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The homoscedasticity assumption (the variance of the error term is the same across all the observations) is a key assumption in the ordinary linear squares (OLS) solution of a linear regression model. The validity of this assumption is examined for a multiple linear regression model used to determine the source contributions to the observed black carbon concentrations at 12 background monitoring sites across China using a hybrid modeling approach. Residual analysis from the traditional OLS method, which assumes that the error term is additive and normally distributed with a mean of zero, shows pronounced heteroscedasticity based on the Breusch–Pagan test for 11 datasets. Noticing that the atmospheric black carbon data are log-normally distributed, we make a new assumption that the error terms are multiplicative and log-normally distributed. When the coefficients of the multilinear regression model are determined using the maximum likelihood estimation (MLE), the distribution of the residuals in 8 out of the 12 datasets is in good accordance with the revised assumption. Furthermore, the MLE computation under this novel assumption could be proved mathematically identical to minimizing a log-scale objective function, which considerably reduces the complexity in the MLE calculation. The new method is further demonstrated to have clear advantages in numerical simulation experiments of a 5-variable multiple linear regression model using synthesized data with prescribed coefficients and lognormally distributed multiplicative errors. Under all 9 simulation scenarios, the new method yields the most accurate estimations of the regression coefficients and has significantly higher coverage probability (on average, 95% for all five coefficients) than OLS (79%) and weighted least squares (WLS, 72%) methods. © 2020 Elsevier B.V.

The homoscedasticity assumption (the variance of the error term is the same across all the observations) is a key assumption in the ordinary linear squares (OLS) solution of a linear regression model. The validity of this assumption is examined for a multiple linear regression model used to determine the source contributions to the observed black carbon concentrations at 12 background monitoring sites across China using a hybrid modeling approach. Residual analysis from the traditional OLS method, which assumes that the error term is additive and normally distributed with a mean of zero, shows pronounced heteroscedasticity based on the Breusch–Pagan test for 11 datasets. Noticing that the atmospheric black carbon data are log-normally distributed, we make a new assumption that the error terms are multiplicative and log-normally distributed. When the coefficients of the multilinear regression model are determined using the maximum likelihood estimation (MLE), the distribution of the residuals in 8 out of the 12 datasets is in good accordance with the revised assumption. Furthermore, the MLE computation under this novel assumption could be proved mathematically identical to minimizing a log-scale objective function, which considerably reduces the complexity in the MLE calculation. The new method is further demonstrated to have clear advantages in numerical simulation experiments of a 5-variable multiple linear regression model using synthesized data with prescribed coefficients and lognormally distributed multiplicative errors. Under all 9 simulation scenarios, the new method yields the most accurate estimations of the regression coefficients and has significantly higher coverage probability (on average, 95% for all five coefficients) than OLS (79%) and weighted least squares (WLS, 72%) methods. © 2020 Elsevier B.V.

Severe events of wintertime particulate air pollution in Beijing (winter haze) are associated with high relative humidity (RH) and fast production of particulate sulfate from the oxidation of sulfur dioxide (SO2) emitted by coal combustion. There has been considerable debate regarding the mechanism for SO2 oxidation. Here we show evidence from field observations of a haze event that rapid oxidation of SO2 by nitrogen dioxide (NO2) and nitrous acid (HONO) takes place, the latter producing nitrous oxide (N2O). Sulfate shifts to larger particle sizes during the event, indicative of fog/cloud processing. Fog and cloud readily form under winter haze conditions, leading to high liquid water contents with high pH (>5.5) from elevated ammonia. Such conditions enable fast aqueous-phase oxidation of SO2 by NO2, producing HONO which can in turn oxidize SO2 to yield N2O.This mechanism could provide an explanation for sulfate formation under some winter haze conditions.

The Atmospheric Pollution and Human Health in a Chinese Megacity (APHH-Beijing) programme is an international collaborative project focusing on understanding the sources, processes and health effects of air pollution in the Beijing megacity. APHH-Beijing brings together leading China and UK research groups, state-of-the-art infrastructure and air quality models to work on four research themes: (1) sources and emissions of air pollutants; (2) atmospheric processes affecting urban air pollution; (3) air pollution exposure and health impacts; and (4) interventions and solutions. Themes 1 and 2 are closely integrated and support Theme 3, while Themes 1–3 provide scientific data for Theme 4 to develop cost-effective air pollution mitigation solutions. This paper provides an introduction to (i) the rationale of the APHH-Beijing programme and (ii) the measurement and modelling activities performed as part of it. In addition, this paper introduces the meteorology and air quality conditions during two joint intensive field campaigns – a core integration activity in APHH-Beijing. The coordinated campaigns provided observations of the atmospheric chemistry and physics at two sites: (i) the Institute of Atmospheric Physics in central Beijing and (ii) Pinggu in rural Beijing during 10 November–10 December 2016 (winter) and 21 May–22 June 2017 (summer). The campaigns were complemented by numerical modelling and automatic air quality and low-cost sensor observations in the Beijing megacity. In summary, the paper provides background information on the APHH-Beijing programme and sets the scene for more focused papers addressing specific aspects, processes and effects of air pollution in Beijing.

The Atmospheric Pollution and Human Health in a Chinese Megacity (APHH-Beijing) programme is an international collaborative project focusing on understanding the sources, processes and health effects of air pollution in the Beijing megacity. APHH-Beijing brings together leading China and UK research groups, state-of-the-art infrastructure and air quality models to work on four research themes: (1) sources and emissions of air pollutants; (2) atmospheric processes affecting urban air pollution; (3) air pollution exposure and health impacts; and (4) interventions and solutions. Themes 1 and 2 are closely integrated and support Theme 3, while Themes 1–3 provide scientific data for Theme 4 to develop cost-effective air pollution mitigation solutions. This paper provides an introduction to (i) the rationale of the APHH-Beijing programme and (ii) the measurement and modelling activities performed as part of it. In addition, this paper introduces the meteorology and air quality conditions during two joint intensive field campaigns – a core integration activity in APHH-Beijing. The coordinated campaigns provided observations of the atmospheric chemistry and physics at two sites: (i) the Institute of Atmospheric Physics in central Beijing and (ii) Pinggu in rural Beijing during 10 November–10 December 2016 (winter) and 21 May–22 June 2017 (summer). The campaigns were complemented by numerical modelling and automatic air quality and low-cost sensor observations in the Beijing megacity. In summary, the paper provides background information on the APHH-Beijing programme and sets the scene for more focused papers addressing specific aspects, processes and effects of air pollution in Beijing.

info:eu-repo/semantics/published

Satellite measurements from the thermal Infrared Atmospheric Sounding Interferometer (IASI), aircraft data from the MOZAIC/IAGOS project, as well as observations from ground-based stations, are used to assess the tropospheric ozone (O3) variability during the East Asian Summer Monsoon (EASM). Six years 2008-2013 of IASI data analysis reveals the ability of the instrument to detect the onset and the progression of the monsoon seen by a decrease in the tropospheric 0-6km O3 column due to the EASM, and to reproduce this decrease from one year to the other. The year-to-year variability is found to be mainly dependent on meteorology. Focusing on the period of May-August 2011, taken as an example year, IASI data show clear inverse relationship between tropospheric 0-6km O3 on one hand and meteorological parameters such as cloud cover, relative humidity and wind speed, on the other hand. Aircraft data from the MOZAIC/IAGOS project for the EASM of 2008-2013 are used to validate the IASI data and to assess the effect of the monsoon on the vertical distribution of the tropospheric O3 at different locations. Results show good agreement with a correlation coefficient of 0.73 (12%) between the 0-6km O3 column derived from IASI and aircraft data. IASI captures very well the inter-annual variation of tropospheric O3 observed by the aircraft data over the studied domain. Analysis of vertical profiles of the aircraft data shows a decrease in the tropospheric O3 that is more important in the free troposphere than in the boundary layer and at 10-20°N than elsewhere. Ground station data at different locations in India and China show a spatiotemporal dependence on meteorology during the monsoon, with a decrease up to 22ppbv in Hyderabad, and up to 5ppbv in the North China Plain., SCOPUS: ar.j, SCOPUS: re.j, info:eu-repo/semantics/published

Polyurethane foam disk passive air sampling was carried out to investigate the levels, vertical distributions, and potential sources of polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs) and organochlorine pesticides (OCPs) in the atmospheric boundary layer of an urban site in Asia. Sampling was performed at nine heights (15, 47, 80, 120, 160, 200, 240, 280, 320 m) of the 325-m meteorological tower in Beijing, China over three 2-month periods between December 2006 and August 2007. This is the first study to report vertical variations of PBDEs in the ABL and one of only a few studies to investigate vertical distributions of persistent organic pollutants. The levels of sigma19PCBs and sigma8PBDEs were relatively low, ranging from 22 to 65 and from 2.3 to 18 pg m-3, respectively. Air concentrations of gamma-HCH were high, with values in the range of 39-103 pg m-3 in winter, 100-180 pg m-3 in spring, and 115-242 pg m-3 in summer, respectively. alpha-HCH concentrations ranged from 20 to 86 pg m-3, p,p'-DDT between 7.3 and 78 pg m-3, and HCB between 15 and 160 pg m-3. The seasonal variations of PCBs, PBDEs, and OCPs may reflect different sources for these chemicals, such as those related with regional use (gamma-HCH), volatilization/re-emission (PBDEs, PCBs, alpha-HCH), and pesticide impurities (HCB). Although the performance reference compounds (PRCs) were spiked before deployment, the sampling rates showed strong dependency on wind speeds, resulting in large variations in uptake rates in the ABL, ranging from approximately 7.0 m3 day-1 at ground level to 11 m3 day-1 at 320 m. Levels of PCBs, PBDEs, and OCPs decreased with increasing ABL height indicating the potential of Beijing as the local sources., Sponsors:National Natural Science Foundation of China Grant(s): 20621703 20897010 National Basic Research Program of China Grant(s): 2009CB421605 Chinese Academy of Sciences Grant(s): KJCX2-YW-H04

Polyurethane foam disk passive air sampling was carried out to investigate the levels, vertical distributions, and potential sources of polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs) and organochlorine pesticides (OCPs) in the atmospheric boundary layer of an urban site in Asia. Sampling was performed at nine heights (15, 47, 80, 120, 160, 200, 240, 280, 320 m) of the 325-m meteorological tower in Beijing, China over three 2-month periods between December 2006 and August 2007. This is the first study to report vertical variations of PBDEs in the ABL and one of only a few studies to investigate vertical distributions of persistent organic pollutants. The levels of sigma19PCBs and sigma8PBDEs were relatively low, ranging from 22 to 65 and from 2.3 to 18 pg m-3, respectively. Air concentrations of gamma-HCH were high, with values in the range of 39-103 pg m-3 in winter, 100-180 pg m-3 in spring, and 115-242 pg m-3 in summer, respectively. alpha-HCH concentrations ranged from 20 to 86 pg m-3, p,p'-DDT between 7.3 and 78 pg m-3, and HCB between 15 and 160 pg m-3. The seasonal variations of PCBs, PBDEs, and OCPs may reflect different sources for these chemicals, such as those related with regional use (gamma-HCH), volatilization/re-emission (PBDEs, PCBs, alpha-HCH), and pesticide impurities (HCB). Although the performance reference compounds (PRCs) were spiked before deployment, the sampling rates showed strong dependency on wind speeds, resulting in large variations in uptake rates in the ABL, ranging from approximately 7.0 m3 day-1 at ground level to 11 m3 day-1 at 320 m. Levels of PCBs, PBDEs, and OCPs decreased with increasing ABL height indicating the potential of Beijing as the local sources., Sponsors:National Natural Science Foundation of China Grant(s): 20621703 20897010 National Basic Research Program of China Grant(s): 2009CB421605 Chinese Academy of Sciences Grant(s): KJCX2-YW-H04

Three monosaccharide anhydrides (MAs: levoglucosan, mannosan, and galactosan) and sugar alcohols (arabitol and mannitol) are widely used as organic tracers for source identification of aerosols emitted from biomass burning and fungal spores, respectively. In the past, these two types of organic tracer have been measured separately or conjointly using different analytical techniques, with which a number of disadvantages have been experienced during the application to environmental aerosol samples, including organic solvent involved extraction, time-consuming derivatization, or poor separation efficiency due to overlapping peaks, etc. Hence, in this study a more environment-friendly, effective and integrated extraction and analytical method has been developed for simultaneous determination of the above mentioned organic tracers in the same aerosol sample using ultrasonication and high performance liquid chromatography with tandem mass spectrometry (HPLC-MS/MS). The ultrasonication assisted extraction process using ultrapure water can achieve satisfactory recoveries in the range of 100.3 ± 1.3% to 108.4 ± 1.6% for these tracers. All the parameters related to LC and MS/MS have been optimized to ensure good identification and pronounced intensity for each compound. A series of rigorous validation steps have been conducted. This newly developed analytical method using ultrasonication and HPLC-MS/MS has been successfully applied to environmental aerosol samples of different pollution levels for the simultaneous measurement of the above mentioned five organic tracers from biomass burning and fungal spores.

Three monosaccharide anhydrides (MAs: levoglucosan, mannosan, and galactosan) and sugar alcohols (arabitol and mannitol) are widely used as organic tracers for source identification of aerosols emitted from biomass burning and fungal spores, respectively. In the past, these two types of organic tracer have been measured separately or conjointly using different analytical techniques, with which a number of disadvantages have been experienced during the application to environmental aerosol samples, including organic solvent involved extraction, time-consuming derivatization, or poor separation efficiency due to overlapping peaks, etc. Hence, in this study a more environment-friendly, effective and integrated extraction and analytical method has been developed for simultaneous determination of the above mentioned organic tracers in the same aerosol sample using ultrasonication and high performance liquid chromatography with tandem mass spectrometry (HPLC-MS/MS). The ultrasonication assisted extraction process using ultrapure water can achieve satisfactory recoveries in the range of 100.3 ± 1.3% to 108.4 ± 1.6% for these tracers. All the parameters related to LC and MS/MS have been optimized to ensure good identification and pronounced intensity for each compound. A series of rigorous validation steps have been conducted. This newly developed analytical method using ultrasonication and HPLC-MS/MS has been successfully applied to environmental aerosol samples of different pollution levels for the simultaneous measurement of the above mentioned five organic tracers from biomass burning and fungal spores.

Three monosaccharide anhydrides (MAs: levoglucosan, mannosan, and galactosan) and sugar alcohols (arabitol and mannitol) are widely used as organic tracers for source identification of aerosols emitted from biomass burning and fungal spores, respectively. In the past, these two types of organic tracer have been measured separately or conjointly using different analytical techniques, with which a number of disadvantages have been experienced during the application to environmental aerosol samples, including organic solvent involved extraction, time-consuming derivatization, or poor separation efficiency due to overlapping peaks, etc. Hence, in this study a more environment-friendly, effective and integrated extraction and analytical method has been developed for simultaneous determination of the above mentioned organic tracers in the same aerosol sample using ultrasonication and high performance liquid chromatography with tandem mass spectrometry (HPLC-MS/MS). The ultrasonication assisted extraction process using ultrapure water can achieve satisfactory recoveries in the range of 100.3 ± 1.3% to 108.4 ± 1.6% for these tracers. All the parameters related to LC and MS/MS have been optimized to ensure good identification and pronounced intensity for each compound. A series of rigorous validation steps have been conducted. This newly developed analytical method using ultrasonication and HPLC-MS/MS has been successfully applied to environmental aerosol samples of different pollution levels for the simultaneous measurement of the above mentioned five organic tracers from biomass burning and fungal spores.

Three monosaccharide anhydrides (MAs: levoglucosan, mannosan, and galactosan) and sugar alcohols (arabitol and mannitol) are widely used as organic tracers for source identification of aerosols emitted from biomass burning and fungal spores, respectively. In the past, these two types of organic tracer have been measured separately or conjointly using different analytical techniques, with which a number of disadvantages have been experienced during the application to environmental aerosol samples, including organic solvent involved extraction, time-consuming derivatization, or poor separation efficiency due to overlapping peaks, etc. Hence, in this study a more environment-friendly, effective and integrated extraction and analytical method has been developed for simultaneous determination of the above mentioned organic tracers in the same aerosol sample using ultrasonication and high performance liquid chromatography with tandem mass spectrometry (HPLC-MS/MS). The ultrasonication assisted extraction process using ultrapure water can achieve satisfactory recoveries in the range of 100.3 ± 1.3% to 108.4 ± 1.6% for these tracers. All the parameters related to LC and MS/MS have been optimized to ensure good identification and pronounced intensity for each compound. A series of rigorous validation steps have been conducted. This newly developed analytical method using ultrasonication and HPLC-MS/MS has been successfully applied to environmental aerosol samples of different pollution levels for the simultaneous measurement of the above mentioned five organic tracers from biomass burning and fungal spores.

Three monosaccharide anhydrides (MAs: levoglucosan, mannosan, and galactosan) and sugar alcohols (arabitol and mannitol) are widely used as organic tracers for source identification of aerosols emitted from biomass burning and fungal spores, respectively. In the past, these two types of organic tracer have been measured separately or conjointly using different analytical techniques, with which a number of disadvantages have been experienced during the application to environmental aerosol samples, including organic solvent involved extraction, time-consuming derivatization, or poor separation efficiency due to overlapping peaks, etc. Hence, in this study a more environment-friendly, effective and integrated extraction and analytical method has been developed for simultaneous determination of the above mentioned organic tracers in the same aerosol sample using ultrasonication and high performance liquid chromatography with tandem mass spectrometry (HPLC-MS/MS). The ultrasonication assisted extraction process using ultrapure water can achieve satisfactory recoveries in the range of 100.3 ± 1.3% to 108.4 ± 1.6% for these tracers. All the parameters related to LC and MS/MS have been optimized to ensure good identification and pronounced intensity for each compound. A series of rigorous validation steps have been conducted. This newly developed analytical method using ultrasonication and HPLC-MS/MS has been successfully applied to environmental aerosol samples of different pollution levels for the simultaneous measurement of the above mentioned five organic tracers from biomass burning and fungal spores.

Three monosaccharide anhydrides (MAs: levoglucosan, mannosan, and galactosan) and sugar alcohols (arabitol and mannitol) are widely used as organic tracers for source identification of aerosols emitted from biomass burning and fungal spores, respectively. In the past, these two types of organic tracer have been measured separately or conjointly using different analytical techniques, with which a number of disadvantages have been experienced during the application to environmental aerosol samples, including organic solvent involved extraction, time-consuming derivatization, or poor separation efficiency due to overlapping peaks, etc. Hence, in this study a more environment-friendly, effective and integrated extraction and analytical method has been developed for simultaneous determination of the above mentioned organic tracers in the same aerosol sample using ultrasonication and high performance liquid chromatography with tandem mass spectrometry (HPLC-MS/MS). The ultrasonication assisted extraction process using ultrapure water can achieve satisfactory recoveries in the range of 100.3 ± 1.3% to 108.4 ± 1.6% for these tracers. All the parameters related to LC and MS/MS have been optimized to ensure good identification and pronounced intensity for each compound. A series of rigorous validation steps have been conducted. This newly developed analytical method using ultrasonication and HPLC-MS/MS has been successfully applied to environmental aerosol samples of different pollution levels for the simultaneous measurement of the above mentioned five organic tracers from biomass burning and fungal spores.