scholarly journals Estimates of the organic aerosol volatility in a boreal forest using two independent methods

2017 ◽  
Vol 17 (6) ◽  
pp. 4387-4399 ◽  
Author(s):  
Juan Hong ◽  
Mikko Äijälä ◽  
Silja A. K. Häme ◽  
Liqing Hao ◽  
Jonathan Duplissy ◽  
...  
Keyword(s):  
Boreal Forest ◽  
Organic Aerosols ◽  
Field Measurements ◽  
Accommodation Coefficient ◽  
Vaporization Enthalpy ◽  
Particle Phase ◽  
Forest Environment ◽  
Aerosol Mass ◽  
Mass Accommodation Coefficient ◽  
Mass Fractions

Abstract. The volatility distribution of secondary organic aerosols that formed and had undergone aging – i.e., the particle mass fractions of semi-volatile, low-volatility and extremely low volatility organic compounds in the particle phase – was characterized in a boreal forest environment of Hyytiälä, southern Finland. This was done by interpreting field measurements using a volatility tandem differential mobility analyzer (VTDMA) with a kinetic evaporation model. The field measurements were performed during April and May 2014. On average, 40 % of the organics in particles were semi-volatile, 34 % were low-volatility organics and 26 % were extremely low volatility organics. The model was, however, very sensitive to the vaporization enthalpies assumed for the organics (ΔHVAP). The best agreement between the observed and modeled temperature dependence of the evaporation was obtained when effective vaporization enthalpy values of 80 kJ mol−1 were assumed. There are several potential reasons for the low effective enthalpy value, including molecular decomposition or dissociation that might occur in the particle phase upon heating, mixture effects and compound-dependent uncertainties in the mass accommodation coefficient. In addition to the VTDMA-based analysis, semi-volatile and low-volatility organic mass fractions were independently determined by applying positive matrix factorization (PMF) to high-resolution aerosol mass spectrometer (HR-AMS) data. The factor separation was based on the oxygenation levels of organics, specifically the relative abundance of mass ions at m∕z 43 (f43) and m∕z 44 (f44). The mass fractions of these two organic groups were compared against the VTDMA-based results. In general, the best agreement between the VTDMA results and the PMF-derived mass fractions of organics was obtained when ΔHVAP =  80 kJ mol−1 was set for all organic groups in the model, with a linear correlation coefficient of around 0.4. However, this still indicates that only about 16 % (R2) of the variation can be explained by the linear regression between the results from these two methods. The prospect of determining of extremely low volatility organic aerosols (ELVOAs) from AMS data using the PMF analysis should be assessed in future studies.

scholarly journals Estimates of the organic aerosol volatility in a boreal forest using two independent methods

2016 ◽  
Author(s):  
Juan Hong ◽  
Mikko Äijälä ◽  
Silja A. K. Häme ◽  
Liqing Hao ◽  
Jonathan Duplissy ◽  
...  
Keyword(s):  
Boreal Forest ◽  
Organic Aerosols ◽  
Field Measurements ◽  
Accommodation Coefficient ◽  
Vaporization Enthalpy ◽  
Forest Environment ◽  
Aerosol Mass ◽  
Mass Accommodation Coefficient ◽  
Volatile Organic ◽  
Mass Fractions

Abstract. Volatility distribution of secondary organic aerosols, i.e. the particle mass fractions of semi-volatile, low-volatility and extremely low-volatility organic compounds was characterized in a boreal forest environment of Hyytiälä, Southern Finland. This was done by interpreting field measurements using a Volatility Tandem Differential Mobility Analyzer (VTDMA) with a kinetic evaporation model. The field measurements were performed during April and May of 2014. On average, 40 % of organics in particles was semi-volatile; 34 % low-volatility organics and 26 % extremely low-volatility organics. The model was, however, very sensitive towards the vaporization enthalpies assumed for the organics (ΔHVAP). The best agreement between the observed and modeled temperature-dependence of the evaporation was obtained when effective vaporization enthalpy values of 80 kJ/mol were assumed. The low effective enthalpy value might result from several potential reasons, including molecular decomposition or dissociation that might occur in the particle phase upon heating, mixture effects and compound-dependent uncertainties in the mass accommodation coefficient. In addition to the VTDMA-based analysis, semi-volatile and low-volatile organic mass fractions were independently determined by applying Positive Matrix Factorization (PMF) to High-Resolution Aerosol Mass Spectrometer (HR-AMS) data. The factor separation was based on the oxygenation levels of organics, specifically the relative abundance of mass ions at m/z 43 (f43) and m/z 44 (f44). The mass fractions of these two organic groups were compared against the VTDMA-based results. In general, the agreement between the VTDMA results and the PMF-derived mass fractions of organics was reasonable with a linear correlation coefficient of around 0.4 with ΔHVAP = 80 kJ/mol set for all organic groups. The prospect of determining of extremely low volatile organic aerosols (ELVOA) from AMS data using the PMF analysis should be assessed in future studies.

scholarly journals Mass accommodation and gas–particle partitioning in secondary organic aerosols: dependence on diffusivity, volatility, particle-phase reactions, and penetration depth

2021 ◽  
Vol 21 (3) ◽  
pp. 1565-1580
Author(s):  
Manabu Shiraiwa ◽  
Ulrich Pöschl
Keyword(s):  
Effective Mass ◽  
Penetration Depth ◽  
Secondary Organic Aerosols ◽  
Organic Aerosols ◽  
Accommodation Coefficient ◽  
Solid Particles ◽  
Particle Phase ◽  
Multilayer Model ◽  
Mass Accommodation Coefficient ◽  
Semi Solid

Abstract. Mass accommodation is an essential process for gas–particle partitioning of organic compounds in secondary organic aerosols (SOA). The mass accommodation coefficient is commonly described as the probability of a gas molecule colliding with the surface to enter the particle phase. It is often applied, however, without specifying if and how deep a molecule has to penetrate beneath the surface to be regarded as being incorporated into the condensed phase (adsorption vs. absorption). While this aspect is usually not critical for liquid particles with rapid surface–bulk exchange, it can be important for viscous semi-solid or glassy solid particles to distinguish and resolve the kinetics of accommodation at the surface, transfer across the gas–particle interface, and further transport into the particle bulk. For this purpose, we introduce a novel parameter: an effective mass accommodation coefficient αeff that depends on penetration depth and is a function of surface accommodation coefficient, volatility, bulk diffusivity, and particle-phase reaction rate coefficient. Application of αeff in the traditional Fuchs–Sutugin approximation of mass-transport kinetics at the gas–particle interface yields SOA partitioning results that are consistent with a detailed kinetic multilayer model (kinetic multilayer model of gas–particle interactions in aerosols and clouds, KM-GAP; Shiraiwa et al., 2012) and two-film model solutions (Model for Simulating Aerosol Interactions and Chemistry, MOSAIC; Zaveri et al., 2014) but deviate substantially from earlier modeling approaches not considering the influence of penetration depth and related parameters. For highly viscous or semi-solid particles, we show that the effective mass accommodation coefficient remains similar to the surface accommodation coefficient in the case of low-volatility compounds, whereas it can decrease by several orders of magnitude in the case of semi-volatile compounds. Such effects can explain apparent inconsistencies between earlier studies deriving mass accommodation coefficients from experimental data or from molecular dynamics simulations. Our findings challenge the approach of traditional SOA models using the Fuchs–Sutugin approximation of mass transfer kinetics with a fixed mass accommodation coefficient, regardless of particle phase state and penetration depth. The effective mass accommodation coefficient introduced in this study provides an efficient new way of accounting for the influence of volatility, diffusivity, and particle-phase reactions on SOA partitioning in process models as well as in regional and global air quality models. While kinetic limitations may not be critical for partitioning into liquid SOA particles in the planetary boundary layer (PBL), the effects are likely important for amorphous semi-solid or glassy SOA in the free and upper troposphere (FT–UT) as well as in the PBL at low relative humidity and low temperature.

scholarly journals Mass Accommodation and Gas-Particle Partitioning in Secondary Organic Aerosols: Dependence on Diffusivity, Volatility, Particle-phase Reactions, and Penetration Depth

2020 ◽  
Author(s):  
Manabu Shiraiwa ◽  
Ulrich Pöschl
Keyword(s):  
Volatile Compounds ◽  
Effective Mass ◽  
Penetration Depth ◽  
Secondary Organic Aerosols ◽  
Organic Aerosols ◽  
Accommodation Coefficient ◽  
Solid Particles ◽  
Phase Reaction ◽  
Particle Phase ◽  
Mass Accommodation Coefficient

Abstract. Mass accommodation is an essential process for gas-particle partitioning of organic compounds in secondary organic aerosols (SOA). The mass accommodation coefficient is commonly described as the probability of a gas molecule colliding with the surface to enter the particle phase. It is often applied, however, without specifying if and how deep a molecule has to penetrate beneath the surface to be regarded as incorporated into the condensed phase (adsorption vs. absorption). While this aspect is usually not critical for liquid particles with rapid surface-bulk exchange, it can be important for viscous semisolid or glassy solid particles to distinguish and resolve the kinetics of accommodation at the surface, transfer across the gas-particle interface, and further transport into the particle bulk. For this purpose, we introduce a novel parameter: an effective mass accommodation coefficient αeff that depends on penetration depth and is a function of surface accommodation coefficient, volatility, bulk diffusivity, and particle-phase reaction rate coefficient. Application of αeff in the traditional Fuchs-Sutugin approximation of mass-transport kinetics at the gas-particle interface yields SOA partitioning results that are consistent with a detailed kinetic multilayer model (KM-GAP, Shiraiwa et al., 2012) and two-film model solutions (MOSAIC, Zaveri et al., 2014) but deviate substantially from earlier modeling approaches not considering the influence of penetration depth and related parameters. For highly viscous or semisolid particles, we show that the effective mass accommodation coefficient remains similar to the surface accommodation coefficient in case of low-volatile compounds, whereas it can decrease by several orders of magnitude in case of semi-volatile compounds. Such effects can explain apparent inconsistencies between earlier studies deriving mass accommodation coefficients from experimental data or from molecular dynamics simulations. Our findings challenge the approach of traditional SOA models using the Fuchs-Sutugin approximation of mass transfer kinetics with a fixed mass accommodation coefficient regardless of particle phase state and penetration depth. The effective mass accommodation coefficient introduced in this study provides an efficient new way of accounting for the influence of volatility, diffusivity, and particle-phase reactions on SOA partitioning in process models as well as in regional and global air quality models.

scholarly journals Measuring the atmospheric organic aerosol volatility distribution: a theoretical analysis

2014 ◽  
Vol 7 (9) ◽  
pp. 2953-2965 ◽  
Author(s):  
E. Karnezi ◽  
I. Riipinen ◽  
S. N. Pandis
Keyword(s):  
Experimental Approach ◽  
Organic Aerosol ◽  
Accommodation Coefficient ◽  
Vaporization Enthalpy ◽  
Typical Result ◽  
Volatile Components ◽  
Particulate Phase ◽  
Aerosol Mass ◽  
Mass Accommodation Coefficient ◽  
Atmospheric Concentrations

Abstract. Organic compounds represent a significant fraction of submicrometer atmospheric aerosol mass. Even if most of these compounds are semi-volatile in atmospheric concentrations, the ambient organic aerosol volatility is quite uncertain. The most common volatility measurement method relies on the use of a thermodenuder (TD). The aerosol passes through a heated tube where its more volatile components evaporate, leaving the less volatile components behind in the particulate phase. The typical result of a thermodenuder measurement is the mass fraction remaining (MFR), which depends, among other factors, on the organic aerosol (OA) vaporization enthalpy and the accommodation coefficient. We use a new method combining forward modeling, introduction of "experimental" error, and inverse modeling with error minimization for the interpretation of TD measurements. The OA volatility distribution, its effective vaporization enthalpy, the mass accommodation coefficient and the corresponding uncertainty ranges are calculated. Our results indicate that existing TD-based approaches quite often cannot estimate reliably the OA volatility distribution, leading to large uncertainties, since there are many different combinations of the three properties that can lead to similar thermograms. We propose an improved experimental approach combining TD and isothermal dilution measurements. We evaluate this experimental approach using the same model, and show that it is suitable for studies of OA volatility in the lab and the field.

scholarly journals Measuring the atmospheric organic aerosol volatility distribution: a theoretical analysis

2014 ◽  
Vol 7 (1) ◽  
pp. 859-893 ◽  
Author(s):  
E. Karnezi ◽  
I. Riipinen ◽  
S. N. Pandis
Keyword(s):  
Experimental Approach ◽  
Organic Aerosol ◽  
Accommodation Coefficient ◽  
Vaporization Enthalpy ◽  
Typical Result ◽  
Volatile Components ◽  
Particulate Phase ◽  
Aerosol Mass ◽  
Mass Accommodation Coefficient ◽  
Atmospheric Concentrations

Abstract. Organic compounds represent a significant fraction of submicrometer atmospheric aerosol mass. Even if most of these compounds are semi-volatile in atmospheric concentrations, the ambient organic aerosol volatility is quite uncertain. The most common volatility measurement method relies on the use of a thermodenuder (TD). The aerosol passes through a heated tube where its more volatile components evaporate leaving the less volatile behind in the particulate phase. The typical result of a~thermodenuder measurement is the mass fraction remaining (MFR), which depends among other factors on the organic aerosol (OA) vaporization enthalpy and the accommodation coefficient. We use a new method combining forward modeling, introduction of "experimental" error and inverse modeling with error minimization for the interpretation of TD measurements. The OA volatility distribution, its effective vaporization enthalpy, the mass accommodation coefficient and the corresponding uncertainty ranges are calculated. Our results indicate that existing TD-based approaches quite often cannot estimate reliably the OA volatility distribution, leading to large uncertainties, since there are many different combinations of the three properties that can lead to similar thermograms. We propose an improved experimental approach combining TD and isothermal dilution measurements. We evaluate this experimental approach using the same model and show that it is suitable for studies of OA volatility in the lab and the field.

scholarly journals Studying volatility from composition, dilution, and heating measurements of secondary organic aerosols formed during <i>α</i>-pinene ozonolysis

2018 ◽  
Vol 18 (8) ◽  
pp. 5455-5466 ◽  
Author(s):  
Kei Sato ◽  
Yuji Fujitani ◽  
Satoshi Inomata ◽  
Yu Morino ◽  
Kiyoshi Tanabe ◽  
...  
Keyword(s):  
Secondary Organic Aerosols ◽  
Yield Curve ◽  
Volume Fraction ◽  
Organic Aerosols ◽  
Accommodation Coefficient ◽  
Oh Radicals ◽  
Ionization Mass ◽  
Mass Accommodation Coefficient ◽  
Kinetic Inhibition ◽  
Photochemical Aging

Abstract. Traditional yield curve analysis shows that semi-volatile organic compounds are a major component of secondary organic aerosols (SOAs). We investigated the volatility distribution of SOAs from α-pinene ozonolysis using positive electrospray ionization mass analysis and dilution- and heat-induced evaporation measurements. Laboratory chamber experiments were conducted on α-pinene ozonolysis, in the presence and absence of OH scavengers. Among these, we identified not only semi-volatile products, but also less volatile highly oxygenated molecules (HOMs) and dimers. Ozonolysis products were further exposed to OH radicals to check the effects of photochemical aging. HOMs were also formed during OH-initiated photochemical aging. Most HOMs that formed from ozonolysis and photochemical aging had 10 or fewer carbons. SOA particle evaporation after instantaneous dilution was measured at  < 1 and  ∼ 40 % relative humidity. The volume fraction remaining of SOAs decreased with time and the equilibration timescale was determined to be 24–46 min for SOA evaporation. The experimental results of the equilibration timescale can be explained when the mass accommodation coefficient is assumed to be 0.1, suggesting that the existence of low-volatility materials in SOAs, kinetic inhibition, or some combined effect may affect the equilibration timescale measured in this study.

scholarly journals Relating the hygroscopic properties of submicron aerosol to both gas- and particle-phase chemical composition in a boreal forest environment

2015 ◽  
Vol 15 (11) ◽  
pp. 15511-15541
Author(s):  
J. Hong ◽  
J. Kim ◽  
T. Nieminen ◽  
J. Duplissy ◽  
M. Ehn ◽  
...  
Keyword(s):  
Organic Matter ◽  
Chemical Composition ◽  
Growth Factor ◽  
Boreal Forest ◽  
Gas Phase ◽  
Mixing Rule ◽  
Particle Phase ◽  
Hygroscopic Growth ◽  
Forest Environment ◽  
Composition Data

Abstract. Measurements of the hygroscopicity of 15–145 nm particles in a boreal forest environment were conducted using two Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) systems during the Pan-European Gas-AeroSOIs-climate interaction Study (PEGASOS) campaign in spring 2013. Measurements of the chemical composition of non-size segregated particles were also performed using a High-Resolution Aerosol Mass Spectrometer (HR-AMS) in parallel with hygroscopicity measurements. On average, the hygroscopic growth factor (HGF) of particles was observed to increase from the morning until afternoon. In case of accumulation mode particles, the main reasons for this behavior were increases in the ratio of sulfate to organic matter and oxidation level (O : C ratio) of the organic matter in the particle phase. Using an O : C dependent hygroscopic growth factor of organic matter (HGForg), fitted using the inverse Zdanovskii–Stokes–Robinson (ZSR) mixing rule, clearly improved the agreement between measured HGF and that predicted based on HR-AMS composition data. Besides organic oxidation level, the influence of inorganic species was tested when using the ZSR mixing rule to estimate the hygroscopic growth factor of organics in the aerosols. While accumulation and Aitken mode particles were predicted fairly well by the bulk aerosol composition data, the hygroscopicity of nucleation mode particles showed little correlation. However, we observed them to be more sensitive to the gas phase concentration of condensable vapors: the more there was sulfuric acid in the gas phase, the more hygroscopic the nucleation mode particles were. No clear dependence was found between the extremely low-volatility organics (ELVOCs) concentration and the HGF of particles of any size.

scholarly journals Estimation of the volatility distribution of organic aerosol combining thermodenuder and isothermal dilution measurements

2017 ◽  
Vol 10 (10) ◽  
pp. 3909-3918 ◽  
Author(s):  
Evangelos E. Louvaris ◽  
Eleni Karnezi ◽  
Evangelia Kostenidou ◽  
Christos Kaltsonoudis ◽  
Spyros N. Pandis
Keyword(s):  
Organic Compounds ◽  
Organic Aerosol ◽  
Accommodation Coefficient ◽  
Vaporization Enthalpy ◽  
Semivolatile Organic Compounds ◽  
Scanning Mobility Particle Sizer ◽  
Aerosol Mass ◽  
Clean Air ◽  
Particle Sizer ◽  
Almost All

Abstract. A method is developed following the work of Grieshop et al. (2009) for the determination of the organic aerosol (OA) volatility distribution combining thermodenuder (TD) and isothermal dilution measurements. The approach was tested in experiments that were conducted in a smog chamber using organic aerosol (OA) produced during meat charbroiling. A TD was operated at temperatures ranging from 25 to 250 °C with a 14 s centerline residence time coupled to a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and a scanning mobility particle sizer (SMPS). In parallel, a dilution chamber filled with clean air was used to dilute isothermally the aerosol of the larger chamber by approximately a factor of 10. The OA mass fraction remaining was measured as a function of temperature in the TD and as a function of time in the isothermal dilution chamber. These two sets of measurements were used together to estimate the volatility distribution of the OA and its effective vaporization enthalpy and accommodation coefficient. In the isothermal dilution experiments approximately 20 % of the OA evaporated within 15 min. Almost all the OA evaporated in the TD at approximately 200 °C. The resulting volatility distributions suggested that around 60–75 % of the cooking OA (COA) at concentrations around 500 µg m−3 consisted of low-volatility organic compounds (LVOCs), 20–30 % of semivolatile organic compounds (SVOCs), and around 10 % of intermediate-volatility organic compounds (IVOCs). The estimated effective vaporization enthalpy of COA was 100 ± 20 kJ mol−1 and the effective accommodation coefficient was 0.06–0.07. Addition of the dilution measurements to the TD data results in a lower uncertainty of the estimated vaporization enthalpy as well as the SVOC content of the OA.

scholarly journals Estimation of the volatility distribution of organic aerosol combining thermodenuder and isothermal dilution measurements

2017 ◽  
Author(s):  
Evangelos E. Louvaris ◽  
Eleni Karnezi ◽  
Evangelia Kostenidou ◽  
Christos Kaltsonoudis ◽  
Spyros N. Pandis
Keyword(s):  
Organic Compounds ◽  
Organic Aerosol ◽  
Accommodation Coefficient ◽  
Vaporization Enthalpy ◽  
Scanning Mobility Particle Sizer ◽  
Aerosol Mass ◽  
Clean Air ◽  
Dilution Experiments ◽  
Particle Sizer ◽  
Almost All

Abstract. A method is developed for the determination of the organic aerosol (OA) volatility distribution combining thermodenuder and isothermal dilution measurements. The approach was tested in experiments that were conducted in a smog chamber using organic aerosol (OA) produced during meat charbroiling. A thermodenuder (TD) was operated at temperatures ranging from 25 to 250 °C with a 14 s centerline residence time coupled to a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and a Scanning Mobility Particle Sizer (SMPS). In parallel, a dilution chamber filled with clean air was used to dilute isothermally the aerosol of the larger chamber by approximately a factor of 10. The OA mass fraction remaining was measured as a function of temperature in the TD and as a function of time in the isothermal dilution chamber. These two sets of measurements were used together to estimate the volatility distribution of the OA and its effective vaporization enthalpy and accommodation coefficient. In the isothermal dilution experiments approximately 20 % of the OA evaporated within 15 min. Almost all the OA evaporated in the TD at approximately 200 °C. The resulting volatility distributions suggested that around 60–75 % of the cooking OA (COA) at concentrations around 500 μg m−3 consisted of low volatility organic compounds (LVOCs), 20–30 % of semi-volatile organic compounds (SVOCs) and around 10 % of intermediate volatility organic compounds (IVOCs). The estimated effective vaporization enthalpy of COA was 100 ± 20 kJ mol−1 and the effective accommodation coefficient was 0.06–0.07. Addition of the dilution measurements to the TD data results in a lower uncertainty of the estimated vaporization enthalpy as well as the SVOC content of the OA.

The seasonal cycle of biogenic ice-nucleating particles in a boreal forest environment

2020 ◽  
Author(s):  
Julia Schneider ◽  
Kristina Höhler ◽  
Paavo Heikkilä ◽  
Jorma Keskinen ◽  
Barbara Bertozzi ◽  
...  
Keyword(s):  
Boreal Forest ◽  
Seasonal Cycle ◽  
Field Measurements ◽  
Climate Projections ◽  
Research Station ◽  
Forest Environment ◽  
Institute Of Technology ◽  
The University ◽  
Karlsruhe Institute

&lt;p&gt;By triggering the formation of cloud ice crystals in the atmosphere, ice-nucleating particles (INP) strongly influence cloud properties, cloud life cycle and precipitation. Describing the abundance of atmospheric INPs in weather forecasts and climate projections remains challenging, as the global distribution and variability of INPs depend on a variety of different aerosol types and sources. Although widespread field measurements have been conducted, neither short-term variability nor long-term seasonal cycles have yet been well characterized by continuous measurements. In 2018, the University of Helsinki and the Karlsruhe Institute of Technology (KIT) initiated a field campaign HyICE to perform comprehensive long-term INP measurements in the Finnish boreal forest. The campaign took place in Hyyti&amp;#228;l&amp;#228;, Southern Finland at the University of Helsinki SMEARII research station (Hari and Kulmala, 2005). KIT provided the INSEKT (Ice Nucleation Spectrometer of the Karlsruhe Institute of Technology) to analyse the INP content of ambient aerosols sampled on filters. INSEKT is able to measure INP concentrations in the immersion-freezing mode at temperatures between 273 K and 248 K. The measurements started in March 2018 and ended in May 2019, which provides a unique continuous long-term time series of INP concentrations for over more than one year with a time resolution of about one to three days. This long-term observation record is used to examine systematic seasonal trends in the INP concentrations and to find meteorological and aerosol related parameters to describe the observed trends and variabilities. These findings will enable to find new parameterizations of atmospheric INP concentrations, as current parameterizations do not reproduce the observed seasonal cycle yet. In addition to INP concentration measurements, heat treatment tests of the aerosol samples have been conducted providing additional indications about the INP types dominating the INP population in the boreal forest, also in dependence on the season. Finally, this contribution will summarize and discuss major findings and implications from the HyICE long-term INP observation.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;&lt;p&gt;Hari and Kulmala (2005), Boreal Environ Res. 14, 315-322.&lt;/p&gt;

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