A global two-dimensional zonally averaged chemistry model is developed to study the chemi-cal composition of atmosphere. The region of the model is from 90°S to 90°N and from the ground to the altitude of 20...A global two-dimensional zonally averaged chemistry model is developed to study the chemi-cal composition of atmosphere. The region of the model is from 90°S to 90°N and from the ground to the altitude of 20 km with a resolution of 5° x 1 km. The wind field is residual circulation calcu-lated from diabatic rate. 34 species and 104 chemical and photochemical reactions are considered in the model. The sources of CH4, CO and NOx, which are divided into seasonal sources and non-seasonal sources, are parameterized as a function of latitude and time. The chemical composi-tion of atmosphere was simulated with emission level of CH4, CO and NOx in 1990. The results are compared with observations and other model results, showing that the model is successful to simu-late the atmospheric chemical composition and distribution of CH4. Key words Global two-dimensional chemistry model - Atmospheric composition - Emission This work was supported by the State Key Program for basic research “ Climate Dynamics and Cli-mate Prediction Theory” (Pandeng-yu-21).The authors would like to express their thanks to the National Oceanic and Atmospheric Administration (NOAA), Climate Monitoring and Diagnostics Laboratory (CMDL), Carbon Cycle Group for providing the observational data of CO and CH4.展开更多
This analysis of the multi-model aerosol optical depth (AOD) in eastern China using the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) datasets shows that the global models underestimate the ...This analysis of the multi-model aerosol optical depth (AOD) in eastern China using the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) datasets shows that the global models underestimate the AOD by 33% and 44% in southern and northern China, respectively, and decrease the relative humidity (RH) of the air in the surface layer to 71%–80%, which is less than the RH of 77%–92% in reanalysis meteorological datasets. This indicates that the low biases in the RH partially account for the errors in the AOD. The AOD is recalculated based on the model aerosol concentrations and the reanalysis humidity data. Improving the mean value of the RH increases the multi-model annual mean AOD by 45% in southern China and by 33% in June–August in northern China. This method of improving the AOD is successful in most of the ACCMIP models, but it is unlikely to be successful in GISS-E2-R, in which the plot of its AOD efficiency against RH strongly deviates from the rest of the models. The effect of the improvement in the modeled RH on the AOD depends on the concentration of aerosols. The shape error in the frequency distribution of the RH is likely to be more important than the error in the mean value of the RH, but this requires further research.展开更多
To realistically simulate the impacts of marine isoprene and primary organic aerosols (POA) on atmospheric chemistry, a unified model framework with online emissions, comprehensive treatment of gas-phase chemistry, an...To realistically simulate the impacts of marine isoprene and primary organic aerosols (POA) on atmospheric chemistry, a unified model framework with online emissions, comprehensive treatment of gas-phase chemistry, and advanced aerosol microphysics is required. In this work, the global-through-urban WRF/Chem model (GU-WRF/Chem) implemented with the online emissions of marine isoprene and size-resolved marine POA is applied to examine such impacts. The net effect of these emissions was increased surface concentrations of isoprene and organic aerosols and decreased surfaced concentrations of hydroxyl radical and ozone over most marine regions. With the inclusion of these emissions, GU-WRF/Chem better predicted the surface concentrations of isoprene and organic aerosols and the aerosol number size distribution when compared to measurements in clean marine conditions.展开更多
As one of the regions with intensive agriculture and rapid economic development in China,North China also has a high nitrogen(N)deposition.This study characterized the spatial pattern of N deposition in North China,co...As one of the regions with intensive agriculture and rapid economic development in China,North China also has a high nitrogen(N)deposition.This study characterized the spatial pattern of N deposition in North China,combining the tropospheric columns from satellite measurements and the simulated profiles from an atmospheric chemistry transport model.The total N deposition fluxes ranged from 16.3 to 106.5 kg N ha−1 yr−1,with an average of 54.5±17.2 kg N ha−1 yr−1.The high values were concentrated in urban and farmland areas,while low values were found in forests and grasslands with less human activities.Of the total N deposition,36%was deposited via precipitation,12%was deposited through dry particulate deposition,and the remaining 52%was comprised of dry gaseous deposition.For the seasonal variation of dry deposition,gaseous HNO3 and particulate NO3−were higher in winter and autumn,but lower in spring and summer.In contrast,gaseous NH3 and particulate NH4+were higher in spring and summer,but lower in winter and autumn.This is possibly caused by the seasonal differences in emission intensity between NOx and NH3 emission sources.The gaseous NO2 deposition did not show strong seasonal variation.The wet deposition was mainly affected by precipitation,with high values in summer and low values in winter.This research provides an objective spatial perspective and insight into the total N deposition in North China.展开更多
The atmospheric chemical mechanism is an essential component of airshed models used for investigating the chemical behaviors and impacts of species.Since the first tropospheric chemical mechanism was proposed in the 1...The atmospheric chemical mechanism is an essential component of airshed models used for investigating the chemical behaviors and impacts of species.Since the first tropospheric chemical mechanism was proposed in the 1960s,various mechanisms including Master Chemical Mechanism(MCM),Carbon Bond Mechanism(CBM),Statewide Air Pollution Research Center(SAPRC)and Regional Atmospheric Chemistry Mechanism(RACM)have been developed for different research purposes.This work summarizes the development and applications of these mechanisms,introduces their compositions and lumping methods,and compares the ways the mechanisms treat radicals with box model simulations.CBM can reproduce urban pollution events with relatively low cost compared to SAPRC and RACM,whereas the chemical behaviors of radicals and the photochemical production of ozone are described in detail in RACM.The photolysis rates of some oxygenated compounds are low in SAPRC07,which may result in underestimation of radical levels.As an explicit chemical mechanism,MCM describes the chemical processes of primary pollutants and their oxidation products in detail.MCM can be used to investigate certain chemical processes;however,due to its large size,it is rarely used in regional model simulations.A box model case study showed that the chemical behavior of OH and HO_(2)radicals and the production of ozone were well described by all mechanisms.CBM and SAPRC underestimated the radical levels for different chemical treatments,leading to low ozone production values in both cases.MCM and RACM are widely used in box model studies,while CBM and SAPRC are often selected in regional simulations.展开更多
气候变化引起的地面气溶胶浓度变化与区域空气质量密切相关。本文利用"国际大气化学—气候模式比较计划"(Atmospheric Chemistry and Climate Model Intercomparison Project,ACCMIP)中4个模式的试验数据分析了RCP8.5情景下20...气候变化引起的地面气溶胶浓度变化与区域空气质量密切相关。本文利用"国际大气化学—气候模式比较计划"(Atmospheric Chemistry and Climate Model Intercomparison Project,ACCMIP)中4个模式的试验数据分析了RCP8.5情景下2000~2100年气候变化对中国气溶胶浓度的影响。结果显示,在人为气溶胶排放固定在2000年、仅考虑气候变化的影响时,2000~2100年气候变化导致中国北部地区(31°N^45°N,105°E^122°E)硫酸盐、有机碳和黑碳气溶胶分别增加28%、21%和9%,硝酸盐气溶胶在中国东部地区减少30%。气候变化对细颗粒物(PM_(2.5))浓度的影响有显著的季节变化特征,冬季PM_(2.5)浓度在中国东部减少15%,这主要是由硝酸盐气溶胶在冬季的显著减少造成的;夏季PM_(2.5)浓度在中国北部地区增加16%,而长江以南地区减少为9%,这可能与模式模拟的未来东亚夏季风环流的增强有关。展开更多
初步建立了以二氧化硫、硫酸盐、黑碳、沙尘气溶胶等作为主要研究对象的全球环境大气输送模式（Global Environmental Atmospheric Transport Model,GEATM）,其水平分辨率为1°×1°,垂直方向分为20层,采用地形追随坐标系,...初步建立了以二氧化硫、硫酸盐、黑碳、沙尘气溶胶等作为主要研究对象的全球环境大气输送模式（Global Environmental Atmospheric Transport Model,GEATM）,其水平分辨率为1°×1°,垂直方向分为20层,采用地形追随坐标系,考虑了上述大气化学成分的地面源排放、平流与扩散、化学转化以及干沉降、湿清除等过程.利用NCEP/NCAR再分析资料作为驱动气象场,对2004年进行长期模拟,分析了二氧化硫、硫酸盐、黑碳、沙尘气溶胶的浓度分布和输送态势.与观测的比较表明,模式对于大气化学成分分布状况具有较强的模拟能力,在欧洲的Jarczew和Leba观测站,二氧化硫日平均浓度的相关系数分别达到了0.69和0.66;在中国,有47个站点的二氧化硫日平均浓度相关系数高于0.50,其中北京、天津、上海等28个站点的浓度相关系数达到了0.60以上.同时,模拟的沙尘气溶胶总体柱浓度分布状况与卫星观测输出的气溶胶光学厚度具有很好的一致性,体现了气溶胶粒子的输送态势和分布特征.模拟结果显示二氧化硫、硫酸盐、黑碳的浓度高值区主要位于污染排放较大的欧洲、东亚和北美地区,二氧化硫地面最大年均浓度值为1500×10^-12,硫酸盐为500×10^-12,黑碳气溶胶为1000ng/m^3.沙尘浓度与下垫面土壤类型以及地面气象条件关系密切,全球沙尘浓度主要分布在撒哈拉沙漠、阿拉伯半岛、中亚地区、澳大利亚西部以及拉丁美洲南部地区,并且呈现了较为显著的季节变化特征,撒哈拉沙漠输送最强时期是在6～8月,影响范围覆盖了整个赤道大西洋,最西端伸展到了北美的加勒比海地区;阿拉伯半岛沙尘输送最强时期是3～8月,影响范围包括阿拉伯海和孟加拉湾地区;亚洲在3～5月有非常强烈的沙尘东传过程,浓度输送带一直贯穿了整个北太平洋地区.展开更多
目前气候模式对沙尘气溶胶直接辐射强迫模拟仍有很大不确定性,多模式对比有助于定量评估不确定范围。国际大气化学—气候模式比较计划(Atmospheric Chemistry and Climate Model Intercomparison Project,ACCMIP)旨在评估当前模式对短...目前气候模式对沙尘气溶胶直接辐射强迫模拟仍有很大不确定性,多模式对比有助于定量评估不确定范围。国际大气化学—气候模式比较计划(Atmospheric Chemistry and Climate Model Intercomparison Project,ACCMIP)旨在评估当前模式对短寿命大气成分辐射强迫和气候效应的模拟能力。基于7个ACCMIP模式模拟的中国地区沙尘气溶胶浓度,我们评估了中国区域沙尘气溶胶直接辐射强迫和不确定性范围。结果显示,中国区域沙尘气溶胶年排放总量为215±163 Tg a^(-1),区域年均地表浓度为41±27μg m^(-3),柱浓度为9±4 kg m^(-2),光学厚度为0.09±0.05。中国区域年均沙尘气溶胶产生的大气顶短波、长波和总辐射强迫分别为-1.3±0.8 W m^(-2)、0.7±0.4W m^(-2)和-0.5±0.7 W m-2;地表短波、长波和总的辐射强迫值为-1.5±1.0 W m^(-2)、1.8±0.9 W m^(-2)和0.2±0.2 W m^(-2)。沙尘气溶胶长波辐射强迫对沙尘浓度的垂直分布敏感。高层沙尘气溶胶浓度越大,其在大气顶产生更强的正值长波辐射强迫。然而,沙尘气溶胶短波辐射强迫主要受整层沙尘柱浓度控制,对沙尘浓度的垂直分布较不敏感。本文结果可为中国沙尘气溶胶的气候模拟提供参考。展开更多
文摘A global two-dimensional zonally averaged chemistry model is developed to study the chemi-cal composition of atmosphere. The region of the model is from 90°S to 90°N and from the ground to the altitude of 20 km with a resolution of 5° x 1 km. The wind field is residual circulation calcu-lated from diabatic rate. 34 species and 104 chemical and photochemical reactions are considered in the model. The sources of CH4, CO and NOx, which are divided into seasonal sources and non-seasonal sources, are parameterized as a function of latitude and time. The chemical composi-tion of atmosphere was simulated with emission level of CH4, CO and NOx in 1990. The results are compared with observations and other model results, showing that the model is successful to simu-late the atmospheric chemical composition and distribution of CH4. Key words Global two-dimensional chemistry model - Atmospheric composition - Emission This work was supported by the State Key Program for basic research “ Climate Dynamics and Cli-mate Prediction Theory” (Pandeng-yu-21).The authors would like to express their thanks to the National Oceanic and Atmospheric Administration (NOAA), Climate Monitoring and Diagnostics Laboratory (CMDL), Carbon Cycle Group for providing the observational data of CO and CH4.
基金jointly supported by the National Key Research and Development Program of China [grant number2016YFE0201400]the Basic Research Program of the State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry,Institute of Atmospheric Physics,Chinese Academy of Sciences [grant number 7-082999]
文摘This analysis of the multi-model aerosol optical depth (AOD) in eastern China using the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) datasets shows that the global models underestimate the AOD by 33% and 44% in southern and northern China, respectively, and decrease the relative humidity (RH) of the air in the surface layer to 71%–80%, which is less than the RH of 77%–92% in reanalysis meteorological datasets. This indicates that the low biases in the RH partially account for the errors in the AOD. The AOD is recalculated based on the model aerosol concentrations and the reanalysis humidity data. Improving the mean value of the RH increases the multi-model annual mean AOD by 45% in southern China and by 33% in June–August in northern China. This method of improving the AOD is successful in most of the ACCMIP models, but it is unlikely to be successful in GISS-E2-R, in which the plot of its AOD efficiency against RH strongly deviates from the rest of the models. The effect of the improvement in the modeled RH on the AOD depends on the concentration of aerosols. The shape error in the frequency distribution of the RH is likely to be more important than the error in the mean value of the RH, but this requires further research.
文摘To realistically simulate the impacts of marine isoprene and primary organic aerosols (POA) on atmospheric chemistry, a unified model framework with online emissions, comprehensive treatment of gas-phase chemistry, and advanced aerosol microphysics is required. In this work, the global-through-urban WRF/Chem model (GU-WRF/Chem) implemented with the online emissions of marine isoprene and size-resolved marine POA is applied to examine such impacts. The net effect of these emissions was increased surface concentrations of isoprene and organic aerosols and decreased surfaced concentrations of hydroxyl radical and ozone over most marine regions. With the inclusion of these emissions, GU-WRF/Chem better predicted the surface concentrations of isoprene and organic aerosols and the aerosol number size distribution when compared to measurements in clean marine conditions.
基金This study was supported by the National Natural Science Foundation of China[grant numbers 41471343 and 41601457].
文摘As one of the regions with intensive agriculture and rapid economic development in China,North China also has a high nitrogen(N)deposition.This study characterized the spatial pattern of N deposition in North China,combining the tropospheric columns from satellite measurements and the simulated profiles from an atmospheric chemistry transport model.The total N deposition fluxes ranged from 16.3 to 106.5 kg N ha−1 yr−1,with an average of 54.5±17.2 kg N ha−1 yr−1.The high values were concentrated in urban and farmland areas,while low values were found in forests and grasslands with less human activities.Of the total N deposition,36%was deposited via precipitation,12%was deposited through dry particulate deposition,and the remaining 52%was comprised of dry gaseous deposition.For the seasonal variation of dry deposition,gaseous HNO3 and particulate NO3−were higher in winter and autumn,but lower in spring and summer.In contrast,gaseous NH3 and particulate NH4+were higher in spring and summer,but lower in winter and autumn.This is possibly caused by the seasonal differences in emission intensity between NOx and NH3 emission sources.The gaseous NO2 deposition did not show strong seasonal variation.The wet deposition was mainly affected by precipitation,with high values in summer and low values in winter.This research provides an objective spatial perspective and insight into the total N deposition in North China.
基金supported by the National Key Research and Development Program of China(No.2019YFC0214801)。
文摘The atmospheric chemical mechanism is an essential component of airshed models used for investigating the chemical behaviors and impacts of species.Since the first tropospheric chemical mechanism was proposed in the 1960s,various mechanisms including Master Chemical Mechanism(MCM),Carbon Bond Mechanism(CBM),Statewide Air Pollution Research Center(SAPRC)and Regional Atmospheric Chemistry Mechanism(RACM)have been developed for different research purposes.This work summarizes the development and applications of these mechanisms,introduces their compositions and lumping methods,and compares the ways the mechanisms treat radicals with box model simulations.CBM can reproduce urban pollution events with relatively low cost compared to SAPRC and RACM,whereas the chemical behaviors of radicals and the photochemical production of ozone are described in detail in RACM.The photolysis rates of some oxygenated compounds are low in SAPRC07,which may result in underestimation of radical levels.As an explicit chemical mechanism,MCM describes the chemical processes of primary pollutants and their oxidation products in detail.MCM can be used to investigate certain chemical processes;however,due to its large size,it is rarely used in regional model simulations.A box model case study showed that the chemical behavior of OH and HO_(2)radicals and the production of ozone were well described by all mechanisms.CBM and SAPRC underestimated the radical levels for different chemical treatments,leading to low ozone production values in both cases.MCM and RACM are widely used in box model studies,while CBM and SAPRC are often selected in regional simulations.
文摘气候变化引起的地面气溶胶浓度变化与区域空气质量密切相关。本文利用"国际大气化学—气候模式比较计划"(Atmospheric Chemistry and Climate Model Intercomparison Project,ACCMIP)中4个模式的试验数据分析了RCP8.5情景下2000~2100年气候变化对中国气溶胶浓度的影响。结果显示,在人为气溶胶排放固定在2000年、仅考虑气候变化的影响时,2000~2100年气候变化导致中国北部地区(31°N^45°N,105°E^122°E)硫酸盐、有机碳和黑碳气溶胶分别增加28%、21%和9%,硝酸盐气溶胶在中国东部地区减少30%。气候变化对细颗粒物(PM_(2.5))浓度的影响有显著的季节变化特征,冬季PM_(2.5)浓度在中国东部减少15%,这主要是由硝酸盐气溶胶在冬季的显著减少造成的;夏季PM_(2.5)浓度在中国北部地区增加16%,而长江以南地区减少为9%,这可能与模式模拟的未来东亚夏季风环流的增强有关。
文摘初步建立了以二氧化硫、硫酸盐、黑碳、沙尘气溶胶等作为主要研究对象的全球环境大气输送模式（Global Environmental Atmospheric Transport Model,GEATM）,其水平分辨率为1°×1°,垂直方向分为20层,采用地形追随坐标系,考虑了上述大气化学成分的地面源排放、平流与扩散、化学转化以及干沉降、湿清除等过程.利用NCEP/NCAR再分析资料作为驱动气象场,对2004年进行长期模拟,分析了二氧化硫、硫酸盐、黑碳、沙尘气溶胶的浓度分布和输送态势.与观测的比较表明,模式对于大气化学成分分布状况具有较强的模拟能力,在欧洲的Jarczew和Leba观测站,二氧化硫日平均浓度的相关系数分别达到了0.69和0.66;在中国,有47个站点的二氧化硫日平均浓度相关系数高于0.50,其中北京、天津、上海等28个站点的浓度相关系数达到了0.60以上.同时,模拟的沙尘气溶胶总体柱浓度分布状况与卫星观测输出的气溶胶光学厚度具有很好的一致性,体现了气溶胶粒子的输送态势和分布特征.模拟结果显示二氧化硫、硫酸盐、黑碳的浓度高值区主要位于污染排放较大的欧洲、东亚和北美地区,二氧化硫地面最大年均浓度值为1500×10^-12,硫酸盐为500×10^-12,黑碳气溶胶为1000ng/m^3.沙尘浓度与下垫面土壤类型以及地面气象条件关系密切,全球沙尘浓度主要分布在撒哈拉沙漠、阿拉伯半岛、中亚地区、澳大利亚西部以及拉丁美洲南部地区,并且呈现了较为显著的季节变化特征,撒哈拉沙漠输送最强时期是在6～8月,影响范围覆盖了整个赤道大西洋,最西端伸展到了北美的加勒比海地区;阿拉伯半岛沙尘输送最强时期是3～8月,影响范围包括阿拉伯海和孟加拉湾地区;亚洲在3～5月有非常强烈的沙尘东传过程,浓度输送带一直贯穿了整个北太平洋地区.
文摘目前气候模式对沙尘气溶胶直接辐射强迫模拟仍有很大不确定性,多模式对比有助于定量评估不确定范围。国际大气化学—气候模式比较计划(Atmospheric Chemistry and Climate Model Intercomparison Project,ACCMIP)旨在评估当前模式对短寿命大气成分辐射强迫和气候效应的模拟能力。基于7个ACCMIP模式模拟的中国地区沙尘气溶胶浓度,我们评估了中国区域沙尘气溶胶直接辐射强迫和不确定性范围。结果显示,中国区域沙尘气溶胶年排放总量为215±163 Tg a^(-1),区域年均地表浓度为41±27μg m^(-3),柱浓度为9±4 kg m^(-2),光学厚度为0.09±0.05。中国区域年均沙尘气溶胶产生的大气顶短波、长波和总辐射强迫分别为-1.3±0.8 W m^(-2)、0.7±0.4W m^(-2)和-0.5±0.7 W m-2;地表短波、长波和总的辐射强迫值为-1.5±1.0 W m^(-2)、1.8±0.9 W m^(-2)和0.2±0.2 W m^(-2)。沙尘气溶胶长波辐射强迫对沙尘浓度的垂直分布敏感。高层沙尘气溶胶浓度越大,其在大气顶产生更强的正值长波辐射强迫。然而,沙尘气溶胶短波辐射强迫主要受整层沙尘柱浓度控制,对沙尘浓度的垂直分布较不敏感。本文结果可为中国沙尘气溶胶的气候模拟提供参考。
