This paper explores the role of the secondary inorganic aerosol (SIA) species ammonium,NH4+,nitrate,NO3-,and sulfate,SO24-,during haze and fog events using hourly mass concentrations of PM2.5 measured at a suburban...This paper explores the role of the secondary inorganic aerosol (SIA) species ammonium,NH4+,nitrate,NO3-,and sulfate,SO24-,during haze and fog events using hourly mass concentrations of PM2.5 measured at a suburban site in Hangzhou,China.A total of 546 samples were collected between 1 April and 8 May 2012.The samples were analyzed and classified as clear,haze or fog depending on visibility and relative humidity (RH).The contribution of SIA species to PM2.5 mass increased to ~50% during haze and fog.The mass contribution of nitrate to PM2.5 increased from 11% during clear to 20% during haze episodes.Nitrate mass exceeded sulfate mass during haze,while near equal concentrations were observed during fog episodes.The role of RH on the correlation between concentrations of SIA and visibility was examined,with optimal correlation at 60%-70% RH.The total acidity during clear,haze and fog periods was 42.38,48.38 and 45.51 nmol m-3,respectively,indicating that sulfate,nitrate and chloride were not neutralized by ammonium during any period.The nitrate to sulfate molar ratio,as a function of the ammonium to sulfate molar ratio,indicated that nitrate formation during fog started at a higher ammonium to sulfate molar ratio compared to clear and haze periods.During haze and fog,the nitrate oxidation ratio increased by a factor of 1.6-1.7,while the sulfur oxidation ratio increased by a factor of 1.2-1.5,indicating that both gaseous NO2 and SO2 were involved in the reduced visibility.展开更多
In this study,online water-soluble inorganic ions were detected to deduce the formation mechanism of secondary inorganic aerosol in Xianyang,China during wintertime.The dominant inorganic ions of sulfate(SO_(4)^(2-)),...In this study,online water-soluble inorganic ions were detected to deduce the formation mechanism of secondary inorganic aerosol in Xianyang,China during wintertime.The dominant inorganic ions of sulfate(SO_(4)^(2-)),nitrate(NO_(3)^(-)),and ammonium(NH_(4)^(+))(the sum of those is abbreviated as SNA)accounted for 17%,21%,and 12% of PM_(2.5)mass,respectively.While the air quality deteriorated from excellent to poor grades,the precursor gas sulfur dioxide(SO_(2))of SO_(4)^(2-)increased and then decreased with a fluctuation,while nitrogen dioxide(NO_(2))and ammonia(NH_(3)),precursors of NO_(3)^(-)and NH_(4)^(+),and SNA show increasing trends.Meteorological factors including boundary layer height(BLH),temperature,and wind speed also show decline trends,except relative humidity(RH).Meanwhile,the secondary conversion ratio shows a remarkable increasing trend,indicating that there was a strong secondary transformation.From the perspective of chemical mechanisms,RH is positively correlated with sulfur oxidation ratios(SOR),nitrogen oxidation ratios(NOR),and ammonia conversion ratios,representing that the increase of humidity could promote the generation of SNA.Notably,SOR and NOR were also positively related to the ammonia.On the one hand,the low wind speed and BLH led to the accumulation of pollutants.On the other hand,the increases of RH and ammonia promoted more formations of SNA and PM_(2.5).The results advance our identification of the contributors to the haze episodes and assist to establish more efficient emission controls in Xianyang,in addition to other cities with similar emission and geographical characteristics.展开更多
A WRF-Chem model including a comprehensive gas-phase nitrogen chemistry module was used to simulate a severe dust event appearing in the eastern China on 19-25 March, 2002. The modeling result well reproduced PM10 con...A WRF-Chem model including a comprehensive gas-phase nitrogen chemistry module was used to simulate a severe dust event appearing in the eastern China on 19-25 March, 2002. The modeling result well reproduced PM10 concentrations in various distances from the dust sources and the transport pathway of the dust strom. The results showed that both the concentrations and the dry deposition fluxes of PM10 increased over the China seas during the dust event following the passage of a cold front system. The maximum fluxes of PM10 in the Yellow Sea and the East China Sea during the dust event were 5.5 and 8.4 times of those before the event, respectively. However, the temporal variations of the dry deposition fluxes of particulate inorganic nitrogen differed over the Yellow Sea from those over the East China Sea. Nitrate and ammonium in the whole northern China rapidly decreased because of the intrusion of dust-loaded air on 19 March. The dust plume arrived in the Yellow Sea on 20 March, decreasing the particulate inorganic nitrogen in mass concentration accordingly. The minimum dry deposition fluxes of nitrate and ammonium in the Yellow Sea were about 3/5 and 1/6 of those before the dust arrival, respectively. In contrast, when the dust plume crossed over the Yangtze Delta area, it became abundant in nitrate and ammonium and increased the concentrations and dry deposition fluxes of particulate inorganic nitrogen over the East China Sea, where the maximum dry deposition fluxes of nitrate and ammonium increased approximately by 4.1 and 2.6 times of those prior to the dust arrival.展开更多
A modified two-dimensional Eulerian air quality model was used to simulate both the gaseous and particulate pollutant concentrations during October 21-24, 2004 in the Pearl River Delta (PRD) region, China. The most ...A modified two-dimensional Eulerian air quality model was used to simulate both the gaseous and particulate pollutant concentrations during October 21-24, 2004 in the Pearl River Delta (PRD) region, China. The most significant improvement to the model is the added capability to predict the secondary organic aerosols (SOA) concentrations because of the inclusion of the SOA formation chemistry. The meteorological input data were prepared using the CALMET meteorological model. The concentrations of aerosol-bound species such as NO3^-, NH4^+, SO4^2-, and SOA were calculated in the fine particle size range (〈2.5 μm). The results of the two-dimensional model were compared to the measurements at the ground level during the PRD Intensive Monitoring Campaign (IMC). Overall, there were good agreements between the measured and modeled concentrations of inorganic aerosol components and O3. Both the measured and the modeled results indicated that the maximum hourly O3 concentrations exceeded the China National Air Quality Standard. The predicted 24-h average SOA concentrations were in reasonable agreement with those predicted by the method of minimum OC/EC ratio.展开更多
A field experiment from 18 August to 8 September 2006 in Beijing, China, was carried out. A hazy day was defined as visibility 〈 10 km and RH(relative humidity) 〈 90%. Four haze episodes, which accounted for ~ 60...A field experiment from 18 August to 8 September 2006 in Beijing, China, was carried out. A hazy day was defined as visibility 〈 10 km and RH(relative humidity) 〈 90%. Four haze episodes, which accounted for ~ 60% of the time during the whole campaign, were characterized by increases of SNA(sulfate, nitrate, and ammonium) and SOA(secondary organic aerosol) concentrations. The average values with standard deviation of SO2-+4, NO-3, NH4 and SOA were 49.8(± 31.6), 31.4(±22.3), 25.8(±16.6) and 8.9(±4.1) μg/m3, respectively, during the haze episodes, which were 4.3, 3.4, 4.1, and 1.7 times those in the non-haze days. The SO2-4,NO-3, NH+4, and SOA accounted for 15.8%, 8.8%, 7.3%, and 6.0% of the total mass concentration of PM10 during the non-haze days. The respective contributions of SNA species to PM10 rose to about27.2%, 15.9%, and 13.9% during the haze days, while the contributions of SOA maintained the same level with a slight decrease to about 4.9%. The observed mass concentrations of SNA and SOA increased with the increase of PM10 mass concentration, however, the rate of increase of SNA was much faster than that of the SOA. The SOR(sulfur oxidation ratio) and NOR(nitrogen oxidation ratio) increased from non-haze days to hazy days, and increased with the increase of RH. High concentrations of aerosols and water vapor favored the conversion of SO2 to SO2-4and NO2 to NO-3, which accelerated the accumulation of the aerosols and resulted in the formation of haze in Beijing.展开更多
Haze episodes have become a major concern in Malaysia over the past few decades and have an increasingly important impact on the country each and every year. During haze episodes from biomass burning in Southeast Asia...Haze episodes have become a major concern in Malaysia over the past few decades and have an increasingly important impact on the country each and every year. During haze episodes from biomass burning in Southeast Asia, particularly from Sumatra, Indonesia, particulate matter PM2.5 is found to be one of the dangerous sources of airborne pollution and is known to seriously affect human health. This study determines the composition of carbohydrates (as levoglucosan), surfactants, major elements, and anions in PM2.5 during a 2013 haze episode. PM2.5 samples were collected from Universiti Kebangsaan Malaysia, Bangi, using a high volume sampler during a seven-day monitoring campaign during the peak of that year's haze episode. PM2.5 concentrations ranged between 14.52 and 160.93 μg/m3, exceeding the 2005 WHO air quality guidelines for PM2.5 (25 μg/m3 for 24-h mean). The patterns for levoglucosan, surfactants, major elements, and anionic compositions were proportional to the PM2.5 concentrations. Changes in PM2.5 observed on days 3 and 4 were influenced by a combination of meteorological factors, which substantiate the theory that such factors play a pivotal role in haze episodes.展开更多
基金supported by the National Natural Science Foundation of China (Grant Nos. 21190053 and 21177025)the Shanghai Science and Technology Commission of Shanghai Municipality (Grant Nos. 12DJ1400100 and 13XD 1400700)the Priority Fields for Ph.D. Programs Foundation of the Ministry of Education of China (Grant No.20110071130003)
文摘This paper explores the role of the secondary inorganic aerosol (SIA) species ammonium,NH4+,nitrate,NO3-,and sulfate,SO24-,during haze and fog events using hourly mass concentrations of PM2.5 measured at a suburban site in Hangzhou,China.A total of 546 samples were collected between 1 April and 8 May 2012.The samples were analyzed and classified as clear,haze or fog depending on visibility and relative humidity (RH).The contribution of SIA species to PM2.5 mass increased to ~50% during haze and fog.The mass contribution of nitrate to PM2.5 increased from 11% during clear to 20% during haze episodes.Nitrate mass exceeded sulfate mass during haze,while near equal concentrations were observed during fog episodes.The role of RH on the correlation between concentrations of SIA and visibility was examined,with optimal correlation at 60%-70% RH.The total acidity during clear,haze and fog periods was 42.38,48.38 and 45.51 nmol m-3,respectively,indicating that sulfate,nitrate and chloride were not neutralized by ammonium during any period.The nitrate to sulfate molar ratio,as a function of the ammonium to sulfate molar ratio,indicated that nitrate formation during fog started at a higher ammonium to sulfate molar ratio compared to clear and haze periods.During haze and fog,the nitrate oxidation ratio increased by a factor of 1.6-1.7,while the sulfur oxidation ratio increased by a factor of 1.2-1.5,indicating that both gaseous NO2 and SO2 were involved in the reduced visibility.
基金supported by the National Key R&D Program of China(No.2022YFF0802501)the Key Research and Development Program of Shaanxi Province(No.2018-ZDXM3-01)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2019402)。
文摘In this study,online water-soluble inorganic ions were detected to deduce the formation mechanism of secondary inorganic aerosol in Xianyang,China during wintertime.The dominant inorganic ions of sulfate(SO_(4)^(2-)),nitrate(NO_(3)^(-)),and ammonium(NH_(4)^(+))(the sum of those is abbreviated as SNA)accounted for 17%,21%,and 12% of PM_(2.5)mass,respectively.While the air quality deteriorated from excellent to poor grades,the precursor gas sulfur dioxide(SO_(2))of SO_(4)^(2-)increased and then decreased with a fluctuation,while nitrogen dioxide(NO_(2))and ammonia(NH_(3)),precursors of NO_(3)^(-)and NH_(4)^(+),and SNA show increasing trends.Meteorological factors including boundary layer height(BLH),temperature,and wind speed also show decline trends,except relative humidity(RH).Meanwhile,the secondary conversion ratio shows a remarkable increasing trend,indicating that there was a strong secondary transformation.From the perspective of chemical mechanisms,RH is positively correlated with sulfur oxidation ratios(SOR),nitrogen oxidation ratios(NOR),and ammonia conversion ratios,representing that the increase of humidity could promote the generation of SNA.Notably,SOR and NOR were also positively related to the ammonia.On the one hand,the low wind speed and BLH led to the accumulation of pollutants.On the other hand,the increases of RH and ammonia promoted more formations of SNA and PM_(2.5).The results advance our identification of the contributors to the haze episodes and assist to establish more efficient emission controls in Xianyang,in addition to other cities with similar emission and geographical characteristics.
基金supported by the National Science Foundation of China (No.40976063)International Cooperative Projects of MOST (No.2010DFA91350)
文摘A WRF-Chem model including a comprehensive gas-phase nitrogen chemistry module was used to simulate a severe dust event appearing in the eastern China on 19-25 March, 2002. The modeling result well reproduced PM10 concentrations in various distances from the dust sources and the transport pathway of the dust strom. The results showed that both the concentrations and the dry deposition fluxes of PM10 increased over the China seas during the dust event following the passage of a cold front system. The maximum fluxes of PM10 in the Yellow Sea and the East China Sea during the dust event were 5.5 and 8.4 times of those before the event, respectively. However, the temporal variations of the dry deposition fluxes of particulate inorganic nitrogen differed over the Yellow Sea from those over the East China Sea. Nitrate and ammonium in the whole northern China rapidly decreased because of the intrusion of dust-loaded air on 19 March. The dust plume arrived in the Yellow Sea on 20 March, decreasing the particulate inorganic nitrogen in mass concentration accordingly. The minimum dry deposition fluxes of nitrate and ammonium in the Yellow Sea were about 3/5 and 1/6 of those before the dust arrival, respectively. In contrast, when the dust plume crossed over the Yangtze Delta area, it became abundant in nitrate and ammonium and increased the concentrations and dry deposition fluxes of particulate inorganic nitrogen over the East China Sea, where the maximum dry deposition fluxes of nitrate and ammonium increased approximately by 4.1 and 2.6 times of those prior to the dust arrival.
基金Project supported by the National Natural Science Foundation of China (No. 40375038)the National Basic Research Program of China (No. 2002CB410802, 2002CB410801).
文摘A modified two-dimensional Eulerian air quality model was used to simulate both the gaseous and particulate pollutant concentrations during October 21-24, 2004 in the Pearl River Delta (PRD) region, China. The most significant improvement to the model is the added capability to predict the secondary organic aerosols (SOA) concentrations because of the inclusion of the SOA formation chemistry. The meteorological input data were prepared using the CALMET meteorological model. The concentrations of aerosol-bound species such as NO3^-, NH4^+, SO4^2-, and SOA were calculated in the fine particle size range (〈2.5 μm). The results of the two-dimensional model were compared to the measurements at the ground level during the PRD Intensive Monitoring Campaign (IMC). Overall, there were good agreements between the measured and modeled concentrations of inorganic aerosol components and O3. Both the measured and the modeled results indicated that the maximum hourly O3 concentrations exceeded the China National Air Quality Standard. The predicted 24-h average SOA concentrations were in reasonable agreement with those predicted by the method of minimum OC/EC ratio.
基金supported by the National Natural Science Foundation of China (Nos. 41475113, 41175018)the CAS Strategic Priority Research Program (No. XDB05010500)
文摘A field experiment from 18 August to 8 September 2006 in Beijing, China, was carried out. A hazy day was defined as visibility 〈 10 km and RH(relative humidity) 〈 90%. Four haze episodes, which accounted for ~ 60% of the time during the whole campaign, were characterized by increases of SNA(sulfate, nitrate, and ammonium) and SOA(secondary organic aerosol) concentrations. The average values with standard deviation of SO2-+4, NO-3, NH4 and SOA were 49.8(± 31.6), 31.4(±22.3), 25.8(±16.6) and 8.9(±4.1) μg/m3, respectively, during the haze episodes, which were 4.3, 3.4, 4.1, and 1.7 times those in the non-haze days. The SO2-4,NO-3, NH+4, and SOA accounted for 15.8%, 8.8%, 7.3%, and 6.0% of the total mass concentration of PM10 during the non-haze days. The respective contributions of SNA species to PM10 rose to about27.2%, 15.9%, and 13.9% during the haze days, while the contributions of SOA maintained the same level with a slight decrease to about 4.9%. The observed mass concentrations of SNA and SOA increased with the increase of PM10 mass concentration, however, the rate of increase of SNA was much faster than that of the SOA. The SOR(sulfur oxidation ratio) and NOR(nitrogen oxidation ratio) increased from non-haze days to hazy days, and increased with the increase of RH. High concentrations of aerosols and water vapor favored the conversion of SO2 to SO2-4and NO2 to NO-3, which accelerated the accumulation of the aerosols and resulted in the formation of haze in Beijing.
文摘Haze episodes have become a major concern in Malaysia over the past few decades and have an increasingly important impact on the country each and every year. During haze episodes from biomass burning in Southeast Asia, particularly from Sumatra, Indonesia, particulate matter PM2.5 is found to be one of the dangerous sources of airborne pollution and is known to seriously affect human health. This study determines the composition of carbohydrates (as levoglucosan), surfactants, major elements, and anions in PM2.5 during a 2013 haze episode. PM2.5 samples were collected from Universiti Kebangsaan Malaysia, Bangi, using a high volume sampler during a seven-day monitoring campaign during the peak of that year's haze episode. PM2.5 concentrations ranged between 14.52 and 160.93 μg/m3, exceeding the 2005 WHO air quality guidelines for PM2.5 (25 μg/m3 for 24-h mean). The patterns for levoglucosan, surfactants, major elements, and anionic compositions were proportional to the PM2.5 concentrations. Changes in PM2.5 observed on days 3 and 4 were influenced by a combination of meteorological factors, which substantiate the theory that such factors play a pivotal role in haze episodes.