To better understand the characteristics and transformation mechanisms of secondary inorganic aerosols,hourly mass concentrations of water-soluble inorganic ions(WSIIs)in PM_(2.5)and their gaseous precursors were meas...To better understand the characteristics and transformation mechanisms of secondary inorganic aerosols,hourly mass concentrations of water-soluble inorganic ions(WSIIs)in PM_(2.5)and their gaseous precursors were measured online from 2016 to 2018 at an urban site in Beijing.Seasonal and diurnal variations in water-soluble ions and gaseous precursors were discussed and their gas-particle conversion and partitioning were also examined,some related parameters were characterized.The(TNH_(3))Rich was also defined to describe the variations of the excess NH_(3)in different seasons.In addition,a sensitivity test was carried out by using ISORROPIA II to outline the driving factors of gas-particle partitioning.In Beijing,the relative contribution of nitrate to PM_(2.5)has increased markedly in recent years,especially under polluted conditions.In the four seasons,only a small portion of NO_(2)in the atmosphere was converted into total nitrate(TNO_(3)),and more than 80%of TNO_(3)occurred in the form of nitrate due to the abundant ammonia.The concentration of total ammonia(TNH_(3))was much higher than that required to neutralize acid gases,and most of the TNH_(3)occurred as gaseous NH_(3).The nitrous acid(HONO)concentration was highly correlated with NH_(3)concentration and had increased significantly in Beijing compared with previous studies.The total chloride(TCl)was the highest in winter,andε(Cl^(-))was more sensitive to variations in the ambient temperature(T)and relative humidity(RH)thanε(NO_(3)^(-)).展开更多
Air pollution in China is complex,and the formation mechanism of chemical components in particulate matter is still unclear.This study selected three consecutive heavy haze pollution episodes(HPEs)during winter in Bei...Air pollution in China is complex,and the formation mechanism of chemical components in particulate matter is still unclear.This study selected three consecutive heavy haze pollution episodes(HPEs)during winter in Beijing for continuous field observation,including an episode with heavy air pollution under red alert.Clean days during the observation period were selected for comparison.The HPE characteristics of Beijing in winter were:under the influence of adverse meteorological conditions such as high relative humidity,temperature inversion and low wind speed;and strengthening of secondary transformation reactions,which further intensified the accumulation of secondary aerosols and other pollutants,promoting the explosive growth of PM_(2.5).PM_(2.5)/CO values,as indicators of the contribution of secondary transformation in PM_(2.5),were approximately 2 times higher in the HPEs than the average PM_(2.5)/CO during the clean period.The secondary inorganic aerosols(sulfate nitrate and ammonium salt)were significantly enhanced during the HPEs,and the conversion coefficients were remarkably improved.In addition,it is interesting to observe that the production of sulfate tended to exceed that of nitrate in the late stage of all three HPEs.The existence of aqueous phase reactions led to the explosive growth sulfur oxidation ratio(SOR)and rapid generation of sulfate under high relative humidity(RH>70%).展开更多
To understand the size-resolved aerosol ionic composition and the factors influencing secondary aerosol formation in the upper boundary layer in South Central China, size-segregated aerosol samples were collected usin...To understand the size-resolved aerosol ionic composition and the factors influencing secondary aerosol formation in the upper boundary layer in South Central China, size-segregated aerosol samples were collected using a micro-orifice uniform deposit irnpactor （MOUDI） in spring 2009 at the summit of Mount Heng （1269 m asl）, followed by subsequent laboratory analyses of 13 inorganic and organic water-soluble ions. During non- dust-storm periods, the average PM1.8 concentration was 41.8 μg·m^-3, contributing to 55% of the PM10. Sulfates, nitrates, and ammonium, the dominant ions in the fine particles, amounted to 46.8% of the PM1.8. Compared with Mount Tai in the North China Plain, the concentrations of both fine and coarse particles and the ions contained therein were substantially lower. When the air masses from Southeast Asia prevailed, intensive biomass burning there led to elevated concentrations of sulfates, nitrates, ammonium, potassium, and chloride in the fine particles at Mount Heng. The air masses originating from the north Gobi brought heavy dust storms that resulted in the remarkable production of sulfates, ammonium, methane sulfonic acid, and oxalates in the coarse particles. Generally, the sulfates were primarily produced in the form of （NH4）2SO4 in the droplet mode via heterogeneous aqueous reactions. Only approximately one-third of the nitrates were distributed in the fine mode, and high humidity facilitated the secondary formation of fine nitrates. The heterogeneous formation of coarse nitrates and ammonium on dry alkaline dust surfaces was found to be less efficient than that on the coarse particles during non-dust-storm periods.展开更多
基金supported by the National Natural Science Foundation of China(No.42005079,41675131)the Beijing Natural Science Foundation(No.8131003)the Beijing Talents Fund(No.2014000021223ZK49)。
文摘To better understand the characteristics and transformation mechanisms of secondary inorganic aerosols,hourly mass concentrations of water-soluble inorganic ions(WSIIs)in PM_(2.5)and their gaseous precursors were measured online from 2016 to 2018 at an urban site in Beijing.Seasonal and diurnal variations in water-soluble ions and gaseous precursors were discussed and their gas-particle conversion and partitioning were also examined,some related parameters were characterized.The(TNH_(3))Rich was also defined to describe the variations of the excess NH_(3)in different seasons.In addition,a sensitivity test was carried out by using ISORROPIA II to outline the driving factors of gas-particle partitioning.In Beijing,the relative contribution of nitrate to PM_(2.5)has increased markedly in recent years,especially under polluted conditions.In the four seasons,only a small portion of NO_(2)in the atmosphere was converted into total nitrate(TNO_(3)),and more than 80%of TNO_(3)occurred in the form of nitrate due to the abundant ammonia.The concentration of total ammonia(TNH_(3))was much higher than that required to neutralize acid gases,and most of the TNH_(3)occurred as gaseous NH_(3).The nitrous acid(HONO)concentration was highly correlated with NH_(3)concentration and had increased significantly in Beijing compared with previous studies.The total chloride(TCl)was the highest in winter,andε(Cl^(-))was more sensitive to variations in the ambient temperature(T)and relative humidity(RH)thanε(NO_(3)^(-)).
基金supported by the Natural Science Foundation of Beijing Municipal(No.8202052)the National Natural Science Foundation of China(Nos.21777191,42075082 and 41875147)+2 种基金S&T Development Fund of Chinese Academy of Meteorological Sciences(No.2020KJ001)Basic Research Fund of Chinese Academy of Meteorological Sciences(No.2020Z002)supported by the Innovation Team for Haze-fog Observation and Forecasts of Ministry of Science and Technology of the People’s Republic of China and China Meteorological Administration
文摘Air pollution in China is complex,and the formation mechanism of chemical components in particulate matter is still unclear.This study selected three consecutive heavy haze pollution episodes(HPEs)during winter in Beijing for continuous field observation,including an episode with heavy air pollution under red alert.Clean days during the observation period were selected for comparison.The HPE characteristics of Beijing in winter were:under the influence of adverse meteorological conditions such as high relative humidity,temperature inversion and low wind speed;and strengthening of secondary transformation reactions,which further intensified the accumulation of secondary aerosols and other pollutants,promoting the explosive growth of PM_(2.5).PM_(2.5)/CO values,as indicators of the contribution of secondary transformation in PM_(2.5),were approximately 2 times higher in the HPEs than the average PM_(2.5)/CO during the clean period.The secondary inorganic aerosols(sulfate nitrate and ammonium salt)were significantly enhanced during the HPEs,and the conversion coefficients were remarkably improved.In addition,it is interesting to observe that the production of sulfate tended to exceed that of nitrate in the late stage of all three HPEs.The existence of aqueous phase reactions led to the explosive growth sulfur oxidation ratio(SOR)and rapid generation of sulfate under high relative humidity(RH>70%).
文摘To understand the size-resolved aerosol ionic composition and the factors influencing secondary aerosol formation in the upper boundary layer in South Central China, size-segregated aerosol samples were collected using a micro-orifice uniform deposit irnpactor （MOUDI） in spring 2009 at the summit of Mount Heng （1269 m asl）, followed by subsequent laboratory analyses of 13 inorganic and organic water-soluble ions. During non- dust-storm periods, the average PM1.8 concentration was 41.8 μg·m^-3, contributing to 55% of the PM10. Sulfates, nitrates, and ammonium, the dominant ions in the fine particles, amounted to 46.8% of the PM1.8. Compared with Mount Tai in the North China Plain, the concentrations of both fine and coarse particles and the ions contained therein were substantially lower. When the air masses from Southeast Asia prevailed, intensive biomass burning there led to elevated concentrations of sulfates, nitrates, ammonium, potassium, and chloride in the fine particles at Mount Heng. The air masses originating from the north Gobi brought heavy dust storms that resulted in the remarkable production of sulfates, ammonium, methane sulfonic acid, and oxalates in the coarse particles. Generally, the sulfates were primarily produced in the form of （NH4）2SO4 in the droplet mode via heterogeneous aqueous reactions. Only approximately one-third of the nitrates were distributed in the fine mode, and high humidity facilitated the secondary formation of fine nitrates. The heterogeneous formation of coarse nitrates and ammonium on dry alkaline dust surfaces was found to be less efficient than that on the coarse particles during non-dust-storm periods.
