To better understand the seasonal characteristics of urban organic aerosol(OA)in the North China Plain(NCP),PM2.5 samples in the urban atmosphere of Liaocheng were collected and analyzed.The molecular distribution of ...To better understand the seasonal characteristics of urban organic aerosol(OA)in the North China Plain(NCP),PM2.5 samples in the urban atmosphere of Liaocheng were collected and analyzed.The molecular distribution of the organic markers in the urban atmosphere of Liaocheng reveals that n-alkanes(39.3%)was the most abundant species all year round,followed by saccharides(28.2%),phthalic acids(Ph,20.8%),biogenic secondary organic aerosol(BSOA)tracers(9.4%),and polycyclic aromatic hydrocarbon(PAHs,2.3%).PM2.5,organic carbon(OC),elemental carbon(EC),and primary organic markers exhibit the highest concentrations in winter,due largely to the increased biomass burning and coal combustion for house heating in local and surrounding regions.However,the concentration and relative abundance of BSOA are significantly higher in summer than other seasons,induced by the more favorable meteoro-logical conditions that would promote the emissions of biogenic volatile organic compounds(BVOCs)and the secondary production of BSOA.The ratios of OC/EC and 3-methyl-1,2,3-butanetricarboxylic acid to cis-pinic acid plus cis-pinonic acid(MBTCA/(PA+PNA)are higher in the warm seasons than those in the cold seasons,indicating that the oxidation of OA is sensitive to air temperature.Compared to 2017,the concentration level of PAHs during wintertime decreased by 40.8%,confirming that the stringent regulation of coal burning is effective.The highest concentration of high molecular weight(HMW)n-alkanes and three anhydrosugars in winter,and the close correlation of levoglucosan with HMW n-al-kanes suggests that the impact of biomass burning was more significant in winter.The same seasonal characteristic of the ratios of high-/low-NO_(x) products with NO_(x) and the strong correlation of high-/low-NO_(x) products with levoglucosan indicate that the formation of isoprene SOA(SOA1)tracers was signif-icantly influenced by anthropogenic emissions.The molecular compositions,the distributions of fire spots,backward trajectories of air masses,and correlation analysis suggest that air pollution events in spring were primarily resulted from biomass burning and secondary oxidation,while pollution events in winter were largely driven by the increased combustion sources,and promoted aqueous secondary formation.Our results suggest that the reduction of biomass and coal combustion should be taken into account to improve the urban air quality in the NCP.展开更多
To investigate the effect of covID-19 control measures on aerosol chemistry,the chemical compositions,mixing states,and formation mechanisms of carbonaceous particles in the urban atmosphere of Liao-cheng in the North...To investigate the effect of covID-19 control measures on aerosol chemistry,the chemical compositions,mixing states,and formation mechanisms of carbonaceous particles in the urban atmosphere of Liao-cheng in the North China Plain(NCP)were compared before and during the pandemic using a single particle aerosol mass spectrometry(SPAMS).The results showed that the concentrations of five air pollutants including PM2.5,PM1o,SO2,NO2,and cO decreased by 41.2%-71.5%during the pandemic compared to those before the pandemic,whereas O3 increased by 1.3 times during the pandemic because of the depressed titration of O3 and more favorable meteorological conditions.The count and percentage contribution of carbonaceous particles in the total detected particles were lower during the pandemic than those before the pandemic.The carbonaceous particles were dominated by elemental and organic carbon(ECOC,35.9%),followed by elemental carbon-aged(EC-aged,19.6%)and organic carbon-fresh(OC-fresh,13.5%)before the pandemic,while EC-aged(25.3%),ECOC(17.9%),and secondary ions-rich(SEC,17.8%)became the predominant species during the pandemic.The carbonaceous particle sizes during the pandemic showed a broader distribution than that before the pandemic,due to the condensation and coagulation of carbonaceous particles in the aging processes.The relative aerosol acidity(Rra)was smaller before the pandemic than that during the pandemic,indicating the more acidic particle aerosol during the pandemic closely related to the secondary species and relative humidity(RH).More than 95.0%and 86.0%of carbonaceous particles in the whole period were internally mixed with nitrate and sulfate,implying that most of the carbonaceous particles were associated with secondary oxidation during their formation processes.The diurnal variations of oxalate particles and correlation analyses suggested that oxalate particles before the pandemic were derived from aqueous oxidation driven by RH and liquid water content(LwC),while oxalate particles during the pandemic were originated from O3-dominatedphotochemical oxidation.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.42177083)the Natural Science Foundation of Shandong Province(Grant No.ZR2020MD113)the Open Funds of State Key Laboratory of Loess and Quaternary Geology,Institute of Earth Environment,Chinese Academy of Sciences(Grant No.SKLLOG 2020).
文摘To better understand the seasonal characteristics of urban organic aerosol(OA)in the North China Plain(NCP),PM2.5 samples in the urban atmosphere of Liaocheng were collected and analyzed.The molecular distribution of the organic markers in the urban atmosphere of Liaocheng reveals that n-alkanes(39.3%)was the most abundant species all year round,followed by saccharides(28.2%),phthalic acids(Ph,20.8%),biogenic secondary organic aerosol(BSOA)tracers(9.4%),and polycyclic aromatic hydrocarbon(PAHs,2.3%).PM2.5,organic carbon(OC),elemental carbon(EC),and primary organic markers exhibit the highest concentrations in winter,due largely to the increased biomass burning and coal combustion for house heating in local and surrounding regions.However,the concentration and relative abundance of BSOA are significantly higher in summer than other seasons,induced by the more favorable meteoro-logical conditions that would promote the emissions of biogenic volatile organic compounds(BVOCs)and the secondary production of BSOA.The ratios of OC/EC and 3-methyl-1,2,3-butanetricarboxylic acid to cis-pinic acid plus cis-pinonic acid(MBTCA/(PA+PNA)are higher in the warm seasons than those in the cold seasons,indicating that the oxidation of OA is sensitive to air temperature.Compared to 2017,the concentration level of PAHs during wintertime decreased by 40.8%,confirming that the stringent regulation of coal burning is effective.The highest concentration of high molecular weight(HMW)n-alkanes and three anhydrosugars in winter,and the close correlation of levoglucosan with HMW n-al-kanes suggests that the impact of biomass burning was more significant in winter.The same seasonal characteristic of the ratios of high-/low-NO_(x) products with NO_(x) and the strong correlation of high-/low-NO_(x) products with levoglucosan indicate that the formation of isoprene SOA(SOA1)tracers was signif-icantly influenced by anthropogenic emissions.The molecular compositions,the distributions of fire spots,backward trajectories of air masses,and correlation analysis suggest that air pollution events in spring were primarily resulted from biomass burning and secondary oxidation,while pollution events in winter were largely driven by the increased combustion sources,and promoted aqueous secondary formation.Our results suggest that the reduction of biomass and coal combustion should be taken into account to improve the urban air quality in the NCP.
基金supported by the National Natural Science Fund of China(grant number 42177083)Natural Science Foundation of Shandong Province(grant number ZR2020MD113)and Open Funds of State Key Laboratory of Loess and Quaternary Geology,Institute of Earth Environment,Chinese Academy of Sciences(grant number SKLLOG2020).
文摘To investigate the effect of covID-19 control measures on aerosol chemistry,the chemical compositions,mixing states,and formation mechanisms of carbonaceous particles in the urban atmosphere of Liao-cheng in the North China Plain(NCP)were compared before and during the pandemic using a single particle aerosol mass spectrometry(SPAMS).The results showed that the concentrations of five air pollutants including PM2.5,PM1o,SO2,NO2,and cO decreased by 41.2%-71.5%during the pandemic compared to those before the pandemic,whereas O3 increased by 1.3 times during the pandemic because of the depressed titration of O3 and more favorable meteorological conditions.The count and percentage contribution of carbonaceous particles in the total detected particles were lower during the pandemic than those before the pandemic.The carbonaceous particles were dominated by elemental and organic carbon(ECOC,35.9%),followed by elemental carbon-aged(EC-aged,19.6%)and organic carbon-fresh(OC-fresh,13.5%)before the pandemic,while EC-aged(25.3%),ECOC(17.9%),and secondary ions-rich(SEC,17.8%)became the predominant species during the pandemic.The carbonaceous particle sizes during the pandemic showed a broader distribution than that before the pandemic,due to the condensation and coagulation of carbonaceous particles in the aging processes.The relative aerosol acidity(Rra)was smaller before the pandemic than that during the pandemic,indicating the more acidic particle aerosol during the pandemic closely related to the secondary species and relative humidity(RH).More than 95.0%and 86.0%of carbonaceous particles in the whole period were internally mixed with nitrate and sulfate,implying that most of the carbonaceous particles were associated with secondary oxidation during their formation processes.The diurnal variations of oxalate particles and correlation analyses suggested that oxalate particles before the pandemic were derived from aqueous oxidation driven by RH and liquid water content(LwC),while oxalate particles during the pandemic were originated from O3-dominatedphotochemical oxidation.
