Laser-induced aerosols,predominantly submicron in size,pose significant environmental and health risks during the decommissioning of nuclear reactors.This study experimentally investigated the removal of laser-generat...Laser-induced aerosols,predominantly submicron in size,pose significant environmental and health risks during the decommissioning of nuclear reactors.This study experimentally investigated the removal of laser-generated aerosol particles using a water spray system integrated with an innovative system for pre-injecting electrically charged mist in our facility.To simulate aerosol generation in reactor decommissioning,a high-power laser was used to irradiate various materials(including stainless steel,carbon steel,and concrete),generating aerosol particles that were agglomerated with injected water mist and subsequently scavenged by water spray.Experimental results demonstrate enhanced aerosol removal via aerosol-mist agglomeration,with charged mist significantly improving particle capture by increasing wettability and size.The average improvements for the stainless steel,carbon steel,and concrete were 40%,44%,and 21%,respectively.The results of experiments using charged mist with different polarities(both positive and negative)and different surface coatings reveal that the dominant polarity of aerosols varies with the irradiated materials,influenced by their crystal structure and electron emission properties.Notably,surface coatings such as ZrO_(2)and CeO_(2)were found to possibly alter aerosol charging characteristics,thereby affecting aerosol removal efficiency with charged mist configurations.The innovative aerosol-mist agglomeration approach shows promise in mitigating radiation exposure,ensuring environmental safety,and reducing contaminated water during reactor dismantling.This study contributes critical knowledge for the development of advanced aerosol management strategies for nuclear reactor decommissioning.The understanding obtained in this work is also expected to be useful for various environmental and chemical engineering applications such as gas decontamination,air purification,and pollution control.展开更多
The relative dispersion of cloud and fog droplets has significant impacts on aerosol indirect effects,radiative transfer,and microphysical processes.However,previous studies have been mostly concerned with clouds,with...The relative dispersion of cloud and fog droplets has significant impacts on aerosol indirect effects,radiative transfer,and microphysical processes.However,previous studies have been mostly concerned with clouds,with limited studies on fog,particularly those that examine the combined influences of all key physical processes and their roles during fog evolution.As such,this study aims to conduct a comprehensive investigation by examining the relationships between relative dispersion and other microphysical variables,as well as the underlying microphysical and dynamic processes,based on field fog campaigns in polluted and clean conditions.In polluted fog,droplet concentrations are higher,leading to smaller droplets and increased dispersion.The correlation between dispersion and droplet volume-mean radius is positive in the polluted fog,but shifts to negative in clean fog.We attribute the difference to various microphysical processes like aerosol activation,condensation,collision-coalescence,and entrainment-mixing.In polluted fog,high aerosol concentrations,low supersaturations,and strong turbulence(entrainment-mixing)provide suitable conditions for the simultaneous occurrence of droplet condensation and aerosol activation,resulting in a positive correlation between dispersion and volume-mean radius,especially during the fog formation stage.In contrast,during the mature stage in clean fog,condensation is dominant with weak aerosol activation leading to a negative correlation between relative dispersion and volume-mean radius.The collision-coalescence process is more active in the mature stage,increasing radii and leading to the negative correlation between dispersion and volume-mean radius.This result sheds new light on understanding the relative dispersion and mechanisms in fog under different aerosol backgrounds.展开更多
Along with decrease of fine particulate matter(PM_(2.5))concentration in recent years in China,secondary species become increasingly important.This work focuses on characterizing secondary components,and a few importa...Along with decrease of fine particulate matter(PM_(2.5))concentration in recent years in China,secondary species become increasingly important.This work focuses on characterizing secondary components,and a few important groups of organics including organic nitrogen(ON),organonitrates(OrgN),organosulfates(OS)and polycyclic aromatic hydrocarbons(PAHs),via online measurement of submicron aerosols(PM_(1))in Nanjing,China,during 2022 summer.The average PM_(1) concentration was 15.39μg/m^(3),dominated by secondary components(69.1%),which were even more important at higher PM_(1) levels.The primary organic aerosols(POA)were from traffic,industry and cooking;the two secondary OA factors were both closely linked with photochemistry,with one(OOA1)being relatively fresh and important in early afternoon and another(OOA2)being aged and important in late afternoon.Sulfate formation was also governed by photochemistry but resembled that of OOA2 not OOA1;nitrate formation was associated strongly with heterogeneous hydrolysis and thermodynamic equilibrium.Results also reveal a possible photochemical reaction channel from POA to OOA1,then to OOA2.Case studies show that formations of secondary components responded differently to different weather conditions and governed summer PM_(1) pollution.The average ON,OrgN,OS and PAHs concentrations were determined to be 122.8,84.4,45.6 and 3.3 ng/m^(3),respectively.ON was dominated by primary sources(53.8%).OrgN varied similarly to nitrate.OS formation was linked with aqueous-phase reactions,which were insignificant therefore its level was low.PAHs was mainly from traffic,and photochemical oxidation might be its important sink during afternoon.展开更多
Temperature has a substantial impact on the emission of biogenic volatile organic compounds(BVOCs).Moder-ate warm temperatures,e.g.,30–40°C,could boost plant metabolism,increasing BVOC emissions.Against the back...Temperature has a substantial impact on the emission of biogenic volatile organic compounds(BVOCs).Moder-ate warm temperatures,e.g.,30–40°C,could boost plant metabolism,increasing BVOC emissions.Against the backdrop of global warming,plants emit more BVOCs to cope with thermal stress,leading to elevated concen-trations of tropospheric ozone(O_(3))and secondary organic aerosols(SOA).In recent years,a considerable body of research has explored the interaction between tree species and BVOCs under the influence of various environ-mental factors.Although many studies have examined explored the temperature dependence of BVOC emissions in the past,few studies have conducted a comprehensive and in-depth investigation into the impacts of tempera-ture.This review summarizes the relevant studies on BVOCs in the past decade,including the main biosynthetic pathways,emission observation techniques and emission inventories,as well as how temperature affects isoprene and monoterpene emission rates and the formation of O_(3) and SOA.Our work offers a theoretical foundation and guidance for future efforts to advance the comprehension of BVOC emission characteristics and develop strategies to mitigate secondary pollution.展开更多
The January 2022 eruption of Hunga injected unprecedented volumes of water vapor(150 Tg)and modest sulfur dioxide(SO_(2))into the stratosphere,producing accelerated sulfate aerosol formation in the early plume.As the ...The January 2022 eruption of Hunga injected unprecedented volumes of water vapor(150 Tg)and modest sulfur dioxide(SO_(2))into the stratosphere,producing accelerated sulfate aerosol formation in the early plume.As the aerosols gradually spread into the global stratosphere,the role of water vapor,among other factors in the spread and residence time of the sulfate aerosols,remained unclear.We used multisatellite observations to better understand the role of water vapor in the spread and lifetime of Hunga volcanic aerosols.Stratospheric circulation transported the plumes to~26 km within the polar vortices-the Antarctic by August 2022 and the Arctic by January 2023-with the arrival of aerosols lagging behind that of water vapor by months.Even though high injection altitudes(58 km)and strong Brewer-Dobson circulation contributed to prolonging the residence time of aerosols,the water vapor enhanced particle growth and thus accelerated gravitational settling,with the half lifetime of aerosols being 14 months.Our analysis revealed a critical trade-off:after the eruption of the Hunga volcano,an extremely high injection height and strong upward motion slowed the removal of aerosols,but extreme water vapor loading still had a certain impact on the half lifetime of the aerosols.These findings highlight the role of water vapor in the persistence of aerosols from submarine eruptions.展开更多
To elucidate the dispersion and explosion characteristics of multi-metal powder and liquid composite fuel formulations,high-energy metal powders(aluminum(Al),boron(B),and magnesium hydride(MgH_(2)))are incorporated in...To elucidate the dispersion and explosion characteristics of multi-metal powder and liquid composite fuel formulations,high-energy metal powders(aluminum(Al),boron(B),and magnesium hydride(MgH_(2)))are incorporated into a liquid fuel primarily composed of diethyl ether(DEE)and isopropyl nitrate(IPN).The explosion characteristics of different solid-liquid fuel-air-explosive(FAE)under unconfined conditions are investigated using a high-speed camera,infrared thermal imaging,and a pressure measurement system.Results demonstrate that high-energy metal powders significantly enhance detonation energy dissipation,with aluminum exhibiting the most pronounced effect.Fuel 5#(45.4 wt%DEE,9.2 wt%IPN,29.5 wt%Al,9.1 wt%B,6.8 wt%MgH_(2))exhibits superior explosion performance,achieving higher values of overpressure,impulse,and thermal radiation damage during the detonation stage compared to other fuels.However,Fuel 5#also displays faster decay rates,attributed to accelerated heat release rates induced by B and MgH_(2)powders.This study reveals that different metal powders in solid-liquid FAE exhibit distinct enhancements in explosion performance,providing critical insights for optimizing composite fuel design.展开更多
Imidazole(IM)particles in the atmosphere affect climate,atmospheric chemical reactions,and human health.However,research on IM particles in the Sichuan Basin(SCB),one of the areas of China affected most heavily by haz...Imidazole(IM)particles in the atmosphere affect climate,atmospheric chemical reactions,and human health.However,research on IM particles in the Sichuan Basin(SCB),one of the areas of China affected most heavily by haze,remains very scarce.This study used single-particle aerosol mass spectrometry to investigate IM-containing particles in Chengdu,one of the megacities in the SCB,during summer and winter before and after implemen-tation of the Three-year Action Plan to Win the Blue-Sky Defense War(BSDW).We found that IM-containing particles accounted for 1.2%–12.0%of all detected particles,and they highly mixed with carbonaceous com-ponents,secondary inorganic species,and organic nitrogen.From before to after the BSDW,the proportion of IM-containing particles decreased by 1.8%in summer,but increased by 9.6%in winter.Ammonium/amines and carbonyl compounds were closely related to IM-containing particles;the highest proportion of IM-containing particles occurred in particles mixed with amines and carbonyls.The number fraction of IM-containing particles in all seasons was higher at night than during daytime.The potential source areas of IM-containing particles showed notable narrowing after the BSDW,and the high-value areas were found distributed closer to Chengdu and its surrounding areas.In the winter before the BSDW,most IM-containing particles(>70%)were mixed with organic carbon(OC)particles,and the contributions of OC and mixed organic–elemental carbon(OC-EC)particles increased with aggravation of pollution,whereas OC-EC and Metal particles played a more crucial role in the winter after the BSDW.展开更多
Worldwide radiation records suggest that the amount of sunlight received at the Earth's surface(surface solar radiation, SSR) has not been stable over the years, but underwent significant decadal variations, popul...Worldwide radiation records suggest that the amount of sunlight received at the Earth's surface(surface solar radiation, SSR) has not been stable over the years, but underwent significant decadal variations, popularly also known as “global dimming and brightening”. These variations have been particularly evident in China, where the SSR substantially declined from the 1960s to the 1990s(dimming), with indications for a trend reversal in the 2000s and a slight recovery(brightening) in recent years. This perspective/review paper will discuss recent updates and remaining challenges regarding our knowledge of the magnitudes, causes, and implications of these variations in SSR worldwide, with a particular emphasis on the developments in China.展开更多
We present a comprehensive description and benchmark evaluation of the global–regional chemical transport model called the Emission and Atmospheric Processes Integrated and Coupled Community(EPICC)model.The framework...We present a comprehensive description and benchmark evaluation of the global–regional chemical transport model called the Emission and Atmospheric Processes Integrated and Coupled Community(EPICC)model.The framework incorporates(1)grid configuration,(2)transport dynamics,(3)chemical mechanisms,(4)aerosol processes,(5)wet/dry deposition parameterizations,and(6)heterogeneous chemistry treatments associated with sulfate,nitrous acid(HONO)chemistry,and aerosol/cloud–photolysis interactions(APIs/CPIs).Openly shared with the atmospheric research community,the model facilitates integration of advanced physicochemical schemes to enhance simulation accuracy.Globally,the model demonstrates realistic representations of ozone(O_(3))and aerosol optical depth.The EPICC model generally demonstrates robust performance in simulating regional concentrations of O_(3) and PM_(2.5)(and its components)in China.It successfully captures vertical profiles of both global and regional O_(3).Notably,the model mitigates frequently reported sulfate underestimations in highly industrialized regions of China.The model accurately captures two regional severe pollution episodes observed in eastern China(January/June 2021).Sensitivity experiments highlight the critical roles of heterogeneous chemical mechanisms associated with sulfate,HONO chemistry,APIs,and CPIs in capturing PM_(2.5) and O_(3) concentrations in China.Improved sulfate mechanisms result in an increase of approximately 32.4%(2.8μg m^(−3))in simulated winter sulfate concentrations when observations exceed 10μg m^(−3).Enhanced HONO elevates winter O_(3) and PM_(2.5) by≤20 and≤10μg m^(−3),respectively.Overall,CPIs dominate over APIs in improving O_(3) and PM_(2.5) simulations across China.Locally,APIs mitigate PM_(2.5) and O_(3) discrepancies in the Sichuan Basin.Seasonal cloud–chemistry coupling explains the weaker impact of PM_(2.5) in summer.展开更多
Smoke generator constitute an important class of pesticide formulations widely used in protected agriculture,forestry,mushroom cultivation,and storage environments.Unlike conventional sprays,smoke generator rely on he...Smoke generator constitute an important class of pesticide formulations widely used in protected agriculture,forestry,mushroom cultivation,and storage environments.Unlike conventional sprays,smoke generator rely on heat-induced phase transitions of active ingredients to produce fine aerosolized particles that disperse through Brownian motion,thereby markedly improving application efficiency.Despite their long history and broad utility,the development of smoke generator has largely stagnated over the past two decades.Here,we provide a comprehensive assessment of their historical evolution,registration landscape,physicochemical mechanisms,and current deployment in agricultural systems.Based on this analysis,we outline key directions for nextgeneration smoke generator technology.First,transitioning from chemical heating to electric heating is essential to enable automation and unmanned pesticide delivery.Second,expanding the air-purification functionality of smoke formulations offers a promising strategy to suppress airborne pest and pathogen populations.Finally,integrating principles of crystal engineering to modulate particle morphology and interfacial affinity may overcome current limitations in deposition efficiency and biological performance.Together,these advances will underpin the development of high-efficiency,intelligent smoke generator and support precision plant protection and sustainable intensification in protected agriculture.展开更多
In winter 2018,an aerosol physicochemical experiment was conducted in the Western Pacific Ocean(WPO)aboard the Research Vessel KEXUE of Chinese Academy of Sciences.This study systematically investigated both natural a...In winter 2018,an aerosol physicochemical experiment was conducted in the Western Pacific Ocean(WPO)aboard the Research Vessel KEXUE of Chinese Academy of Sciences.This study systematically investigated both natural and anthropogenic effects on marine aerosols optical properties,as well as the applicability of multi-satellite products and IMPROVE equation.The averaged aerosol optical depth(AOD500 nm)was 0.31±0.16 andÅngström exponent440–675 nm was 0.29±0.30.In offshore China,significant anthropogenic emissions affected the marine environment.In remote WPO,dust aerosols transported from northern China,Siberia,Central Asia,and those settling from the upper troposphere originating from north Africa,Arabian peninsula,and western India,were dominant.The spatial trends of AOD were opposite in the mid-latitude and southern seas of WPO.The highest AOD,0.32±0.23,appeared along the coast of South Asia at mid-latitude,decreasing from offshore seas to remote oceans.In low-latitude and equatorial seas,AOD significantly increased from coast to remote oceans.Ångström exponent dropped significantly from the coast to remote oceans as anthropogenic influence diminished across the entire WPO.Correlation analysis showed that both MODIS-C6 and Himawari AOD prod-ucts showed similar applicability in coastal urban areas,while Himawari AOD is highly recommended for coastal background and marine environment due to its finer resolution.The extinction coefficient derived from PM_(2.5) chemical compositions using IMPROVE algorithm exhibited a significant correlation(R^(2)=0.58)with the con-currently measured AOD in the absence of long-distance transport,suggesting that the IMPROVE is a reasonable proxy of the columnar average of marine aerosol extinctions free from transport influences.展开更多
Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previo...Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previous research,providing a long-term perspective on carbonyl compound variations and their environmental implica-tions.Atmospheric observations were conducted at Beijing(BJ)and Xianghe(XH)during the summer and winter months of 2018,2019,and 2023 to study the sources and impacts of carbonyl compounds in typical urban areas and peri‑urban areas.Notably,concentrations in the summer of 2023 increased compared to 2018 and 2019.The predominant carbonyl compounds—formaldehyde,acetaldehyde,and acetone—accounted for over 60%of the total.The mean values of OFP in BJ ranged from 18.55 to 58.61μg/m3,lower than those in XH(29.82 to 65.48μg/m3),with formaldehyde and acetaldehyde contributing over 80%of the total.SOAP exhibited a similar pattern,with values in XH(69.21 to 508.55μg/m3)significantly exceeding those in BJ(34.47 to 159.78μg/m3).The PMF model highlighted vehicle exhaust,secondary pollution,and biomass combustion as major sources of carbonyl compounds,emphasizing differences in source contributions between the two regions.This study’s com-parative analysis over different years and locations provides new insights into the dynamic changes in carbonyl compounds and their environmental importance.These results not only reinforce the importance of carbonyl compounds regulation but also offer a valuable reference for evaluating and refining emission control strategies during this period.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
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
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
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 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
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 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
Nitrate renoxification significantly influences atmospheric nitrogen cycling and global OH budgets.Although numerous nitrite acid(HONO)formation pathways from nitrate photolysis have been widely reported,the influence...Nitrate renoxification significantly influences atmospheric nitrogen cycling and global OH budgets.Although numerous nitrite acid(HONO)formation pathways from nitrate photolysis have been widely reported,the influence of various environmental factors and aerosol properties on reactive nitrogen production remains largely unclear.In this work,we employed NaNO_(3)/humic acid(HA)as a model nitrate photosensitization system to investigate the crucial roles of aerosol acidity,organic fraction,and dissolved oxygen in the production of HONO,NO_(2),and NO_(2)^(-).The presence of HA at 10 mg/L resulted in a remarkable increase in HONO production rates by approximately 2–3 times and NO_(2)^(-) concentration by 3–6 times across a pH range of 5.2 to 2.0.Meanwhile,the molar fraction of gaseous HONO in total N(Ⅲ)production increased from4%to 69%as bulk-phase pH decreased from 5.2 to 2.0.The higher organic fraction(i.e.,20 and 50 mg/L HA concentration)instead inhibited HONO and NO_(2) release.The presence of dissolved oxygen was found to be adverse for reactive nitrogen production.This suggests that the HA photosensitizer promoted the secondary conversion of NO_(2) to HONO mainly via reduced ketyl radical intermediates,while superoxide radical formation might exert a negative effect.Our findings provide comprehensive insights into reactive nitrogen production from photosensitized nitrate photolysis mediated by various external and internal factors,potentially accounting for discrepancies between field observations and model simulations.展开更多
基金financial support from the Nuclear Energy Science&Technology and Human Resource Development Project of the Japan Atomic Energy Agency/Collaborative Laboratories for Advanced Decommissioning Science(No.R04I034)The author Ruicong Xu appreciates the scholarship(financial support)from the China Scholarship Council(CSC,No.202106380073).
文摘Laser-induced aerosols,predominantly submicron in size,pose significant environmental and health risks during the decommissioning of nuclear reactors.This study experimentally investigated the removal of laser-generated aerosol particles using a water spray system integrated with an innovative system for pre-injecting electrically charged mist in our facility.To simulate aerosol generation in reactor decommissioning,a high-power laser was used to irradiate various materials(including stainless steel,carbon steel,and concrete),generating aerosol particles that were agglomerated with injected water mist and subsequently scavenged by water spray.Experimental results demonstrate enhanced aerosol removal via aerosol-mist agglomeration,with charged mist significantly improving particle capture by increasing wettability and size.The average improvements for the stainless steel,carbon steel,and concrete were 40%,44%,and 21%,respectively.The results of experiments using charged mist with different polarities(both positive and negative)and different surface coatings reveal that the dominant polarity of aerosols varies with the irradiated materials,influenced by their crystal structure and electron emission properties.Notably,surface coatings such as ZrO_(2)and CeO_(2)were found to possibly alter aerosol charging characteristics,thereby affecting aerosol removal efficiency with charged mist configurations.The innovative aerosol-mist agglomeration approach shows promise in mitigating radiation exposure,ensuring environmental safety,and reducing contaminated water during reactor dismantling.This study contributes critical knowledge for the development of advanced aerosol management strategies for nuclear reactor decommissioning.The understanding obtained in this work is also expected to be useful for various environmental and chemical engineering applications such as gas decontamination,air purification,and pollution control.
基金supported by the Chinese National Natural Science Foundation under Grant Nos.(41975181,42325503,42375197,42575207,42205090)Y.LIU is supported by the U.S.Department of Energy’s Atmospheric System Research(ASR)program.
文摘The relative dispersion of cloud and fog droplets has significant impacts on aerosol indirect effects,radiative transfer,and microphysical processes.However,previous studies have been mostly concerned with clouds,with limited studies on fog,particularly those that examine the combined influences of all key physical processes and their roles during fog evolution.As such,this study aims to conduct a comprehensive investigation by examining the relationships between relative dispersion and other microphysical variables,as well as the underlying microphysical and dynamic processes,based on field fog campaigns in polluted and clean conditions.In polluted fog,droplet concentrations are higher,leading to smaller droplets and increased dispersion.The correlation between dispersion and droplet volume-mean radius is positive in the polluted fog,but shifts to negative in clean fog.We attribute the difference to various microphysical processes like aerosol activation,condensation,collision-coalescence,and entrainment-mixing.In polluted fog,high aerosol concentrations,low supersaturations,and strong turbulence(entrainment-mixing)provide suitable conditions for the simultaneous occurrence of droplet condensation and aerosol activation,resulting in a positive correlation between dispersion and volume-mean radius,especially during the fog formation stage.In contrast,during the mature stage in clean fog,condensation is dominant with weak aerosol activation leading to a negative correlation between relative dispersion and volume-mean radius.The collision-coalescence process is more active in the mature stage,increasing radii and leading to the negative correlation between dispersion and volume-mean radius.This result sheds new light on understanding the relative dispersion and mechanisms in fog under different aerosol backgrounds.
基金supported by the National Natural Science Foundation of China(Nos.22361162668 and 42021004)the National Key Research and Development Program of China(No.2023YFC3706203).
文摘Along with decrease of fine particulate matter(PM_(2.5))concentration in recent years in China,secondary species become increasingly important.This work focuses on characterizing secondary components,and a few important groups of organics including organic nitrogen(ON),organonitrates(OrgN),organosulfates(OS)and polycyclic aromatic hydrocarbons(PAHs),via online measurement of submicron aerosols(PM_(1))in Nanjing,China,during 2022 summer.The average PM_(1) concentration was 15.39μg/m^(3),dominated by secondary components(69.1%),which were even more important at higher PM_(1) levels.The primary organic aerosols(POA)were from traffic,industry and cooking;the two secondary OA factors were both closely linked with photochemistry,with one(OOA1)being relatively fresh and important in early afternoon and another(OOA2)being aged and important in late afternoon.Sulfate formation was also governed by photochemistry but resembled that of OOA2 not OOA1;nitrate formation was associated strongly with heterogeneous hydrolysis and thermodynamic equilibrium.Results also reveal a possible photochemical reaction channel from POA to OOA1,then to OOA2.Case studies show that formations of secondary components responded differently to different weather conditions and governed summer PM_(1) pollution.The average ON,OrgN,OS and PAHs concentrations were determined to be 122.8,84.4,45.6 and 3.3 ng/m^(3),respectively.ON was dominated by primary sources(53.8%).OrgN varied similarly to nitrate.OS formation was linked with aqueous-phase reactions,which were insignificant therefore its level was low.PAHs was mainly from traffic,and photochemical oxidation might be its important sink during afternoon.
基金supported by the National Key R&D Program of China(No.2024YFC3714200)Guangxi Key Research and Development Program,China(No.Guike AB24010074)+2 种基金the National Natural Science Foundation of China(Nos.22276099,U24A20515 and 22361162668)the Natural Science Foundation of Jiangsu Province(No.BK20240036)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX24_1529).
文摘Temperature has a substantial impact on the emission of biogenic volatile organic compounds(BVOCs).Moder-ate warm temperatures,e.g.,30–40°C,could boost plant metabolism,increasing BVOC emissions.Against the backdrop of global warming,plants emit more BVOCs to cope with thermal stress,leading to elevated concen-trations of tropospheric ozone(O_(3))and secondary organic aerosols(SOA).In recent years,a considerable body of research has explored the interaction between tree species and BVOCs under the influence of various environ-mental factors.Although many studies have examined explored the temperature dependence of BVOC emissions in the past,few studies have conducted a comprehensive and in-depth investigation into the impacts of tempera-ture.This review summarizes the relevant studies on BVOCs in the past decade,including the main biosynthetic pathways,emission observation techniques and emission inventories,as well as how temperature affects isoprene and monoterpene emission rates and the formation of O_(3) and SOA.Our work offers a theoretical foundation and guidance for future efforts to advance the comprehension of BVOC emission characteristics and develop strategies to mitigate secondary pollution.
基金funding from the National Natural Science Foundation of China(Grant Nos.U2442210 and 42275059)supported by funding from Chengdu University of Information Technology(Grant No.X202310621039).
文摘The January 2022 eruption of Hunga injected unprecedented volumes of water vapor(150 Tg)and modest sulfur dioxide(SO_(2))into the stratosphere,producing accelerated sulfate aerosol formation in the early plume.As the aerosols gradually spread into the global stratosphere,the role of water vapor,among other factors in the spread and residence time of the sulfate aerosols,remained unclear.We used multisatellite observations to better understand the role of water vapor in the spread and lifetime of Hunga volcanic aerosols.Stratospheric circulation transported the plumes to~26 km within the polar vortices-the Antarctic by August 2022 and the Arctic by January 2023-with the arrival of aerosols lagging behind that of water vapor by months.Even though high injection altitudes(58 km)and strong Brewer-Dobson circulation contributed to prolonging the residence time of aerosols,the water vapor enhanced particle growth and thus accelerated gravitational settling,with the half lifetime of aerosols being 14 months.Our analysis revealed a critical trade-off:after the eruption of the Hunga volcano,an extremely high injection height and strong upward motion slowed the removal of aerosols,but extreme water vapor loading still had a certain impact on the half lifetime of the aerosols.These findings highlight the role of water vapor in the persistence of aerosols from submarine eruptions.
基金supported by the National Natural Science Foundation of China(Grant No.12402432)Natural Science Foundation of Jiangsu Province of China(Grant No.BK20230936)Graduate Education and Teaching Reform Project of Nanjing University of Science and Technology(Grant No.KT2024_C14)。
文摘To elucidate the dispersion and explosion characteristics of multi-metal powder and liquid composite fuel formulations,high-energy metal powders(aluminum(Al),boron(B),and magnesium hydride(MgH_(2)))are incorporated into a liquid fuel primarily composed of diethyl ether(DEE)and isopropyl nitrate(IPN).The explosion characteristics of different solid-liquid fuel-air-explosive(FAE)under unconfined conditions are investigated using a high-speed camera,infrared thermal imaging,and a pressure measurement system.Results demonstrate that high-energy metal powders significantly enhance detonation energy dissipation,with aluminum exhibiting the most pronounced effect.Fuel 5#(45.4 wt%DEE,9.2 wt%IPN,29.5 wt%Al,9.1 wt%B,6.8 wt%MgH_(2))exhibits superior explosion performance,achieving higher values of overpressure,impulse,and thermal radiation damage during the detonation stage compared to other fuels.However,Fuel 5#also displays faster decay rates,attributed to accelerated heat release rates induced by B and MgH_(2)powders.This study reveals that different metal powders in solid-liquid FAE exhibit distinct enhancements in explosion performance,providing critical insights for optimizing composite fuel design.
基金supported by Sichuan Science and Technology Program(No.2024NSFSC0060)the National Natural Science Foundation of China(No.U23A2030)the Basic Research Cultivation Support Plan of Southwest Jiaotong University(No.2682023ZTPY016).
文摘Imidazole(IM)particles in the atmosphere affect climate,atmospheric chemical reactions,and human health.However,research on IM particles in the Sichuan Basin(SCB),one of the areas of China affected most heavily by haze,remains very scarce.This study used single-particle aerosol mass spectrometry to investigate IM-containing particles in Chengdu,one of the megacities in the SCB,during summer and winter before and after implemen-tation of the Three-year Action Plan to Win the Blue-Sky Defense War(BSDW).We found that IM-containing particles accounted for 1.2%–12.0%of all detected particles,and they highly mixed with carbonaceous com-ponents,secondary inorganic species,and organic nitrogen.From before to after the BSDW,the proportion of IM-containing particles decreased by 1.8%in summer,but increased by 9.6%in winter.Ammonium/amines and carbonyl compounds were closely related to IM-containing particles;the highest proportion of IM-containing particles occurred in particles mixed with amines and carbonyls.The number fraction of IM-containing particles in all seasons was higher at night than during daytime.The potential source areas of IM-containing particles showed notable narrowing after the BSDW,and the high-value areas were found distributed closer to Chengdu and its surrounding areas.In the winter before the BSDW,most IM-containing particles(>70%)were mixed with organic carbon(OC)particles,and the contributions of OC and mixed organic–elemental carbon(OC-EC)particles increased with aggravation of pollution,whereas OC-EC and Metal particles played a more crucial role in the winter after the BSDW.
基金supported by a sequence of Swiss National Science Foundation Grants (Grant Nos.200021_135395,200020_159938,200020_188601)funding from the Federal Office of Meteorology and Climatology Meteo Swiss within the framework of GCOS Switzerland in support of the Global Energy Balance Archive (GEBA) hosted at ETH Zurich。
文摘Worldwide radiation records suggest that the amount of sunlight received at the Earth's surface(surface solar radiation, SSR) has not been stable over the years, but underwent significant decadal variations, popularly also known as “global dimming and brightening”. These variations have been particularly evident in China, where the SSR substantially declined from the 1960s to the 1990s(dimming), with indications for a trend reversal in the 2000s and a slight recovery(brightening) in recent years. This perspective/review paper will discuss recent updates and remaining challenges regarding our knowledge of the magnitudes, causes, and implications of these variations in SSR worldwide, with a particular emphasis on the developments in China.
文摘We present a comprehensive description and benchmark evaluation of the global–regional chemical transport model called the Emission and Atmospheric Processes Integrated and Coupled Community(EPICC)model.The framework incorporates(1)grid configuration,(2)transport dynamics,(3)chemical mechanisms,(4)aerosol processes,(5)wet/dry deposition parameterizations,and(6)heterogeneous chemistry treatments associated with sulfate,nitrous acid(HONO)chemistry,and aerosol/cloud–photolysis interactions(APIs/CPIs).Openly shared with the atmospheric research community,the model facilitates integration of advanced physicochemical schemes to enhance simulation accuracy.Globally,the model demonstrates realistic representations of ozone(O_(3))and aerosol optical depth.The EPICC model generally demonstrates robust performance in simulating regional concentrations of O_(3) and PM_(2.5)(and its components)in China.It successfully captures vertical profiles of both global and regional O_(3).Notably,the model mitigates frequently reported sulfate underestimations in highly industrialized regions of China.The model accurately captures two regional severe pollution episodes observed in eastern China(January/June 2021).Sensitivity experiments highlight the critical roles of heterogeneous chemical mechanisms associated with sulfate,HONO chemistry,APIs,and CPIs in capturing PM_(2.5) and O_(3) concentrations in China.Improved sulfate mechanisms result in an increase of approximately 32.4%(2.8μg m^(−3))in simulated winter sulfate concentrations when observations exceed 10μg m^(−3).Enhanced HONO elevates winter O_(3) and PM_(2.5) by≤20 and≤10μg m^(−3),respectively.Overall,CPIs dominate over APIs in improving O_(3) and PM_(2.5) simulations across China.Locally,APIs mitigate PM_(2.5) and O_(3) discrepancies in the Sichuan Basin.Seasonal cloud–chemistry coupling explains the weaker impact of PM_(2.5) in summer.
基金supported by National Key Research and Development Program of China(2022YFD1700500)Earmarked Fund for Shandong Agriculture Research System(SDARS-05).
文摘Smoke generator constitute an important class of pesticide formulations widely used in protected agriculture,forestry,mushroom cultivation,and storage environments.Unlike conventional sprays,smoke generator rely on heat-induced phase transitions of active ingredients to produce fine aerosolized particles that disperse through Brownian motion,thereby markedly improving application efficiency.Despite their long history and broad utility,the development of smoke generator has largely stagnated over the past two decades.Here,we provide a comprehensive assessment of their historical evolution,registration landscape,physicochemical mechanisms,and current deployment in agricultural systems.Based on this analysis,we outline key directions for nextgeneration smoke generator technology.First,transitioning from chemical heating to electric heating is essential to enable automation and unmanned pesticide delivery.Second,expanding the air-purification functionality of smoke formulations offers a promising strategy to suppress airborne pest and pathogen populations.Finally,integrating principles of crystal engineering to modulate particle morphology and interfacial affinity may overcome current limitations in deposition efficiency and biological performance.Together,these advances will underpin the development of high-efficiency,intelligent smoke generator and support precision plant protection and sustainable intensification in protected agriculture.
基金supported by the CAS Strategic Priority Research Program(No.XDB0760102),the Ministry of Science and Technology of China(No.2022YFF0802501)the Major Science and Technology Infrastructure Maintenance and Transformation Project of the Chinese Academy of Sciences,Shanghai Science and Technology Innovation Action Plan-Phospherus Project(No.23YF1426200)the National Key Research and Development Program of China(No.2024YFE0212200).
文摘In winter 2018,an aerosol physicochemical experiment was conducted in the Western Pacific Ocean(WPO)aboard the Research Vessel KEXUE of Chinese Academy of Sciences.This study systematically investigated both natural and anthropogenic effects on marine aerosols optical properties,as well as the applicability of multi-satellite products and IMPROVE equation.The averaged aerosol optical depth(AOD500 nm)was 0.31±0.16 andÅngström exponent440–675 nm was 0.29±0.30.In offshore China,significant anthropogenic emissions affected the marine environment.In remote WPO,dust aerosols transported from northern China,Siberia,Central Asia,and those settling from the upper troposphere originating from north Africa,Arabian peninsula,and western India,were dominant.The spatial trends of AOD were opposite in the mid-latitude and southern seas of WPO.The highest AOD,0.32±0.23,appeared along the coast of South Asia at mid-latitude,decreasing from offshore seas to remote oceans.In low-latitude and equatorial seas,AOD significantly increased from coast to remote oceans.Ångström exponent dropped significantly from the coast to remote oceans as anthropogenic influence diminished across the entire WPO.Correlation analysis showed that both MODIS-C6 and Himawari AOD prod-ucts showed similar applicability in coastal urban areas,while Himawari AOD is highly recommended for coastal background and marine environment due to its finer resolution.The extinction coefficient derived from PM_(2.5) chemical compositions using IMPROVE algorithm exhibited a significant correlation(R^(2)=0.58)with the con-currently measured AOD in the absence of long-distance transport,suggesting that the IMPROVE is a reasonable proxy of the columnar average of marine aerosol extinctions free from transport influences.
基金supported by the National Natural Science Foundation of China(Nos.41905108 and 42130704).
文摘Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previous research,providing a long-term perspective on carbonyl compound variations and their environmental implica-tions.Atmospheric observations were conducted at Beijing(BJ)and Xianghe(XH)during the summer and winter months of 2018,2019,and 2023 to study the sources and impacts of carbonyl compounds in typical urban areas and peri‑urban areas.Notably,concentrations in the summer of 2023 increased compared to 2018 and 2019.The predominant carbonyl compounds—formaldehyde,acetaldehyde,and acetone—accounted for over 60%of the total.The mean values of OFP in BJ ranged from 18.55 to 58.61μg/m3,lower than those in XH(29.82 to 65.48μg/m3),with formaldehyde and acetaldehyde contributing over 80%of the total.SOAP exhibited a similar pattern,with values in XH(69.21 to 508.55μg/m3)significantly exceeding those in BJ(34.47 to 159.78μg/m3).The PMF model highlighted vehicle exhaust,secondary pollution,and biomass combustion as major sources of carbonyl compounds,emphasizing differences in source contributions between the two regions.This study’s com-parative analysis over different years and locations provides new insights into the dynamic changes in carbonyl compounds and their environmental importance.These results not only reinforce the importance of carbonyl compounds regulation but also offer a valuable reference for evaluating and refining emission control strategies during this period.
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 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.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(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.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(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 R&D Program of China(No.2022YFC3701102)the National Natural Science Foundation of China(Nos.22376029,22176038,91744205 and 21777025)the Natural Science Foundation of Shanghai City(No.22ZR1404700).
文摘Nitrate renoxification significantly influences atmospheric nitrogen cycling and global OH budgets.Although numerous nitrite acid(HONO)formation pathways from nitrate photolysis have been widely reported,the influence of various environmental factors and aerosol properties on reactive nitrogen production remains largely unclear.In this work,we employed NaNO_(3)/humic acid(HA)as a model nitrate photosensitization system to investigate the crucial roles of aerosol acidity,organic fraction,and dissolved oxygen in the production of HONO,NO_(2),and NO_(2)^(-).The presence of HA at 10 mg/L resulted in a remarkable increase in HONO production rates by approximately 2–3 times and NO_(2)^(-) concentration by 3–6 times across a pH range of 5.2 to 2.0.Meanwhile,the molar fraction of gaseous HONO in total N(Ⅲ)production increased from4%to 69%as bulk-phase pH decreased from 5.2 to 2.0.The higher organic fraction(i.e.,20 and 50 mg/L HA concentration)instead inhibited HONO and NO_(2) release.The presence of dissolved oxygen was found to be adverse for reactive nitrogen production.This suggests that the HA photosensitizer promoted the secondary conversion of NO_(2) to HONO mainly via reduced ketyl radical intermediates,while superoxide radical formation might exert a negative effect.Our findings provide comprehensive insights into reactive nitrogen production from photosensitized nitrate photolysis mediated by various external and internal factors,potentially accounting for discrepancies between field observations and model simulations.
