Exploring secondary organic aerosol(SOA)processes is crucial for understanding climate and air pollution in megacities.This study introduces a new method using positive matrix factorization(PMF)to investigate the SOA ...Exploring secondary organic aerosol(SOA)processes is crucial for understanding climate and air pollution in megacities.This study introduces a new method using positive matrix factorization(PMF)to investigate the SOA process by integrating the OA and associated ions previously misidentified as inorganic aerosol in high-resolution aerosol mass spectrometry data.The mass spectra and time series of primary OA(POA)and less oxidized oxygenated OA(OOA)identified by this new method resembled those resolved by traditional PMF.However,more oxidized OOA(MO-OOA)identified by traditional PMF can be further subdivided into multiple OA factors,including nitrogen-enriched OA(ON-OA)and sulfur-enriched OA(OS-OA)in summer,and ON-OA,OS-OA,and OOA in winter.Our findings highlight the significant role of photochemical processes in the formation of OS-OA compared to ON-OA.The compositions of reconstructed MO-OOA varied under different Ox(=O_(3)+NO_(2))and relative humidity conditions,emphasizing the limitations of using a constant mass spectrum.Aged biomass burning OA(BBOA)and coal combustion OA(CCOA),previously misattributed as POA,contributed 9.2%(0.43μg m^(−3))and 7.0%(0.33μg m^(−3))to SOA,respectively.Aged BBOA was more prone to forming OS-OA,whereas ON-OA showed higher correlations with aged CCOA,indicating distinct molecular compositions of SOA from different aged POA sources.Compared to aged BBOA,aged CCOA was more subject to conversion during aqueous phase processing.These results suggest that the variations in mass spectra and compositions need to be considered when simulating SOA processes.展开更多
Thermodynamic modeling is still themostwidely usedmethod to characterize aerosol acidity,a critical physicochemical property of atmospheric aerosols.However,it remains unclear whether gas-aerosol partitioning should b...Thermodynamic modeling is still themostwidely usedmethod to characterize aerosol acidity,a critical physicochemical property of atmospheric aerosols.However,it remains unclear whether gas-aerosol partitioning should be incorporated when thermodynamicmodels are employed to estimate the acidity of coarse particles.In this work,field measurements were conducted at a coastal city in northern China across three seasons,and covered wide ranges of temperature,relative humidity and NH_(3) concentrations.We examined the performance of different modes of ISORROPIA-II(a widely used aerosol thermodynamic model)in estimating aerosol acidity of coarse and fine particles.The M0 mode,which incorporates gas-phase data and runs the model in the forward mode,provided reasonable estimation of aerosol acidity for coarse and fine particles.Compared to M0,the M1 mode,which runs the model in the forward mode but does not include gas-phase data,may capture the general trend of aerosol acidity but underestimates pH for both coarse and fine particles;M2,which runs the model in the reverse mode,results in large errors in estimated aerosol pH for both coarse and fine particles and should not be used for aerosol acidity calculations.However,M1 significantly underestimates liquid water contents for both fine and coarse particles,while M2 provides reliable estimation of liquid water contents.In summary,our work highlights the importance of incorporating gas-aerosol partitioning when estimating coarse particle acidity,and thus may help improve our understanding of acidity of coarse particles.展开更多
Heterogeneous oxidation by gas-phase oxidants is an important chemical transformation pathway of secondary organic aerosol(SOA)and plays an important role in controlling the abundance,properties,as well as climate and...Heterogeneous oxidation by gas-phase oxidants is an important chemical transformation pathway of secondary organic aerosol(SOA)and plays an important role in controlling the abundance,properties,as well as climate and health impacts of aerosols.However,our knowledge on this heterogeneous chemistry remains inadequate.In this study,the heterogeneous oxidation ofα-pinene ozonolysis SOA by hydroxyl(OH)radicals was investigated under both low and high relative humidity(RH)conditions,with an emphasis on the evolution of molecular composition of SOA and its RH dependence.It is found that the heterogeneous oxidation of SOA at an OH exposure level equivalent to 12 hr of atmospheric aging leads to particle mass loss of 60%at 25%RH and 95%at 90%RH.The heterogeneous oxidation strongly changes the molecular composition of SOA.The dimer-to-monomer signal ratios increase dramatically with rising OH exposure,in particular under high RH conditions,suggesting that aerosol water stimulates the reaction of monomers with OH radicals more than that of dimers.In addition,the typical SOA tracer compounds such as pinic acid,pinonic acid,hydroxy pinonic acid and dimer esters(e.g.,C17H26O8 and C19H28O7)have lifetimes of several hours against heterogeneous OH oxidation under typical atmospheric conditions,which highlights the need for the consideration of their heterogeneous loss in the estimation of monoterpene SOA concentrations using tracer-based methods.Our study sheds lights on the heterogeneous oxidation chemistry ofmonoterpene SOA andwould help to understand their evolution and impacts in the atmosphere.展开更多
Aerosol hygroscopicity and liquid water content(ALWC)have important influences on the environmental and climate effect of aerosols.In this study,we measured the hygroscopic growth factors(GF)of particles with dry diam...Aerosol hygroscopicity and liquid water content(ALWC)have important influences on the environmental and climate effect of aerosols.In this study,we measured the hygroscopic growth factors(GF)of particles with dry diameters of 40,80,150,and 200 nm during the wintertime in Nanjing.Both the GF-derived hygroscopicity parameter(κ_(gf))and ALWC increased with particle size,but displayed differing diurnal variations,withκ_(gf)peaking around the midday,while ALWC peaking in the early morning.Nitrate,ammonium and oxygenated organic aerosols(OOA)were found as the chemical components mostly strongly correlated with ALWC.A closure study suggests that during midday photo-oxidation and nighttime high ALWC periods,theκof organic aerosols(κ_(org))was underestimated when using previous parameterizations.Accordingly,we re-constructed parameterizations forκ_(org)and the oxidation level of organics for these periods,which indicates a higher hygroscopicity of photochemically formed OOA than the aqueous OOA,yet both being much higher than the generally assumed OOA hygroscopicity.Additionally,in a typical high ALWC episode,concurrently increased ALWC,nitrate,OOA as well as aerosol surface area and mass concentrations were observed under elevated ambient RH.This strongly indicates a coupled effect that the hygroscopic secondary aerosols,in particular nitratewith strong hygroscopicity,led to large increase in ALWC,which in turn synergistically boosted nitrate and OOA formation by heterogeneous/aqueous reactions.Such interaction may represent an important mechanism contributing to enhanced formation of secondary aerosols and rapid growth of fine particulate matter under relatively high RH conditions.展开更多
Water-soluble organic aerosol(WSOA)plays a significant role in air quality and human health.Here we characterized the chemical properties and molecular compositions of WSOA at a rural site in North China Plain during ...Water-soluble organic aerosol(WSOA)plays a significant role in air quality and human health.Here we characterized the chemical properties and molecular compositions of WSOA at a rural site in North China Plain during winter using a high-resolution aerosol mass spectrometer and electrospray ionization high-resolution orbitrap mass spectrometer(ESI-HRMS).Our results show that the mass concentration of WSOA was significantly higher than that observed in Beijing in winter 2020,contributing about 56%of OA on average.CHO compounds(56%-74%)and CHN compounds(66%-80%)dominated in negative mode and positive mode,respectively,while CHON accounted for 15%-41%across both modes.The chemical characteristics of WSOA varied with polluted levels and between day and night.As pollution intensified,the abundance of CHO-compounds with condensed aromatics increased by 9%and the number of highly oxygenated molecules(HOMs)molecular formula detected in server haze was more than double that of clean days.CHO-compounds with ten carbon atoms(C_(10))were more abundant at night while those with nine carbon atoms(C_(9))were higher during the day.High levels of CHN+compounds were linked to nighttime biomass burning,whereas CHON compounds were more abundant during the day.Increased pollution also led to the formation of more complex CHON-compounds,indicating that organonitrates continue to play a significant role in rural pollution.展开更多
Aerosol acidity(pH)plays an important role in the multiphase chemical processes of atmospheric particles.In this study,we demonstrated the seasonal trends of aerosol pH calculated with the ISORROPIA-II model in a coas...Aerosol acidity(pH)plays an important role in the multiphase chemical processes of atmospheric particles.In this study,we demonstrated the seasonal trends of aerosol pH calculated with the ISORROPIA-II model in a coastal city of southeast China.We performed quantitative analysis on the various influencing factors on aerosol pH,and explored the responses of aerosol pH to different PM_(2.5)and O_(3)pollution levels.The results showed that the average aerosol pH was 2.92±0.61,following the order of winter>spring>summer>autumn.Sensitivity tests revealed that SO_(4)^(2−),NH_(x),T and RH triggered the variations of aerosol pH.Quantitative analysis results showed that T(37.9%-51.2%)was the main factors affecting pH variations in four seasons,followed by SO_(4)^(2−)(6.1%-23.7%),NH_(x)(7.2%-22.2%)and RH(0–14.2%).Totally,annual mean meteorological factors(52.9%)and chemical compositions(41.3%)commonly contributed the aerosolpH in the coastal city.The concentrations of PM_(2.5)was positively correlated with aerosol liquid water content(R^(2)=0.53)and aerosol pH(R^(2)=0.26),indicating that the increase in pH was related with the elevated NH_(4)NO_(3)and decreased SO_(4)^(2−),and also the changes of T and RH.The O_(x)(O_(3)+NO_(2))was moderately correlated with aerosol pH(R^(2)=-0.48),attributable to the fact that the proportion of SO_(4)^(2−)increased under high T and low RH conditions.The study strengthened our understanding of the contributions of influencing factors to aerosol pH,and also provided scientific evidences for chemical processes of atmospheric particles in coastal areas.展开更多
The outbreak of severe acute respiratory syndrome coronavirus 2(SARS-CoV-2)in late 2019 has negatively affected people's lives and productivity.Because the mode of transmission of SARS-CoV-2 is of great concern,th...The outbreak of severe acute respiratory syndrome coronavirus 2(SARS-CoV-2)in late 2019 has negatively affected people's lives and productivity.Because the mode of transmission of SARS-CoV-2 is of great concern,this review discusses the sources of virus aerosols and possible transmission routes.First,we discuss virus aerosol collection methods,including natural sedimentation,solid impact,liquid impact,centrifugal,cyclone and electrostatic adsorption methods.Then,we review common virus aerosol detection methods,including virus culture,metabolic detection,nucleic acid-based detection and immunology-based detection methods.Finally,possible solutions for the detection of SARS-CoV-2 aerosols are introduced.Point-of-care testing has long been a focus of attention.In the near future,the development of an instrument that integrates sampling and output results will enable the real-time,automatic monitoring of patients.展开更多
The impact of aerosols on clouds,which remains one of the largest aspects of uncertainty in current weather forecasting and climate change research,can be influenced by various factors,such as the underlying surface t...The impact of aerosols on clouds,which remains one of the largest aspects of uncertainty in current weather forecasting and climate change research,can be influenced by various factors,such as the underlying surface type,cloud type,cloud phase,and aerosol type.To explore the impact of different underlying surfaces on the effect of aerosols on cloud development,this study focused on the Yangtze River Delta(YRD)and its offshore regions(YRD sea)for a comparative analysis based on multi-source satellite data,while also considering the variations in cloud type and cloud phase.The results show lower cloud-top height and depth of single-layer clouds over the ocean than land,and higher liquid cloud in spring over the ocean.Aerosols are found to enhance the cumulus cloud depth through microphysical effects,which is particularly evident over the ocean.Aerosols are also found to decrease the cloud droplet effective radius in the ocean region and during the mature stage of cloud development in the land region,while opposite results are found during the early stage of cloud development in the land region.The quantitative results indicate that the indirect effect is positive(0.05)in the land region at relatively high cloud water path,which is smaller than that in the ocean region(0.11).The findings deepen our understanding of the influence aerosols on cloud development and the mechanisms involved,which could then be applied to improve the ability to simulate cloud-associated weather processes.展开更多
With the rapid development of the world economy,complex air pollution has increasingly become a serious threat;for example,with haze events occurring frequently in various regions of the globe.Recent evidence has indi...With the rapid development of the world economy,complex air pollution has increasingly become a serious threat;for example,with haze events occurring frequently in various regions of the globe.Recent evidence has indicated that secondary aerosols play an important role in haze formation,and that heterogeneous processes are among the main forces driving their explosive growth.In this regard,this paper reviews recent advances in the understanding of the impact of heterogeneous processes on haze chemistry,including the impact on NO_(2)chemistry,marine aerosols,and the hygroscopicity and optical properties of atmospheric aerosols.It is distinguished from past reviews on this topic by focusing mainly on new insights from the past five years.We summarize the main findings of the impacts of heterogeneous processes on NO_(2)chemistry,marine aerosols,and the physicochemical properties of atmospheric aerosols,and propose several future research directions.展开更多
Understanding the variations and potential source of air pollution is essential for implementing targeted mitigation actions.However,the distribution and long-term trends of Aerosol Optical Depth(AOD)and its component...Understanding the variations and potential source of air pollution is essential for implementing targeted mitigation actions.However,the distribution and long-term trends of Aerosol Optical Depth(AOD)and its components over the Fenwei Plain(FWP)have not been thoroughly investigated.Furthermore,the potential source contribution of AOD loading is still unclear.Thus,maximum synthesis and Mann-Kendall trend(MK)test with Sen's Slope methods are employed to reveal the spatiotemporal variation characteristics of AOD over the FWP.The Potential Source Contribution Function(PSCF)model was applied to analyze the potential source contribution of AOD over the FWP.Results demonstrated that the AOD in spatial pattern exhibited consistency with the topography.AOD over the FWP fluctuated annually from 2000 to 2020,with an increase in the previous decade followed by a gradual decline after 2011.There was a significant monthly variation in AOD with higher values in August(0.47±0.21)and lower in November(0.29±0.12).A positive AOD trend was confirmed from 2000 to 2010 yet a negative trend is identified from 2011 to 2020.The sulfate aerosol(AODSU)exhibited an increasing trend over an extended period.Clear-sky radiation shows a negative trend at the surface and the top of the atmosphere(TOA)from 2000 to 2010,which is consistent with the trend in AOD.The AOD in FWP was primarily influenced by local emissions,with contributions from northern and northwestern sources.This research offers an enhanced overarching comprehension of the distribution and regional climate effects of aerosols over the FWP.展开更多
To investigate the seasonal characteristics in air pollution in Chengdu,a single particle aerosol mass spectrometry was used to continuously observe atmospheric fine particulate matter during one-month periods in summ...To investigate the seasonal characteristics in air pollution in Chengdu,a single particle aerosol mass spectrometry was used to continuously observe atmospheric fine particulate matter during one-month periods in summer and winter,respectively.The results showed that,apart from O_(3),the concentrations of other pollutants(CO,NO_(2),SO_(2),PM_(2.5)and PM_(10))were significantly higher in winter than in summer.All single particle aerosols were divided into seven categories:biomass burning(BB),coal combustion(CC),Dust,vehicle emission(VE),K mixedwith nitrate(K-NO_(3)),Kmixed with sulfate and nitrate(K-SN),and K mixedwith sulfate(K-SO_(4))particles.The highest contributions in both seasons were VE particles(24%).The higher contributions of K-SO_(4)(16%)and K-NO_(3)(10%)particles occurred in summer and winter,respectively,as a result of their different formation mechanisms.S-containing(KSO_(4)and K-SN),VE,and BB particles caused the evolution of pollution in both seasons,and they can be considered as targets for future pollution reduction.The mixing of primary sources particles(VE,Dust,CC,and BB)with secondary components was stronger in winter than in summer.In summer,as pollution worsens,the mixing of primary sources particles with 62[NO_(3)]−weakened,but themixing with 97[HSO_(4)]−increased.However,in winter,the mixing state of particles did not exhibit an obvious evolution rules.The potential source areas in summer were mainly distributed in the southern region of Sichuan,while in winter,besides the southern region,the contribution of the western region cannot be ignored.展开更多
Ultrasonic humidifiers are commonly used in households to maintain indoor humidity and generate a large number of droplets or spray aerosols.However,there have been various health concerns associated with humidifier u...Ultrasonic humidifiers are commonly used in households to maintain indoor humidity and generate a large number of droplets or spray aerosols.However,there have been various health concerns associated with humidifier use,largely due to aerosols generated during operation.Here,we investigated the size distribution,chemical composition,and charged fraction of aerosol particles emitted from commercial ultrasonic humidifiers.Heavy metals in water used for humidifiers were found to be highly enriched in the ultrasonic humidifier aerosols(UHA),with the enrichment factors ranging from 102 to 107.This enrichment may pose health concerns for the building occupants,as UHA concentrations of up to 106 particles/cm^(3) or 3 mg/m^(3) were observed.Furthermore,approximately 90%of UHA were observed to be electrically charged,for the first time according to our knowledge.Based on this discovery,we proposed and tested a newmethod to remove UHA by using a simple electrical field.The designed electrical field in this work can efficiently remove 81.4%of UHA.Therefore,applying this electrical field could be an effective method to significantly reduce the health risks by UHA.展开更多
Objective:To explore nursing measures for elderly patients with chronic obstructive pulmonary disease(COPD)and analyze the effect of continuous nursing pathways on improving the accuracy of aerosol use.Methods:From Ap...Objective:To explore nursing measures for elderly patients with chronic obstructive pulmonary disease(COPD)and analyze the effect of continuous nursing pathways on improving the accuracy of aerosol use.Methods:From April 2023 to April 2024,76 elderly COPD patients admitted to our hospital were randomly selected for nursing research.They were divided into two groups using a computer double-blind method,with 38 patients in each group.The control group received routine nursing,while the observation group applied the continuous nursing pathway.The nursing effects of the two groups were investigated and compared,including(1)aerosol accuracy;(2)cardiopulmonary function;(3)subjective well-being and self-care ability;(4)quality of life;and(5)nursing satisfaction.Results:Compared with the control group,the observation group had a significantly higher accuracy rate of aerosol use(P<0.05).Before nursing,there were no significant differences in cardiopulmonary function indicators,MUNSH scores,and ESCA scores between the two groups(P>0.05).After nursing,the patient's cardiopulmonary function improved significantly,and their subjective well-being and self-care ability increased.The observation group was significantly better than the control group in all the above indicators(P<0.05).The quality of life scores of the observation group were significantly higher than those of the control group(P<0.05).Conclusion:In the nursing of elderly patients with chronic obstructive pulmonary disease,the application of the continuous nursing pathway can effectively improve the accuracy of aerosol use and improve patients'cardiopulmonary function.展开更多
Aerosol particle pollution has become an increasing serious environmental problem,and urban vegetation plays a long-lasting and positive role in mitigating it.This study compared the particle capture abilities of tree...Aerosol particle pollution has become an increasing serious environmental problem,and urban vegetation plays a long-lasting and positive role in mitigating it.This study compared the particle capture abilities of trees,shrubs,and herbs,and examined the compositions and influence of aerosol particles accumulated on leaf functional traits.Retained particles primarily contained Ca^(2+),K^(+),SO_(4)^(2-),NO_(3)^(-)and NH_(4)^(+),indicating their anthropogenic origins.The leathery-leaved tree Osmanthus fragrans and the papery-leaved herb Alternanthera sessilis demonstrated the higher competence in particle accumulation than other plants,and leaf morphologic structures(e.g.,leaf grooves,trichomes,waxy layers,and stomata characteristics)were closely associated with particle capture by plant species.Particle retention negatively impacted stomata,impeding photosynthesis,and reducing transpiration.In response to particle accumulation,plants tended to decrease specific leaf area and adjust stomatal conductance.Both growth form and leaf texture significantly influenced the particle capture abilities of different plant species.The substantial contribution of plants,particularly herbs in the lower vegetation strata,to particle removal should not be overlooked.Vegetation with a tree-shrub-herb configuration excels at particle capture,offering potential advantages in mitigating particle pollution and enhancing ecological benefits.展开更多
Enhanced mass concentrations of aromatic-derived secondary organic aerosol(SOA)are frequently observed during humid-haze events.However,the influencing mechanism of relative humidity(RH)in aromatic-derived SOA formati...Enhanced mass concentrations of aromatic-derived secondary organic aerosol(SOA)are frequently observed during humid-haze events.However,the influencing mechanism of relative humidity(RH)in aromatic-derived SOA formation remains incompletely understood.Here,the RH dependence of SOA formation in the presence of NOx was explored by a series of chamber experiments for toluene(TOL)and 1,3,5-trimethylbenzene(TMB)photooxidation.The yield of TOL SOA and TMB SOA increased by 221%and 52%with increasing RH from~8%to~70%,respectively.Analytical results from a high-resolution mass spectrometer showed that SOA constituents with high oxygen content(O/C>0.6)were more abundant in SOA formed in the~70%RH experiment.The elevated yields and O/C of SOA could be attributed to the promoted formation and particle-phase diffusivity of highly oxidized molecules.In addition,in comparison with TMB,TOL could produce more unsaturated aldehydes,which are oxidized into carboxylic acids with high O/C,leading to a more sensitive response of TOL SOA formation to the change in RH.Our work provides mechanistic insights into RH roles in aromatic SOA formation and is helpful for a better understanding of humid-haze events.展开更多
We conducted a comprehensive analysis of seasonal and long-term variations in organic carbon(OC),elemental carbon(EC),primary organic carbon(POC),and secondary organic carbon(SOC)among total suspended particles on Hua...We conducted a comprehensive analysis of seasonal and long-term variations in organic carbon(OC),elemental carbon(EC),primary organic carbon(POC),and secondary organic carbon(SOC)among total suspended particles on Huaniao Island,China,from 2011 to 2020.The highest OC and EC concentrations were observed in 2014(OC,4.13μg/m^(3))and 2013(EC,1.21μg/m^(3)),respectively;for both,the lowest concentrations occurred in 2017(OC,1.56μg/m^(3);EC,0.69μg/m^(3)).OC and EC exhibited seasonal variations,such that the highest and lowest values for both occurred in winter and summer,respectively;particularly high concentrations were observed in the winter of 2014 on Huaniao Island.By 2020,winter OC and EC concentrations had decreased by 43%and 36%,whereas autumn OC and EC concentrations increased by 38%and 160%compared with 2014.In terms of carbon components,the proportions of OC4 and EC1 significantly declined,whereas the proportions of OC3 and OC2 increased,during the study period.Higher POC and SOC concentrations were mainly observed during the autumn–winter and winter–spring transition periods.POC was most strongly correlated with OC2,followed by OC4 and EC1.SOC was strongly correlated with OC3,especially in winter.These findings highlight the characteristics of temporal variations in individual carbon components,as well as possible associations with POC and SOC.展开更多
Biomass burning(BB)emits carbonaceous aerosols that significantly influence air quality in Southwest China during spring.To further understand the characteristics of spring BB and its original contribution to organic ...Biomass burning(BB)emits carbonaceous aerosols that significantly influence air quality in Southwest China during spring.To further understand the characteristics of spring BB and its original contribution to organic carbon(OC),daily fine particulate matter(PM_(2.5))samples were collected from March to May 2022 in Pu'er,Southwest China.The concentrations of OC,elemental carbon(EC),levoglucosan(Lev),and potassium from BB(K+BB)during the study period ranged from 5.3 to 31.2μg/m^(3),0.86-13.1μg/m^(3),0.06-0.82μg/m^(3),and 0.05-2.88μg/m^(3),respectively.To eliminate the effects of Lev degradation,this study uses the Aging of Air Mass(AAM)index to correct the atmospheric concentration of Lev and combines Bayesian mixture modeling with a molecular tracer method to assess the original contribution of BB to OC.The results indicated that the AAM index was 0.18±0.05,indicating that the degradation of Lev reached 82%.When considering the degradation of levoglucosan in the atmosphere,the primary source of BB aerosols was crop-straw combustion(71.1%),followed by the combustion of certain hardwoods and softwoods(24.9%)and grasses(4.0%).The original contribution of BB to OC was 62.4%,which was much greater than the contribution when levoglucosan degradation(23.7%)was ignored.The air mass inverse trajectories and Moderate Resolution Imaging Spectroradiometer(MODIS)fire hotspots indicated that the BB plume from Southeast Asia during spring could influence PM_(2.5)long-range transport in remote locations,and the contribution could reach 82%in Southwest China.展开更多
Accurate descriptions of cloud droplet spectra from aerosol activation to vapor condensation using microphysical parameterization schemes are crucial for numerical simulations of precipitation and climate change in we...Accurate descriptions of cloud droplet spectra from aerosol activation to vapor condensation using microphysical parameterization schemes are crucial for numerical simulations of precipitation and climate change in weather forecasting and climate prediction models.Hence,the latest activation and triple-moment condensation schemes were combined to simulate and analyze the evolution characteristics of a cloud droplet spectrum from activation to condensation and compared with a high-resolution Lagrangian bin model and the current double-moment condensation schemes,in which the spectral shape parameter is fixed or diagnosed by an empirical formula.The results demonstrate that the latest schemes effectively capture the evolution characteristics of the cloud droplet spectrum during activation and condensation,which is in line with the performance of the bin model.The simulation of the latest activation and condensation schemes in a parcel model shows that the cloud droplet spectrum gradually widens and exhibits a multimodal distribution during the activation process,accompanied by a decrease in the spectral shape and slope parameters over time.Conversely,during the condensation process,the cloud droplet spectrum gradually narrows,resulting in increases in the spectral shape and slope parameters.However,these double-moment schemes fail to accurately replicate the evolution of the cloud droplet spectrum and its multimodal distribution characteristics.Furthermore,the latest schemes were coupled into a 1.5D cumulus model,and an observation case was simulated.The simulations confirm that the cloud droplet spectrum appears wider at the supersaturated cloud base and cloud top due to activation,while it becomes narrower at the middle altitudes of the cloud due to condensation growth.展开更多
The compositions and distributions of monoterpenes,isoprene,aromatics and sesquiterpene SOA tracers(SOAM,SOAI,SOAA and SOAS,respectively)at an island site(Da Wan Shan Island,DWS)were investigated in the context of the...The compositions and distributions of monoterpenes,isoprene,aromatics and sesquiterpene SOA tracers(SOAM,SOAI,SOAA and SOAS,respectively)at an island site(Da Wan Shan Island,DWS)were investigated in the context of the influence of continental and marine air masses over the Pearl River Estuary(PRE)region in winter 2021.The sum concentration of SOA tracers was 6.2–132.8 ng m^(−3),with SOAM and SOAI as the main components in both continental(scenarios A1 and A2)and marine air masses(scenario A3),as well as their combination(scenario A4).The highest and lowest levels of SOAM were observed in A1 and A3,respectively,which were mainly related to the variations in meteorological conditions,precursor concentrations,and the degree of photochemical processes.Higher MBTCA/HGA(3-methyl-1,2,3-butanetricarboxylic acid/3-hydroxyglutaric acid)ratios suggested a less significant contribution fromα-pinene to SOAM.The variations of SOAI in the different scenarios were associated with differences in relative humidity,particle acidity,and isoprene/NOx ratios.The respective highest and lowest concentrations of aromatics SOA tracers in A1 and A3 revealed the influence of anthropogenic precursors from upwind continental areas,which was confirmed by the correlation among biogenic and anthropogenic precursors.The results of the tracer-based-method suggested dominant contributions of SOAs from aromatics and monoterpenes,with the highest concentrations in A1.A WRF-Chem simulation revealed that the SOAs from the above precursors only contributed 12%–25%to the total SOA at DWS,while the spatial distributions of SOAs further highlighted that the abundance of SOAs over the PRE region in winter is highly associated with air masses transported from upwind continental areas.展开更多
Elucidating the mutual effects between the different volatile organic compounds(VOCs)is crucial for comprehending the formation mechanism of atmospheric secondary organic aerosols(SOA).Here,the mixed VOCs experiments ...Elucidating the mutual effects between the different volatile organic compounds(VOCs)is crucial for comprehending the formation mechanism of atmospheric secondary organic aerosols(SOA).Here,the mixed VOCs experiments of isoprene and△^(3)-carene/β-caryophyllene were carried out in the presence of O_(3)using an indoor smog chamber.The suppression effect of isoprene was recognized by the scanning mobility particle sizer spectrometer,online vacuum ultraviolet free electron laser(VUV-FEL)photoionization aerosol mass spectrometry,and quantum chemical calculations.The results indicate that the suppression effect of isoprene on the ozonolysis of△^(3)-carene andβ-caryophyllene shows fluctuating and monotonous trends,respectively.The carbon content of the precursor could be themain factor for regulating the strength of the suppression effect.Plausible structures and formation mechanisms of several new products generated from the single VOC precursor and VOC-cross-reaction are proposed,which enrich the category of VOC oxidation products.Meanwhile,a new dimerization mechanism of the RO_(2)+R’O_(2)reaction is suggested,which offers an intriguing perspective on the gas phase formation process of particle phase accretion products.The present findings provide valuable insights into clarifying the pivotal roles played by isoprene in the interplay between different VOCs and understanding of SOA formation mechanisms of VOC mixtures,especially nearby the emission origins.展开更多
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB0760200)the National Natural Science Foundation of China(Grant No.42377101,91744207).
文摘Exploring secondary organic aerosol(SOA)processes is crucial for understanding climate and air pollution in megacities.This study introduces a new method using positive matrix factorization(PMF)to investigate the SOA process by integrating the OA and associated ions previously misidentified as inorganic aerosol in high-resolution aerosol mass spectrometry data.The mass spectra and time series of primary OA(POA)and less oxidized oxygenated OA(OOA)identified by this new method resembled those resolved by traditional PMF.However,more oxidized OOA(MO-OOA)identified by traditional PMF can be further subdivided into multiple OA factors,including nitrogen-enriched OA(ON-OA)and sulfur-enriched OA(OS-OA)in summer,and ON-OA,OS-OA,and OOA in winter.Our findings highlight the significant role of photochemical processes in the formation of OS-OA compared to ON-OA.The compositions of reconstructed MO-OOA varied under different Ox(=O_(3)+NO_(2))and relative humidity conditions,emphasizing the limitations of using a constant mass spectrum.Aged biomass burning OA(BBOA)and coal combustion OA(CCOA),previously misattributed as POA,contributed 9.2%(0.43μg m^(−3))and 7.0%(0.33μg m^(−3))to SOA,respectively.Aged BBOA was more prone to forming OS-OA,whereas ON-OA showed higher correlations with aged CCOA,indicating distinct molecular compositions of SOA from different aged POA sources.Compared to aged BBOA,aged CCOA was more subject to conversion during aqueous phase processing.These results suggest that the variations in mass spectra and compositions need to be considered when simulating SOA processes.
基金supported by the National Natural Science Foundation of China (Nos.42022050 and 42277088)the Guangdong Basic and Applied Basic Research Fund Committee (Nos.2021A1515011248 and 2023A1515012010)the Guangdong Foundation for the Program of Science and Technology Research (No.2020B1212060053).
文摘Thermodynamic modeling is still themostwidely usedmethod to characterize aerosol acidity,a critical physicochemical property of atmospheric aerosols.However,it remains unclear whether gas-aerosol partitioning should be incorporated when thermodynamicmodels are employed to estimate the acidity of coarse particles.In this work,field measurements were conducted at a coastal city in northern China across three seasons,and covered wide ranges of temperature,relative humidity and NH_(3) concentrations.We examined the performance of different modes of ISORROPIA-II(a widely used aerosol thermodynamic model)in estimating aerosol acidity of coarse and fine particles.The M0 mode,which incorporates gas-phase data and runs the model in the forward mode,provided reasonable estimation of aerosol acidity for coarse and fine particles.Compared to M0,the M1 mode,which runs the model in the forward mode but does not include gas-phase data,may capture the general trend of aerosol acidity but underestimates pH for both coarse and fine particles;M2,which runs the model in the reverse mode,results in large errors in estimated aerosol pH for both coarse and fine particles and should not be used for aerosol acidity calculations.However,M1 significantly underestimates liquid water contents for both fine and coarse particles,while M2 provides reliable estimation of liquid water contents.In summary,our work highlights the importance of incorporating gas-aerosol partitioning when estimating coarse particle acidity,and thus may help improve our understanding of acidity of coarse particles.
基金supported by the National Natural Science Foundation of China (Nos.22022607 and 42005090)the Shanghai Pujiang Program (No.20PJ1407600)。
文摘Heterogeneous oxidation by gas-phase oxidants is an important chemical transformation pathway of secondary organic aerosol(SOA)and plays an important role in controlling the abundance,properties,as well as climate and health impacts of aerosols.However,our knowledge on this heterogeneous chemistry remains inadequate.In this study,the heterogeneous oxidation ofα-pinene ozonolysis SOA by hydroxyl(OH)radicals was investigated under both low and high relative humidity(RH)conditions,with an emphasis on the evolution of molecular composition of SOA and its RH dependence.It is found that the heterogeneous oxidation of SOA at an OH exposure level equivalent to 12 hr of atmospheric aging leads to particle mass loss of 60%at 25%RH and 95%at 90%RH.The heterogeneous oxidation strongly changes the molecular composition of SOA.The dimer-to-monomer signal ratios increase dramatically with rising OH exposure,in particular under high RH conditions,suggesting that aerosol water stimulates the reaction of monomers with OH radicals more than that of dimers.In addition,the typical SOA tracer compounds such as pinic acid,pinonic acid,hydroxy pinonic acid and dimer esters(e.g.,C17H26O8 and C19H28O7)have lifetimes of several hours against heterogeneous OH oxidation under typical atmospheric conditions,which highlights the need for the consideration of their heterogeneous loss in the estimation of monoterpene SOA concentrations using tracer-based methods.Our study sheds lights on the heterogeneous oxidation chemistry ofmonoterpene SOA andwould help to understand their evolution and impacts in the atmosphere.
基金supported by the National Natural Science Foundation of China(Nos.42275116 and 41975172).
文摘Aerosol hygroscopicity and liquid water content(ALWC)have important influences on the environmental and climate effect of aerosols.In this study,we measured the hygroscopic growth factors(GF)of particles with dry diameters of 40,80,150,and 200 nm during the wintertime in Nanjing.Both the GF-derived hygroscopicity parameter(κ_(gf))and ALWC increased with particle size,but displayed differing diurnal variations,withκ_(gf)peaking around the midday,while ALWC peaking in the early morning.Nitrate,ammonium and oxygenated organic aerosols(OOA)were found as the chemical components mostly strongly correlated with ALWC.A closure study suggests that during midday photo-oxidation and nighttime high ALWC periods,theκof organic aerosols(κ_(org))was underestimated when using previous parameterizations.Accordingly,we re-constructed parameterizations forκ_(org)and the oxidation level of organics for these periods,which indicates a higher hygroscopicity of photochemically formed OOA than the aqueous OOA,yet both being much higher than the generally assumed OOA hygroscopicity.Additionally,in a typical high ALWC episode,concurrently increased ALWC,nitrate,OOA as well as aerosol surface area and mass concentrations were observed under elevated ambient RH.This strongly indicates a coupled effect that the hygroscopic secondary aerosols,in particular nitratewith strong hygroscopicity,led to large increase in ALWC,which in turn synergistically boosted nitrate and OOA formation by heterogeneous/aqueous reactions.Such interaction may represent an important mechanism contributing to enhanced formation of secondary aerosols and rapid growth of fine particulate matter under relatively high RH conditions.
基金supported by the National Natural Science Foundation of China(No.42307139)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB0760200)。
文摘Water-soluble organic aerosol(WSOA)plays a significant role in air quality and human health.Here we characterized the chemical properties and molecular compositions of WSOA at a rural site in North China Plain during winter using a high-resolution aerosol mass spectrometer and electrospray ionization high-resolution orbitrap mass spectrometer(ESI-HRMS).Our results show that the mass concentration of WSOA was significantly higher than that observed in Beijing in winter 2020,contributing about 56%of OA on average.CHO compounds(56%-74%)and CHN compounds(66%-80%)dominated in negative mode and positive mode,respectively,while CHON accounted for 15%-41%across both modes.The chemical characteristics of WSOA varied with polluted levels and between day and night.As pollution intensified,the abundance of CHO-compounds with condensed aromatics increased by 9%and the number of highly oxygenated molecules(HOMs)molecular formula detected in server haze was more than double that of clean days.CHO-compounds with ten carbon atoms(C_(10))were more abundant at night while those with nine carbon atoms(C_(9))were higher during the day.High levels of CHN+compounds were linked to nighttime biomass burning,whereas CHON compounds were more abundant during the day.Increased pollution also led to the formation of more complex CHON-compounds,indicating that organonitrates continue to play a significant role in rural pollution.
基金supported by the National Natural Science Foundation of China(Nos.42277091 and U22A20578)Xiamen Youth Innovation Fund Project(No.3502Z20206094)+1 种基金Fujian Provincial Environmental Protection Science&Technology Plan Projects(No.2023R004)Xiamen Atmospheric Environment Observation and Research Station of Fujian Province.
文摘Aerosol acidity(pH)plays an important role in the multiphase chemical processes of atmospheric particles.In this study,we demonstrated the seasonal trends of aerosol pH calculated with the ISORROPIA-II model in a coastal city of southeast China.We performed quantitative analysis on the various influencing factors on aerosol pH,and explored the responses of aerosol pH to different PM_(2.5)and O_(3)pollution levels.The results showed that the average aerosol pH was 2.92±0.61,following the order of winter>spring>summer>autumn.Sensitivity tests revealed that SO_(4)^(2−),NH_(x),T and RH triggered the variations of aerosol pH.Quantitative analysis results showed that T(37.9%-51.2%)was the main factors affecting pH variations in four seasons,followed by SO_(4)^(2−)(6.1%-23.7%),NH_(x)(7.2%-22.2%)and RH(0–14.2%).Totally,annual mean meteorological factors(52.9%)and chemical compositions(41.3%)commonly contributed the aerosolpH in the coastal city.The concentrations of PM_(2.5)was positively correlated with aerosol liquid water content(R^(2)=0.53)and aerosol pH(R^(2)=0.26),indicating that the increase in pH was related with the elevated NH_(4)NO_(3)and decreased SO_(4)^(2−),and also the changes of T and RH.The O_(x)(O_(3)+NO_(2))was moderately correlated with aerosol pH(R^(2)=-0.48),attributable to the fact that the proportion of SO_(4)^(2−)increased under high T and low RH conditions.The study strengthened our understanding of the contributions of influencing factors to aerosol pH,and also provided scientific evidences for chemical processes of atmospheric particles in coastal areas.
基金the NSFC(Nos.61701176 and 62071119)Macao FDCT(No.0065/2020/A2)+5 种基金Natural Science Foundation of Hunan Province of China(Nos.2022JJ50052,2018JJ3130 and 2020JJ5145)Hunan Key R&D Projects(No.2021SK2003)Nanjing Important Science&Technology Specific Projects(No.2021-11005)2022 Special Project for the Construction of Innovative Provinces to Fight the COVID-19 Outbreak(No.2022SK2115)Open Funding of State Key Laboratory of Oral Diseases(No.SKLOD2022OF05)Shenzhen Innovation and Entrepreneurship Program Innovation and Entrepreneurship Special Project(No.20220624181237005).
文摘The outbreak of severe acute respiratory syndrome coronavirus 2(SARS-CoV-2)in late 2019 has negatively affected people's lives and productivity.Because the mode of transmission of SARS-CoV-2 is of great concern,this review discusses the sources of virus aerosols and possible transmission routes.First,we discuss virus aerosol collection methods,including natural sedimentation,solid impact,liquid impact,centrifugal,cyclone and electrostatic adsorption methods.Then,we review common virus aerosol detection methods,including virus culture,metabolic detection,nucleic acid-based detection and immunology-based detection methods.Finally,possible solutions for the detection of SARS-CoV-2 aerosols are introduced.Point-of-care testing has long been a focus of attention.In the near future,the development of an instrument that integrates sampling and output results will enable the real-time,automatic monitoring of patients.
基金supported by the National Natural Science Foundation of China(Grant No.42230601).
文摘The impact of aerosols on clouds,which remains one of the largest aspects of uncertainty in current weather forecasting and climate change research,can be influenced by various factors,such as the underlying surface type,cloud type,cloud phase,and aerosol type.To explore the impact of different underlying surfaces on the effect of aerosols on cloud development,this study focused on the Yangtze River Delta(YRD)and its offshore regions(YRD sea)for a comparative analysis based on multi-source satellite data,while also considering the variations in cloud type and cloud phase.The results show lower cloud-top height and depth of single-layer clouds over the ocean than land,and higher liquid cloud in spring over the ocean.Aerosols are found to enhance the cumulus cloud depth through microphysical effects,which is particularly evident over the ocean.Aerosols are also found to decrease the cloud droplet effective radius in the ocean region and during the mature stage of cloud development in the land region,while opposite results are found during the early stage of cloud development in the land region.The quantitative results indicate that the indirect effect is positive(0.05)in the land region at relatively high cloud water path,which is smaller than that in the ocean region(0.11).The findings deepen our understanding of the influence aerosols on cloud development and the mechanisms involved,which could then be applied to improve the ability to simulate cloud-associated weather processes.
基金supported by the National Key Research and Development Program of China(No.2022YFC3701000)the National Natural Science Foundation of China(Nos.42130606 and 41931287)+1 种基金the Beijing National Laboratory for Molecular Sciences(BNLMS-CXXM-202011)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.Y2021013).
文摘With the rapid development of the world economy,complex air pollution has increasingly become a serious threat;for example,with haze events occurring frequently in various regions of the globe.Recent evidence has indicated that secondary aerosols play an important role in haze formation,and that heterogeneous processes are among the main forces driving their explosive growth.In this regard,this paper reviews recent advances in the understanding of the impact of heterogeneous processes on haze chemistry,including the impact on NO_(2)chemistry,marine aerosols,and the hygroscopicity and optical properties of atmospheric aerosols.It is distinguished from past reviews on this topic by focusing mainly on new insights from the past five years.We summarize the main findings of the impacts of heterogeneous processes on NO_(2)chemistry,marine aerosols,and the physicochemical properties of atmospheric aerosols,and propose several future research directions.
基金supported by the National Natural Science Foundation of China(No.41905016)the Key Research and Development Program of Shaanxi Province(No.2024SF-YBXM-583)+1 种基金the Key Research and Development Project of Shaanxi Province(No.2021ZDLSF-05-07)the National Key Research and Development Plan of China(No.2017YFC0212206).
文摘Understanding the variations and potential source of air pollution is essential for implementing targeted mitigation actions.However,the distribution and long-term trends of Aerosol Optical Depth(AOD)and its components over the Fenwei Plain(FWP)have not been thoroughly investigated.Furthermore,the potential source contribution of AOD loading is still unclear.Thus,maximum synthesis and Mann-Kendall trend(MK)test with Sen's Slope methods are employed to reveal the spatiotemporal variation characteristics of AOD over the FWP.The Potential Source Contribution Function(PSCF)model was applied to analyze the potential source contribution of AOD over the FWP.Results demonstrated that the AOD in spatial pattern exhibited consistency with the topography.AOD over the FWP fluctuated annually from 2000 to 2020,with an increase in the previous decade followed by a gradual decline after 2011.There was a significant monthly variation in AOD with higher values in August(0.47±0.21)and lower in November(0.29±0.12).A positive AOD trend was confirmed from 2000 to 2010 yet a negative trend is identified from 2011 to 2020.The sulfate aerosol(AODSU)exhibited an increasing trend over an extended period.Clear-sky radiation shows a negative trend at the surface and the top of the atmosphere(TOA)from 2000 to 2010,which is consistent with the trend in AOD.The AOD in FWP was primarily influenced by local emissions,with contributions from northern and northwestern sources.This research offers an enhanced overarching comprehension of the distribution and regional climate effects of aerosols over the FWP.
基金supported by the Basic Research Cultivation Support Plan of Southwest Jiaotong University(No.2682023ZTPY016)the Natural Science Foundation of Sichuan Province(No.2022NSFSC0982)the National Natural Science Foundation of China(Nos.U23A2030,42205100,and 41805095).
文摘To investigate the seasonal characteristics in air pollution in Chengdu,a single particle aerosol mass spectrometry was used to continuously observe atmospheric fine particulate matter during one-month periods in summer and winter,respectively.The results showed that,apart from O_(3),the concentrations of other pollutants(CO,NO_(2),SO_(2),PM_(2.5)and PM_(10))were significantly higher in winter than in summer.All single particle aerosols were divided into seven categories:biomass burning(BB),coal combustion(CC),Dust,vehicle emission(VE),K mixedwith nitrate(K-NO_(3)),Kmixed with sulfate and nitrate(K-SN),and K mixedwith sulfate(K-SO_(4))particles.The highest contributions in both seasons were VE particles(24%).The higher contributions of K-SO_(4)(16%)and K-NO_(3)(10%)particles occurred in summer and winter,respectively,as a result of their different formation mechanisms.S-containing(KSO_(4)and K-SN),VE,and BB particles caused the evolution of pollution in both seasons,and they can be considered as targets for future pollution reduction.The mixing of primary sources particles(VE,Dust,CC,and BB)with secondary components was stronger in winter than in summer.In summer,as pollution worsens,the mixing of primary sources particles with 62[NO_(3)]−weakened,but themixing with 97[HSO_(4)]−increased.However,in winter,the mixing state of particles did not exhibit an obvious evolution rules.The potential source areas in summer were mainly distributed in the southern region of Sichuan,while in winter,besides the southern region,the contribution of the western region cannot be ignored.
基金supported by the National Natural Science Foundation of China (Nos.42077193 and 21976034)the National Key R&D Program (Nos.2022YFC3702600 and 2022YFC3702601)the Shanghai Natural Science Foundation (23ZR1479700).
文摘Ultrasonic humidifiers are commonly used in households to maintain indoor humidity and generate a large number of droplets or spray aerosols.However,there have been various health concerns associated with humidifier use,largely due to aerosols generated during operation.Here,we investigated the size distribution,chemical composition,and charged fraction of aerosol particles emitted from commercial ultrasonic humidifiers.Heavy metals in water used for humidifiers were found to be highly enriched in the ultrasonic humidifier aerosols(UHA),with the enrichment factors ranging from 102 to 107.This enrichment may pose health concerns for the building occupants,as UHA concentrations of up to 106 particles/cm^(3) or 3 mg/m^(3) were observed.Furthermore,approximately 90%of UHA were observed to be electrically charged,for the first time according to our knowledge.Based on this discovery,we proposed and tested a newmethod to remove UHA by using a simple electrical field.The designed electrical field in this work can efficiently remove 81.4%of UHA.Therefore,applying this electrical field could be an effective method to significantly reduce the health risks by UHA.
文摘Objective:To explore nursing measures for elderly patients with chronic obstructive pulmonary disease(COPD)and analyze the effect of continuous nursing pathways on improving the accuracy of aerosol use.Methods:From April 2023 to April 2024,76 elderly COPD patients admitted to our hospital were randomly selected for nursing research.They were divided into two groups using a computer double-blind method,with 38 patients in each group.The control group received routine nursing,while the observation group applied the continuous nursing pathway.The nursing effects of the two groups were investigated and compared,including(1)aerosol accuracy;(2)cardiopulmonary function;(3)subjective well-being and self-care ability;(4)quality of life;and(5)nursing satisfaction.Results:Compared with the control group,the observation group had a significantly higher accuracy rate of aerosol use(P<0.05).Before nursing,there were no significant differences in cardiopulmonary function indicators,MUNSH scores,and ESCA scores between the two groups(P>0.05).After nursing,the patient's cardiopulmonary function improved significantly,and their subjective well-being and self-care ability increased.The observation group was significantly better than the control group in all the above indicators(P<0.05).The quality of life scores of the observation group were significantly higher than those of the control group(P<0.05).Conclusion:In the nursing of elderly patients with chronic obstructive pulmonary disease,the application of the continuous nursing pathway can effectively improve the accuracy of aerosol use and improve patients'cardiopulmonary function.
基金supported by the National Natural Science Foundation of China(No.31700475).
文摘Aerosol particle pollution has become an increasing serious environmental problem,and urban vegetation plays a long-lasting and positive role in mitigating it.This study compared the particle capture abilities of trees,shrubs,and herbs,and examined the compositions and influence of aerosol particles accumulated on leaf functional traits.Retained particles primarily contained Ca^(2+),K^(+),SO_(4)^(2-),NO_(3)^(-)and NH_(4)^(+),indicating their anthropogenic origins.The leathery-leaved tree Osmanthus fragrans and the papery-leaved herb Alternanthera sessilis demonstrated the higher competence in particle accumulation than other plants,and leaf morphologic structures(e.g.,leaf grooves,trichomes,waxy layers,and stomata characteristics)were closely associated with particle capture by plant species.Particle retention negatively impacted stomata,impeding photosynthesis,and reducing transpiration.In response to particle accumulation,plants tended to decrease specific leaf area and adjust stomatal conductance.Both growth form and leaf texture significantly influenced the particle capture abilities of different plant species.The substantial contribution of plants,particularly herbs in the lower vegetation strata,to particle removal should not be overlooked.Vegetation with a tree-shrub-herb configuration excels at particle capture,offering potential advantages in mitigating particle pollution and enhancing ecological benefits.
基金supported by the National Key Research and Development Program of China (Grant No. 2023YFC3706203)the National Natural Science Foundation of China (Grant Nos. 91644214, 22361162668, and 22406109)+1 种基金the China Postdoctoral Science Foundation (Grant No. 2024M751797)Shandong Postdoctoral Science Foundation (SDCX-ZG-202400178)
文摘Enhanced mass concentrations of aromatic-derived secondary organic aerosol(SOA)are frequently observed during humid-haze events.However,the influencing mechanism of relative humidity(RH)in aromatic-derived SOA formation remains incompletely understood.Here,the RH dependence of SOA formation in the presence of NOx was explored by a series of chamber experiments for toluene(TOL)and 1,3,5-trimethylbenzene(TMB)photooxidation.The yield of TOL SOA and TMB SOA increased by 221%and 52%with increasing RH from~8%to~70%,respectively.Analytical results from a high-resolution mass spectrometer showed that SOA constituents with high oxygen content(O/C>0.6)were more abundant in SOA formed in the~70%RH experiment.The elevated yields and O/C of SOA could be attributed to the promoted formation and particle-phase diffusivity of highly oxidized molecules.In addition,in comparison with TMB,TOL could produce more unsaturated aldehydes,which are oxidized into carboxylic acids with high O/C,leading to a more sensitive response of TOL SOA formation to the change in RH.Our work provides mechanistic insights into RH roles in aromatic SOA formation and is helpful for a better understanding of humid-haze events.
基金supported by the National Natural Science Foundation of China(Nos.42076205 and 42376195).
文摘We conducted a comprehensive analysis of seasonal and long-term variations in organic carbon(OC),elemental carbon(EC),primary organic carbon(POC),and secondary organic carbon(SOC)among total suspended particles on Huaniao Island,China,from 2011 to 2020.The highest OC and EC concentrations were observed in 2014(OC,4.13μg/m^(3))and 2013(EC,1.21μg/m^(3)),respectively;for both,the lowest concentrations occurred in 2017(OC,1.56μg/m^(3);EC,0.69μg/m^(3)).OC and EC exhibited seasonal variations,such that the highest and lowest values for both occurred in winter and summer,respectively;particularly high concentrations were observed in the winter of 2014 on Huaniao Island.By 2020,winter OC and EC concentrations had decreased by 43%and 36%,whereas autumn OC and EC concentrations increased by 38%and 160%compared with 2014.In terms of carbon components,the proportions of OC4 and EC1 significantly declined,whereas the proportions of OC3 and OC2 increased,during the study period.Higher POC and SOC concentrations were mainly observed during the autumn–winter and winter–spring transition periods.POC was most strongly correlated with OC2,followed by OC4 and EC1.SOC was strongly correlated with OC3,especially in winter.These findings highlight the characteristics of temporal variations in individual carbon components,as well as possible associations with POC and SOC.
基金supported by the Basic Research Key Project of Science and Technology Department of Yunnan Province(No.202401AS070116)the National Natural Science Foundation of China(No.21966016)。
文摘Biomass burning(BB)emits carbonaceous aerosols that significantly influence air quality in Southwest China during spring.To further understand the characteristics of spring BB and its original contribution to organic carbon(OC),daily fine particulate matter(PM_(2.5))samples were collected from March to May 2022 in Pu'er,Southwest China.The concentrations of OC,elemental carbon(EC),levoglucosan(Lev),and potassium from BB(K+BB)during the study period ranged from 5.3 to 31.2μg/m^(3),0.86-13.1μg/m^(3),0.06-0.82μg/m^(3),and 0.05-2.88μg/m^(3),respectively.To eliminate the effects of Lev degradation,this study uses the Aging of Air Mass(AAM)index to correct the atmospheric concentration of Lev and combines Bayesian mixture modeling with a molecular tracer method to assess the original contribution of BB to OC.The results indicated that the AAM index was 0.18±0.05,indicating that the degradation of Lev reached 82%.When considering the degradation of levoglucosan in the atmosphere,the primary source of BB aerosols was crop-straw combustion(71.1%),followed by the combustion of certain hardwoods and softwoods(24.9%)and grasses(4.0%).The original contribution of BB to OC was 62.4%,which was much greater than the contribution when levoglucosan degradation(23.7%)was ignored.The air mass inverse trajectories and Moderate Resolution Imaging Spectroradiometer(MODIS)fire hotspots indicated that the BB plume from Southeast Asia during spring could influence PM_(2.5)long-range transport in remote locations,and the contribution could reach 82%in Southwest China.
基金supported by the National Natural Science Foundations of China(Grant Nos.42305163 and U22A20577)the Construction Project of Weather Modification Ability in Central China(Grant No.ZQC-H22256)+2 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB0760300)the Projects of the Earth System Numerical Simulation Facility(Grant Nos.2024-EL-PT-000707,2023-ELPT-000482,2023-EL-ZD-00026,and 2022-EL-PT-00083)the STS Program of the Inner Mongolia Meteorological Service,Chongqing Institute of Green and Intelligent Technology,Chinese Academy of Sciences,and Institute of Atmospheric Physics,Chinese Academy of Sciences(Grant No.2021CG0047)。
文摘Accurate descriptions of cloud droplet spectra from aerosol activation to vapor condensation using microphysical parameterization schemes are crucial for numerical simulations of precipitation and climate change in weather forecasting and climate prediction models.Hence,the latest activation and triple-moment condensation schemes were combined to simulate and analyze the evolution characteristics of a cloud droplet spectrum from activation to condensation and compared with a high-resolution Lagrangian bin model and the current double-moment condensation schemes,in which the spectral shape parameter is fixed or diagnosed by an empirical formula.The results demonstrate that the latest schemes effectively capture the evolution characteristics of the cloud droplet spectrum during activation and condensation,which is in line with the performance of the bin model.The simulation of the latest activation and condensation schemes in a parcel model shows that the cloud droplet spectrum gradually widens and exhibits a multimodal distribution during the activation process,accompanied by a decrease in the spectral shape and slope parameters over time.Conversely,during the condensation process,the cloud droplet spectrum gradually narrows,resulting in increases in the spectral shape and slope parameters.However,these double-moment schemes fail to accurately replicate the evolution of the cloud droplet spectrum and its multimodal distribution characteristics.Furthermore,the latest schemes were coupled into a 1.5D cumulus model,and an observation case was simulated.The simulations confirm that the cloud droplet spectrum appears wider at the supersaturated cloud base and cloud top due to activation,while it becomes narrower at the middle altitudes of the cloud due to condensation growth.
基金supported by the State Key Program of the National Natural Science Foundation of China(Grant Nos.42230701,91644215)the National Natural ScienceFoundation of China(Grant Nos.42122062 and 42307137)+3 种基金the Guangdong Basic and Applied Basic Research Foundation(Grant No.2022A1515010852)the Fundamental Research Funds for the Central Universities,Sun Yat-sen University(Grant No.23hytd002)the Southern Marine Science and Engineering Guangdong Laboratory(Zhuhai)(Grant No.SML2023SP218)L.M.acknowledges the Zhuhai Science and Technology Plan Project(Grant No.ZH22036201210115PWC).
文摘The compositions and distributions of monoterpenes,isoprene,aromatics and sesquiterpene SOA tracers(SOAM,SOAI,SOAA and SOAS,respectively)at an island site(Da Wan Shan Island,DWS)were investigated in the context of the influence of continental and marine air masses over the Pearl River Estuary(PRE)region in winter 2021.The sum concentration of SOA tracers was 6.2–132.8 ng m^(−3),with SOAM and SOAI as the main components in both continental(scenarios A1 and A2)and marine air masses(scenario A3),as well as their combination(scenario A4).The highest and lowest levels of SOAM were observed in A1 and A3,respectively,which were mainly related to the variations in meteorological conditions,precursor concentrations,and the degree of photochemical processes.Higher MBTCA/HGA(3-methyl-1,2,3-butanetricarboxylic acid/3-hydroxyglutaric acid)ratios suggested a less significant contribution fromα-pinene to SOAM.The variations of SOAI in the different scenarios were associated with differences in relative humidity,particle acidity,and isoprene/NOx ratios.The respective highest and lowest concentrations of aromatics SOA tracers in A1 and A3 revealed the influence of anthropogenic precursors from upwind continental areas,which was confirmed by the correlation among biogenic and anthropogenic precursors.The results of the tracer-based-method suggested dominant contributions of SOAs from aromatics and monoterpenes,with the highest concentrations in A1.A WRF-Chem simulation revealed that the SOAs from the above precursors only contributed 12%–25%to the total SOA at DWS,while the spatial distributions of SOAs further highlighted that the abundance of SOAs over the PRE region in winter is highly associated with air masses transported from upwind continental areas.
基金supported by the National Natural Science Foundation of China(Nos.92361302,22125303,92061203,and 22288201)the National Key Research and Development Program of China(No.2021YFA1400501)+2 种基金the Innovation Program for Quantum Science and Technology(No.2021ZD0303304)Dalian Institute of Chemical Physics(No.DICP DCLS201702)Chinese Academy of Sciences(No.GJJSTD20220001).
文摘Elucidating the mutual effects between the different volatile organic compounds(VOCs)is crucial for comprehending the formation mechanism of atmospheric secondary organic aerosols(SOA).Here,the mixed VOCs experiments of isoprene and△^(3)-carene/β-caryophyllene were carried out in the presence of O_(3)using an indoor smog chamber.The suppression effect of isoprene was recognized by the scanning mobility particle sizer spectrometer,online vacuum ultraviolet free electron laser(VUV-FEL)photoionization aerosol mass spectrometry,and quantum chemical calculations.The results indicate that the suppression effect of isoprene on the ozonolysis of△^(3)-carene andβ-caryophyllene shows fluctuating and monotonous trends,respectively.The carbon content of the precursor could be themain factor for regulating the strength of the suppression effect.Plausible structures and formation mechanisms of several new products generated from the single VOC precursor and VOC-cross-reaction are proposed,which enrich the category of VOC oxidation products.Meanwhile,a new dimerization mechanism of the RO_(2)+R’O_(2)reaction is suggested,which offers an intriguing perspective on the gas phase formation process of particle phase accretion products.The present findings provide valuable insights into clarifying the pivotal roles played by isoprene in the interplay between different VOCs and understanding of SOA formation mechanisms of VOC mixtures,especially nearby the emission origins.
