Sequential samples of single precipitation event were collected by the use of specially de-signed semi-automatic sequential precipitation collector in the spring of 1988 in Guilin City. ThePH value and soluble chemica...Sequential samples of single precipitation event were collected by the use of specially de-signed semi-automatic sequential precipitation collector in the spring of 1988 in Guilin City. ThePH value and soluble chemical species such as SO, NO, NH, Ca￣(2+), Mg￣(2+), Na￣+, K`+, F￣- andCl￣- were analyzed. An apparent decrease in the concentration of all ions except H￣+ and NO wasobserved at the initial portion of the events. The relative acidity increased as the event progress.The concentration of H￣+ was the result of comprehensive actions of all ions. The average scavengingratio of events was calculated and it is found that SO was the major contributor for acid rain inGuilin and Ca￣(2+) was the important neutralizer.展开更多
Below-cloud aerosol scavenging process by precipitation is important for cleaning the polluted aerosols in the atmosphere, and is also a main process for acid rain formation. However, the related physical mechanism ha...Below-cloud aerosol scavenging process by precipitation is important for cleaning the polluted aerosols in the atmosphere, and is also a main process for acid rain formation. However, the related physical mechanism has not been well documented and clarified yet. In this paper, we investigated the below-cloud PM_(2.5)(particulate matter with aerodynamic diameter being 2.5 μm or less) scavenging by different-intensity rains under polluted conditions characterized by high PM_(2.5) concentrations, based on in-situ measurements from March 2014 to July 2016 in Beijing city. It was found that relatively more intense rainfall events were more efficient in removing the polluted aerosols in the atmosphere. The mean PM_(2.5) scavenging ratio and its standard deviation(SD) were 5.1% ± 25.7%, 38.5% ± 29.0%,and 50.6% ± 21.2% for light, moderate, and heavy rain events, respectively. We further found that the key impact factors on below-cloud PM_(2.5) scavenging ratio for light rain events were rain duration and wind speed rather than raindrop size distribution. However, the impacts of rain duration and wind speed on scavenging ratio were not important for moderate and heavy rain events. To our knowledge, this is the first statistical result about the effects of rain intensity, rain duration, and raindrop size distribution on below-cloud scavenging in China.展开更多
The below-cloud aerosol scavenging process by precipitation is one of the most important mechanisms to remove aerosols from the atmosphere.Due to its complexity and dependence on both aerosol and raindrop sizes,wet sc...The below-cloud aerosol scavenging process by precipitation is one of the most important mechanisms to remove aerosols from the atmosphere.Due to its complexity and dependence on both aerosol and raindrop sizes,wet scavenging process has been poorly treated,especially during the removal of fine particles.This makes the numerical simulation of below-cloud scavenging in large-scale aerosolmodels unrealistic.To consider the slip effects of submicron particles,a simplified expression for the diffusion scavenging was developed by approximating the Cunningham slip correction factor.The derived analytic solution was parameterized as a simple power function of rain intensity under the assumption of the lognormal size distribution of particles.The resultant approximated expression was compared to the observed data and the results of previous studies including a 3D atmospheric chemical transport model simulation.Compared with the default GEOS-Chem coefficient of 0.00106R0.61 and the observation-based coefficient of 0.0144R0.9268,the coefficient of a and b in∧m=aRb spread in the range of 0.0002-0.1959 for a and 0.3261-0.525 for b over a size distribution of GSD of 1.3–2.5 and a geometric mean diameter of 0.01-2.5μm.Overall,this study showed that the scavenging coefficient varies widely by orders of magnitude according to the size distribution of particles and rain intensity.This study also demonstrated that the obtained simplified expression could consider the theoretical approach of aerosol polydispersity.Our proposed analytic approach showed that results can be effectively applied for reduced computational burden in atmospheric modeling.展开更多
-The concentrations of gas phase SO2, O3 and chemical composition of sequential rainwater samples were measured on 6/11/88 to 6/28/88 at some sites of Guiyang area. S (IV) was present in great excess of H2O2 in rainwa...-The concentrations of gas phase SO2, O3 and chemical composition of sequential rainwater samples were measured on 6/11/88 to 6/28/88 at some sites of Guiyang area. S (IV) was present in great excess of H2O2 in rainwater samples collected at residential sites of the city corresponding to high level of gas phase SO2. Considerable H2O2 in rainwater samples was observed in background air at suburbs. The evidence that clean rainwater samples were collected at 20km away from the city in 6/18/88 precipitation event revealed that the major process of acidification of the rain in the high polluted areas was below-cloud scavenging of trace gases. From a simulation calculation it was found that the rate of oxidation of S(IV) by O3 and by Mn2+, Fe3+ catalytic in high pH rainwater is significant, but for low pH the major SO42- is produced by the reaction of S (IV) with H2O2.展开更多
Consideration of stable isotopes in precipitation is valuable for investigating hydrological processes.Therefore,correcting the measured isotopic composition of precipitation under below-cloud evaporation is necessary...Consideration of stable isotopes in precipitation is valuable for investigating hydrological processes.Therefore,correcting the measured isotopic composition of precipitation under below-cloud evaporation is necessary.An accurate description of the underlying processes affecting stable isotopic composition of precipitation could help improve our understanding of the water cycle.The transitivity between monsoonal and arid climates was reflected by the evaporation rate of falling raindrops in precipitation in the Qilian Mountains,a typical transition zone between Tibetan Plateau and arid region of China.Considering 1310 precipitation event-scale samples,based on stable isotope analysis method,the mean below-cloud evaporation rate(f)in the study area was measured as 12.00%during the summer half-year(May-October).The evaporation rate on the northern slopes(12.70%)of the Qilian Mountains in China was significantly higher than that on the southern slopes(9.98%).The transition between monsoonal and arid climates was reflected in the evaporation rate of falling raindrops during precipitation in the Qilian Mountains of China.Below-cloud evaporation contributed to a noticeable enrichment of stable isotopes in the precipitation in the study area.The monthly precipitationδ^(18)O enrichment rate in the Qilian Mountains of China from May to October was 29.18%,23.35%,25.60%,22.99%,31.64%,and 14.72%,respectively.For every 1.00%increase in the evaporation rate of raindrops in Qilian Mountains of China,the changes in the concentration of oxygen isotopes from the bottom of the clouds to the ground increased by 0.92‰;however,with an evaporation rate of<5.00%,for every 1.00%increase in the evaporation rate of raindrops the changes in the concentration of oxygen isotopes from the bottom of the clouds to the ground increased by 1.00‰could also be observed.Furthermore,altitude was an important factor affecting below-cloud evaporation in the study area.展开更多
文摘Sequential samples of single precipitation event were collected by the use of specially de-signed semi-automatic sequential precipitation collector in the spring of 1988 in Guilin City. ThePH value and soluble chemical species such as SO, NO, NH, Ca￣(2+), Mg￣(2+), Na￣+, K`+, F￣- andCl￣- were analyzed. An apparent decrease in the concentration of all ions except H￣+ and NO wasobserved at the initial portion of the events. The relative acidity increased as the event progress.The concentration of H￣+ was the result of comprehensive actions of all ions. The average scavengingratio of events was calculated and it is found that SO was the major contributor for acid rain inGuilin and Ca￣(2+) was the important neutralizer.
基金Supported by the China Meteorological Administration Special Public Welfare Research Fund(GYHY200806001 and GYHY201406001)National Natural Science Foundation of China(41605111)Research Funds of the Chinese Academy of Meteorological Sciences(2016Z004)
文摘Below-cloud aerosol scavenging process by precipitation is important for cleaning the polluted aerosols in the atmosphere, and is also a main process for acid rain formation. However, the related physical mechanism has not been well documented and clarified yet. In this paper, we investigated the below-cloud PM_(2.5)(particulate matter with aerodynamic diameter being 2.5 μm or less) scavenging by different-intensity rains under polluted conditions characterized by high PM_(2.5) concentrations, based on in-situ measurements from March 2014 to July 2016 in Beijing city. It was found that relatively more intense rainfall events were more efficient in removing the polluted aerosols in the atmosphere. The mean PM_(2.5) scavenging ratio and its standard deviation(SD) were 5.1% ± 25.7%, 38.5% ± 29.0%,and 50.6% ± 21.2% for light, moderate, and heavy rain events, respectively. We further found that the key impact factors on below-cloud PM_(2.5) scavenging ratio for light rain events were rain duration and wind speed rather than raindrop size distribution. However, the impacts of rain duration and wind speed on scavenging ratio were not important for moderate and heavy rain events. To our knowledge, this is the first statistical result about the effects of rain intensity, rain duration, and raindrop size distribution on below-cloud scavenging in China.
基金supported by the FRIEND(Fine Particle Research Initiative in East Asia Considering National Differences)Project through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(No.2020M3G1A1114617)the Technology Development Program to Solve Climate Changes through the National Research Foundation of Korea(NRF)funded by the Ministry of Science,ICT(No.2019M1A2A2103953)+1 种基金the National Research Foundation of Korea Grant from the Korean Government(MSIT)(Nos.NRF2021M1A5A1065672/PN22011,NRF2021R1F1A1046878,and NRF2020R1A2C1003215)This research was also supported by Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(No.2020R1A6A1A03044834).
文摘The below-cloud aerosol scavenging process by precipitation is one of the most important mechanisms to remove aerosols from the atmosphere.Due to its complexity and dependence on both aerosol and raindrop sizes,wet scavenging process has been poorly treated,especially during the removal of fine particles.This makes the numerical simulation of below-cloud scavenging in large-scale aerosolmodels unrealistic.To consider the slip effects of submicron particles,a simplified expression for the diffusion scavenging was developed by approximating the Cunningham slip correction factor.The derived analytic solution was parameterized as a simple power function of rain intensity under the assumption of the lognormal size distribution of particles.The resultant approximated expression was compared to the observed data and the results of previous studies including a 3D atmospheric chemical transport model simulation.Compared with the default GEOS-Chem coefficient of 0.00106R0.61 and the observation-based coefficient of 0.0144R0.9268,the coefficient of a and b in∧m=aRb spread in the range of 0.0002-0.1959 for a and 0.3261-0.525 for b over a size distribution of GSD of 1.3–2.5 and a geometric mean diameter of 0.01-2.5μm.Overall,this study showed that the scavenging coefficient varies widely by orders of magnitude according to the size distribution of particles and rain intensity.This study also demonstrated that the obtained simplified expression could consider the theoretical approach of aerosol polydispersity.Our proposed analytic approach showed that results can be effectively applied for reduced computational burden in atmospheric modeling.
文摘-The concentrations of gas phase SO2, O3 and chemical composition of sequential rainwater samples were measured on 6/11/88 to 6/28/88 at some sites of Guiyang area. S (IV) was present in great excess of H2O2 in rainwater samples collected at residential sites of the city corresponding to high level of gas phase SO2. Considerable H2O2 in rainwater samples was observed in background air at suburbs. The evidence that clean rainwater samples were collected at 20km away from the city in 6/18/88 precipitation event revealed that the major process of acidification of the rain in the high polluted areas was below-cloud scavenging of trace gases. From a simulation calculation it was found that the rate of oxidation of S(IV) by O3 and by Mn2+, Fe3+ catalytic in high pH rainwater is significant, but for low pH the major SO42- is produced by the reaction of S (IV) with H2O2.
基金Under the auspices of the Joint Funds of the National Natural Science Foundation of China(No.U22A20592)the National Key Research and Development Program of China(No.2020YFA0607702)+2 种基金the Second Tibetan Plateau Scientific Expedition and Research Program(No.2019QZKK0405)Chinese Academy of Sciences Young Crossover Team Project(No.JCTD-2022-18)Excellent doctoral program in Gansu Province(No.22JR5RA052)。
文摘Consideration of stable isotopes in precipitation is valuable for investigating hydrological processes.Therefore,correcting the measured isotopic composition of precipitation under below-cloud evaporation is necessary.An accurate description of the underlying processes affecting stable isotopic composition of precipitation could help improve our understanding of the water cycle.The transitivity between monsoonal and arid climates was reflected by the evaporation rate of falling raindrops in precipitation in the Qilian Mountains,a typical transition zone between Tibetan Plateau and arid region of China.Considering 1310 precipitation event-scale samples,based on stable isotope analysis method,the mean below-cloud evaporation rate(f)in the study area was measured as 12.00%during the summer half-year(May-October).The evaporation rate on the northern slopes(12.70%)of the Qilian Mountains in China was significantly higher than that on the southern slopes(9.98%).The transition between monsoonal and arid climates was reflected in the evaporation rate of falling raindrops during precipitation in the Qilian Mountains of China.Below-cloud evaporation contributed to a noticeable enrichment of stable isotopes in the precipitation in the study area.The monthly precipitationδ^(18)O enrichment rate in the Qilian Mountains of China from May to October was 29.18%,23.35%,25.60%,22.99%,31.64%,and 14.72%,respectively.For every 1.00%increase in the evaporation rate of raindrops in Qilian Mountains of China,the changes in the concentration of oxygen isotopes from the bottom of the clouds to the ground increased by 0.92‰;however,with an evaporation rate of<5.00%,for every 1.00%increase in the evaporation rate of raindrops the changes in the concentration of oxygen isotopes from the bottom of the clouds to the ground increased by 1.00‰could also be observed.Furthermore,altitude was an important factor affecting below-cloud evaporation in the study area.
