOCs after approximately the same ageing time. The increase of the scattering component was inversely correlated with the SOA volatility. Two RI retrievals determined for the pure biogenic SOA showed a constant RI for up to 5 h of ageing. Mass spectral characterization shows the three types of the SOA formed in this study have a significant amount of semivolatile components. The influence of anthropogenic VOCs on the oxygenated organic aerosol as well as the atmospheric implications are discussed.
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5.
  • Hallquist, Mattias, 1969, et al. (författare)
  • Photochemical smog in China: scientific challenges and implications for air-quality policies
  • 2016
  • Ingår i: National Science Review. - 2095-5138 .- 2053-714X. ; 3:4, s. 401-403
  • Tidskriftsartikel (refereegranskat)abstract
    • In large areas of China severe air pollution events pose a significant threat to human health, ecosystems and climate. Current reduction of primary emissions will also affect secondary pollutants such as ozone (O3) and particulate matter (PM), but the magnitude of the effects is uncertain. Major scientific challenges are related to the formation of O3 and secondary particulate matter including Secondary Organic Aerosols (SOA). Large uncertainties also remain regarding the interactions of soot, SOA and O3 under the influence of different SO2, NOX and VOC concentrations. To improve the understanding of these secondary atmospheric interactions in China, scientific areas of central importance for photochemically induced air pollutants have been identified. In addition to the scientific challenges, results from research need to be synthesized across several disciplines and communicated to stakeholders affected by air pollution and to policy makers responsible for developing abatement strategies. Development of these science-policy interactions can benefit from experience gained under the UN ECE Convention on Long Range Transboundary Air Pollution (LRTAP)
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6.
  • Hallquist, Åsa Marita, et al. (författare)
  • On-board Measurements of Nanoparticles from a SCR-Equipped Marine Diesel Engine
  • 2013
  • Ingår i: Environmental Science & Technology. - : American Chemical Society. - 0013-936X .- 1520-5851. ; 47:2
  • Tidskriftsartikel (refereegranskat)abstract
    • In this study nanoparticle emissions have been characterised on-board a ship with focus on number, size and volatility. Measurements were conducted on one of the ship’s four main 12 600 kW medium–speed diesel engines which use low sulphur marine residual fuel and have a Selective Catalytic Reduction (SCR) system for NOX abatement. The particles were measured after the SCR with an engine exhaust particle sizer spectrometer (EEPS), giving particle number and mass distributions in the size range of 5.6-560 nm. The thermal characteristics of the particles were analysed using a volatility tandem DMA system (VTDMA). A dilution ratio of 450-520 was used which is similar to the initial real-world dilution. At a stable engine load of 75% of the maximum rated power, and after dilution and cooling of the exhaust gas, there was a bimodal number size distribution, with a major peak at ~10 nm and a smaller peak at around 30-40 nm. The mass distribution peaked around 20 nm and at 50-60 nm. The emission factor for particle number, EFPN, for an engine load of 75% in the open-sea was found to be 10.4 ± 1.6 × 1016 (kg fuel)-1 and about 50% of the particles by number were found to have a non-volatile core at 250 °C. Additionally, 20 nm particles consist of ~40% of non-volatile material by volume (evaporative temperature 250 °C) while the particles with a particle diameter <10 nm evaporate completely at a temperature of 130-150 °C. Emission factors for NOX, CO and CO2 for an engine load of 75% in the open-sea were determined to 4.06 ± 0.3 g (kg fuel)-1, 2.15 ± 0.06 g (kg fuel)-1 and 3.23 ± 0.08 kg (kg fuel)-1, respectively. This work contributes to an improved understanding of particle emissions from shipping using modern pollution reduction measures such as SCR and fuel with low sulphur content.
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7.
  • Kong, Xiangrui, et al. (författare)
  • Molecular characterization and optical properties of primary emissions from a residential wood burning boiler
  • 2021
  • Ingår i: Science of the Total Environment. - : Elsevier B.V.. - 0048-9697 .- 1879-1026. ; 754
  • Tidskriftsartikel (refereegranskat)abstract
    • Modern small-scale biomass burners have been recognized as an important renewable energy source because of the economic and environmental advantages of biomass over fossil fuels. However, the characteristics of their gas and particulate emissions remain incompletely understood, and there is substantial uncertainty concerning their health and climate impacts. Here, we present online measurements conducted during the operation of a residential wood-burning boiler. The measured parameters include gas and particle concentrations, optical absorption and chemical characteristics of gases and particles. Positive matrix factorization was performed to analyze data from a high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) equipped with a filter inlet for gases and aerosols (FIGAERO). Six factors were identified and interpreted. Three factors were related to the chemical composition of the fuel representing lignin pyrolysis products, cellulose/hemicellulose pyrolysis products, and nitrogen-containing organics, while three factor were related to the physical characteristics of the emitted compounds: volatile compounds, semi-volatile compounds, and filter-derived compounds. An ordinal analysis was performed based on the factor fractions to identify the most influential masses in each factor, and by deconvoluting high-resolution mass spectra fingerprint molecules for each factor were identified. Results from the factor analysis were linked to the optical properties of the emissions, and lignin and cellulose/hemicellulose pyrolysis products appeared to be the most important sources of brown carbon under the tested burning conditions. It is concluded that the emissions from the complex combustion process can be described by a limited set of physically meaningful factors, which will help to rationalize subsequent transformation and tracing of emissions in the atmosphere and associated impacts on health and climate. 
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8.
  • Le Breton, Michael, 1986, et al. (författare)
  • Application of a FIGAERO ToF CIMS for on-line characterization of real-world fresh and aged particle emissions from buses
  • 2019
  • Ingår i: Aerosol Science and Technology. - 0278-6826 .- 1521-7388. ; 53:3, s. 244-259
  • Tidskriftsartikel (refereegranskat)abstract
    • © 2019, © 2019 The Author(s). Published with license by Taylor & Francis Group, LLC. On-line chemical characterization of real-world particle emissions from 13 transit buses was performed using a chemical ionization mass spectrometer (CIMS) equipped with a filter inlet for gases and aerosols (FIGAERO). In addition to the fresh emissions the emissions were artificially aged using a potential aerosol mass reactor (Go:PAM). The buses studied were running on different fuel types (diesel, compressed natural gas, and rapeseed methyl ester) and exhaust after-treatment systems (selective catalytic reduction (SCR), exhaust gas recirculation (EGR), and a three-way catalyst). When evaluating emissions from passing exhaust plumes using the FIGAERO ToF-CIMS, two technical features were highlighted from this work, the use of high mass calibrants and the factor enhancement method to be able to filter important compounds from mass spectra including hundreds of species. Here, acetate was used as the reagent ion to enable detection of highly oxygenated species in the exhaust particle emissions with potential high toxicity and/or secondary organic aerosol formation (SOA) potential. The acetate ionization scheme accounted for 4% to 46% of the total emitted particulate mass through identification of 61 species in the spectra. For aged emission the various fuel types provided overlapping species that could explain up to 19% of the aged emissions. This is hypothesized to come from the oxidation of engine lubrication oil, thus a common source for various fuels which was further supported by laboratory measurements. Specific markers from the SCR technology, such as urea oxidation products and further byproducts from hydrolysis were identified and attributed to reactions of isocyanic acid.
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9.
  • Le Breton, Michael, 1986, et al. (författare)
  • Chlorine oxidation of VOCs at a semi-rural site in Beijing: significant chlorine liberation from ClNO2 and subsequent gas- and particle-phase Cl-VOC production
  • 2018
  • Ingår i: Atmospheric Chemistry and Physics. - 1680-7316 .- 1680-7324. ; 18:17, s. 13013-13030
  • Tidskriftsartikel (refereegranskat)abstract
    • Nitryl chloride (ClNO2) accumulation at night acts as a significant reservoir for active chlorine and impacts the following day's photochemistry when the chlorine atom is liberated at sunrise. Here, we report simultaneous measurements of N2O5 and a suite of inorganic halogens including ClNO2 and reactions of chloride with volatile organic compounds (Cl-VOCs) in the gas and particle phases utilising the Filter Inlet for Gas and AEROsols time-of-flight chemical ionisation mass spectrometer (FIGAERO-ToF-CIMS) during an intensive measurement campaign 40 km northwest of Beijing in May and June 2016. A maximum mixing ratio of 2900 ppt of ClNO2 was observed with a mean campaign nighttime mixing ratio of 487 ppt, appearing to have an anthropogenic source supported by correlation with SO2, CO and benzene, which often persisted at high levels after sunrise until midday. This was attributed to such high mixing ratios persisting after numerous e-folding times of the photolytic lifetime enabling the chlorine atom production to reach 2.3 x 10(5) molecules cm(-3) from ClNO2 alone, peaking at 09:30 LT and up to 8.4 x 10(5) molecules cm(-3) when including the supporting inorganic halogen measurements. Cl-VOCs were observed in the particle and gas phases for the first time at high time resolution and illustrate how the iodide ToF-CIMS can detect unique markers of chlorine atom chemistry in ambient air from both biogenic and anthropogenic sources. Their presence and abundance can be explained via time series of their measured and steady-state calculated precursors, enabling the assessment of competing OH and chlorine atom oxidation via measurements of products from both of these mechanisms and their relative contribution to secondary organic aerosol (SOA) formation.
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10.
  • Le Breton, Michael, 1986, et al. (författare)
  • Online gas- and particle-phase measurements of organosulfates, organosulfonates and nitrooxy organosulfates in Beijing utilizing a FIGAERO ToF-CIMS
  • 2018
  • Ingår i: Atmospheric Chemistry and Physics. - 1680-7316. ; 18:14, s. 10355-10371
  • Tidskriftsartikel (refereegranskat)abstract
    • A time-of-flight chemical ionization mass spectrometer (CIMS) utilizing the Filter Inlet for Gas and Aerosol (FIGAERO) was deployed at a regional site 40 km north-west of Beijing and successfully identified and measured 17 sulfur-containing organics (SCOs are organo/nitrooxy organosulfates and sulfonates) with biogenic and anthropogenic precursors. The SCOs were quantified using laboratory-synthesized standards of lactic acid sulfate and nitrophenol organosulfate (NP OS). The variation in field observations was confirmed by comparison to offline measurement techniques (orbitrap and high-performance liquid chromatography, HPLC) using daily averages. The mean total (of the 17 identified by CIMS) SCO particle mass concentration was 210 +/- 110 ng m(-3) and had a maximum of 540 ng m(-3), although it contributed to only 2 +/- 1% of the organic aerosol (OA). The CIMS identified a persistent gas-phase presence of SCOs in the ambient air, which was further supported by separate vapour-pressure measurements of NP OS by a Knudsen Effusion Mass Spectrometer (KEMS). An increase in relative humidity (RH) promoted partitioning of SCO to the particle phase, whereas higher temperatures favoured higher gas-phase concentrations. Biogenic emissions contributed to only 19% of total SCOs measured in this study. Here, C10H16NSO7, a monoterpene-derived SCO, represented the highest fraction (10 %) followed by an isoprene-derived SCO. The anthropogenic SCOs with polycyclic aromatic hydrocarbon (PAH) and aromatic precursors dominated the SCO mass loading (51 %) with C11H11SO7, derived from methyl naphthalene oxidation, contributing to 40 ng m(-3) and 0.3% of the OA mass. Anthropogenic-related SCOs correlated well with benzene, although their abundance depended highly on the photochemical age of the air mass, tracked using the ratio between pinonic acid and its oxidation product, acting as a qualitative photochemical clock. In addition to typical anthropogenic and biogenic precursors the biomass-burning precursor nitrophenol (NP) provided a significant level of NP OS. It must be noted that the contribution analysis here is only representative of the detected SCOs. There are likely to be many more SCOs present which the CIMS has not identified. Gas- and particle-phase measurements of glycolic acid suggest that partitioning towards the particle phase promotes glycolic acid sulfate production, contrary to the current formation mechanism suggested in the literature. Furthermore, the HSO4 center dot H2SO4- cluster measured by the CIMS was utilized as a qualitative marker for acidity and indicates that the production of total SCOs is efficient in highly acidic aerosols with high SO42- and organic content. This dependency becomes more complex when observing individual SCOs due to variability of specific VOC precursors.
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