Water-soluble organic matter(WSOM) represents a critical fraction of fine particles(PM2.5)in the air, but its changing behaviors and formation mechanisms are not well understood yet, partly due to the lack of fast...Water-soluble organic matter(WSOM) represents a critical fraction of fine particles(PM2.5)in the air, but its changing behaviors and formation mechanisms are not well understood yet, partly due to the lack of fast techniques for the ambient measurements. In this study,a novel system for the on-line measurement of water-soluble components in PM2.5, the particle-into-liquid sampler(PILS)–Nebulizer–aerosol chemical speciation monitor(ACSM), was developed by combining a PILS, a nebulizer, and an ACSM. High time resolution concentrations of WSOM, sulfate, nitrate, ammonium, and chloride, as well as mass spectra, can be obtained with satisfied quality control results. The system was firstly applied in China for field measurement of WSOM. The mass spectrum of WSOM was found to resemble that of oxygenated organic aerosol, and WSOM agreed well with secondary inorganic ions. All evidence collected in the field campaign demonstrated that WSOM could be a good surrogate of secondary organic aerosol(SOA). The PILS–Nebulizer–ACSM system can thus be a useful tool for intensive study of WSOM and SOA in PM2.5.展开更多
Submicron aerosol particles (with aerody- namic diameters less than 1 pm, PM1) were sampled and measured in Heshan, an urban outflow site of Guangzhou megacity in Pearl River Delta in South China, using an Aerodyne ...Submicron aerosol particles (with aerody- namic diameters less than 1 pm, PM1) were sampled and measured in Heshan, an urban outflow site of Guangzhou megacity in Pearl River Delta in South China, using an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) in November 2010 during 2010 Guangzhou Asian Games. The mean PM~ mass concentration measured was 47.9 ± 17.0 μg.m3 during the campaign, with organic aerosol (OA) and sulfate being the two dominant species, accounting for 36.3% and 20.9% of the total mass, respectively, followed by black carbon (17.1%, measured by an aethalometer), nitrate (12.9%), ammonium (9.6%) and chloride (3.1%). The average size distributions of the species (except black carbon) were dominated by an accumulation mode peaking at -550 nm. Calculations based on high-resolution organic mass spectrum showed that, C, H, O and N on average contributed 58.1%, 7.3%, 30.7%, and 3.9% to the total organic mass, respectively. The average ratio of organic mass over organic carbon mass (OM/OC) was 1.73 ± 0.08. Four components of OA were identified by the Positive Matrix Factorization (PMF) analysis, including a hydro- carbon-like (HOA), a biomass burning (BBOA) and two oxygenated (SV-OOA and LV-OOA) organic aerosol components, which on average accounted for 18.0%, 14.3%, 28.8% and 38.9% of the total organic mass, respectively.展开更多
Haze in China is primarily caused by high pollution of atmospheric fine particulates(PM2.5).However, the detailed source structures of PM2.5 light extinction have not been well established, especially for the roles ...Haze in China is primarily caused by high pollution of atmospheric fine particulates(PM2.5).However, the detailed source structures of PM2.5 light extinction have not been well established, especially for the roles of various organic aerosols, which makes haze management lack specified targets. This study obtained the mass concentrations of the chemical compositions and the light extinction coefficients of fine particles in the winter in Dongguan, Guangdong Province, using high time resolution aerosol observation instruments. We combined the positive matrix factor(PMF) analysis model of organic aerosols and the multiple linear regression method to establish a quantitative relationship model between the main chemical components, in particular the different sources of organic aerosols and the extinction coefficients of fine particles with a high goodness of fit(R^2= 0.953). The results show that the contribution rates of ammonium sulphate,ammonium nitrate, biomass burning organic aerosol(BBOA), secondary organic aerosol(SOA) and black carbon(BC) were 48.1%, 20.7%, 15.0%, 10.6%, and 5.6%, respectively. It can be seen that the contribution of the secondary aerosols is much higher than that of the primary aerosols(79.4% versus 20.6%) and are a major factor in the visibility decline. BBOA is found to have a high visibility destroying potential, with a high mass extinction coefficient, and was the largest contributor during some high pollution periods. A more detailed analysis indicates that the contribution of the enhanced absorption caused by BC mixing state was approximately 37.7% of the total particle absorption and should not be neglected.展开更多
Herein,we use an oxidation flow reactor,Gothenburg:Potential Aerosol Mass(Go:PAM)reactor,to investigate the secondary organic aerosol(SOA)formation from wheat straw burning.Biomass burning emissions are exposed to hig...Herein,we use an oxidation flow reactor,Gothenburg:Potential Aerosol Mass(Go:PAM)reactor,to investigate the secondary organic aerosol(SOA)formation from wheat straw burning.Biomass burning emissions are exposed to high concentrations of hydroxyl radicals(OH)to simulate processes equivalent to atmospheric oxidation of 0-2.55 days.Primary volatile organic compounds(VOCs)were investigated,and particles were measured before and after the Go:PAM reactor.The influence of water content(i.e.5%and 11%)in wheat straw was also explored.Two burning stages,the flaming stage,and non-flaming stages,were identified.Primary particle emission factors(EFs)at a water content of 11%(~3.89 g/kg-fuel)are significantly higher than those at a water content of 5%(~2.26 g/kg-fuel)during the flaming stage.However,the water content showed no significant influence at the non-flaming stage.EFs of aromatics at a non-flaming stage(321.8±46.2 mg/kg-fuel)are larger than that at a flaming stage(130.9±37.1 mg/kg-fuel).The OA enhancement ratios increased with the increase in OH exposure at first and decreased with the additional increment of OH exposure.The maximum OA enhancement ratio is~12 during the non-flaming stages,which is much higher than~1.7 during the flaming stages.The mass spectrum of the primary wheat burning organic aerosols closely resembles that of resolved biomass burning organic aerosols(BBOA)based on measurements in ambient air.Our results show that large gap(0%-90%)still remains to estimate biomass burning SOA if only the oxidation of VOCs were included.展开更多
基金supported by the National Natural Science Foundation of China(Nos.U1301234,21277003)the Ministry of Science and Technology of China(No.2014BAC21B03)the Science and Technology Plan of Shenzhen Municipality
文摘Water-soluble organic matter(WSOM) represents a critical fraction of fine particles(PM2.5)in the air, but its changing behaviors and formation mechanisms are not well understood yet, partly due to the lack of fast techniques for the ambient measurements. In this study,a novel system for the on-line measurement of water-soluble components in PM2.5, the particle-into-liquid sampler(PILS)–Nebulizer–aerosol chemical speciation monitor(ACSM), was developed by combining a PILS, a nebulizer, and an ACSM. High time resolution concentrations of WSOM, sulfate, nitrate, ammonium, and chloride, as well as mass spectra, can be obtained with satisfied quality control results. The system was firstly applied in China for field measurement of WSOM. The mass spectrum of WSOM was found to resemble that of oxygenated organic aerosol, and WSOM agreed well with secondary inorganic ions. All evidence collected in the field campaign demonstrated that WSOM could be a good surrogate of secondary organic aerosol(SOA). The PILS–Nebulizer–ACSM system can thus be a useful tool for intensive study of WSOM and SOA in PM2.5.
文摘Submicron aerosol particles (with aerody- namic diameters less than 1 pm, PM1) were sampled and measured in Heshan, an urban outflow site of Guangzhou megacity in Pearl River Delta in South China, using an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) in November 2010 during 2010 Guangzhou Asian Games. The mean PM~ mass concentration measured was 47.9 ± 17.0 μg.m3 during the campaign, with organic aerosol (OA) and sulfate being the two dominant species, accounting for 36.3% and 20.9% of the total mass, respectively, followed by black carbon (17.1%, measured by an aethalometer), nitrate (12.9%), ammonium (9.6%) and chloride (3.1%). The average size distributions of the species (except black carbon) were dominated by an accumulation mode peaking at -550 nm. Calculations based on high-resolution organic mass spectrum showed that, C, H, O and N on average contributed 58.1%, 7.3%, 30.7%, and 3.9% to the total organic mass, respectively. The average ratio of organic mass over organic carbon mass (OM/OC) was 1.73 ± 0.08. Four components of OA were identified by the Positive Matrix Factorization (PMF) analysis, including a hydro- carbon-like (HOA), a biomass burning (BBOA) and two oxygenated (SV-OOA and LV-OOA) organic aerosol components, which on average accounted for 18.0%, 14.3%, 28.8% and 38.9% of the total organic mass, respectively.
基金supported by the National Natural Science Foundation of China(Nos.41622304,U1301234)the Ministry of Science and Technology of China(Nos.2014BAC21B03,2016YFC0203600)the Science and Technology Plan of Shenzhen Municipality
文摘Haze in China is primarily caused by high pollution of atmospheric fine particulates(PM2.5).However, the detailed source structures of PM2.5 light extinction have not been well established, especially for the roles of various organic aerosols, which makes haze management lack specified targets. This study obtained the mass concentrations of the chemical compositions and the light extinction coefficients of fine particles in the winter in Dongguan, Guangdong Province, using high time resolution aerosol observation instruments. We combined the positive matrix factor(PMF) analysis model of organic aerosols and the multiple linear regression method to establish a quantitative relationship model between the main chemical components, in particular the different sources of organic aerosols and the extinction coefficients of fine particles with a high goodness of fit(R^2= 0.953). The results show that the contribution rates of ammonium sulphate,ammonium nitrate, biomass burning organic aerosol(BBOA), secondary organic aerosol(SOA) and black carbon(BC) were 48.1%, 20.7%, 15.0%, 10.6%, and 5.6%, respectively. It can be seen that the contribution of the secondary aerosols is much higher than that of the primary aerosols(79.4% versus 20.6%) and are a major factor in the visibility decline. BBOA is found to have a high visibility destroying potential, with a high mass extinction coefficient, and was the largest contributor during some high pollution periods. A more detailed analysis indicates that the contribution of the enhanced absorption caused by BC mixing state was approximately 37.7% of the total particle absorption and should not be neglected.
基金supported by National Natural Science Foundation of China(Nos.51636003,91844301,41977179)Beijing Municipal Science and Technology Commission(No.Z201100008220011)+2 种基金Natural Science Foundation of Beijing(No.8192022)China Postdoctoral Science Foundation(No.2020M680242)the Open Research Fund of State Key Laboratory of Multi-phase Complex Systems(No.MPCS-2021-D-12)
文摘Herein,we use an oxidation flow reactor,Gothenburg:Potential Aerosol Mass(Go:PAM)reactor,to investigate the secondary organic aerosol(SOA)formation from wheat straw burning.Biomass burning emissions are exposed to high concentrations of hydroxyl radicals(OH)to simulate processes equivalent to atmospheric oxidation of 0-2.55 days.Primary volatile organic compounds(VOCs)were investigated,and particles were measured before and after the Go:PAM reactor.The influence of water content(i.e.5%and 11%)in wheat straw was also explored.Two burning stages,the flaming stage,and non-flaming stages,were identified.Primary particle emission factors(EFs)at a water content of 11%(~3.89 g/kg-fuel)are significantly higher than those at a water content of 5%(~2.26 g/kg-fuel)during the flaming stage.However,the water content showed no significant influence at the non-flaming stage.EFs of aromatics at a non-flaming stage(321.8±46.2 mg/kg-fuel)are larger than that at a flaming stage(130.9±37.1 mg/kg-fuel).The OA enhancement ratios increased with the increase in OH exposure at first and decreased with the additional increment of OH exposure.The maximum OA enhancement ratio is~12 during the non-flaming stages,which is much higher than~1.7 during the flaming stages.The mass spectrum of the primary wheat burning organic aerosols closely resembles that of resolved biomass burning organic aerosols(BBOA)based on measurements in ambient air.Our results show that large gap(0%-90%)still remains to estimate biomass burning SOA if only the oxidation of VOCs were included.