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
Mineral dust is one of the major aerosols in the atmosphere.To assess its impact on trace atmospheric gases,in this work we present a laboratory study of the effect of temperature on the heterogeneous reaction of NO2 ...Mineral dust is one of the major aerosols in the atmosphere.To assess its impact on trace atmospheric gases,in this work we present a laboratory study of the effect of temperature on the heterogeneous reaction of NO2 on the surface of ambient Chinese dust over the temperature range from 258 to 313 K.The results suggest that nitrogen dioxide could mainly be adsorbed on these types of Chinese mineral dust reversibly with little temperature dependence.Similar to a previous study on NO2 uptake on mineral aerosols,the uptake coefficients are mainly on the order of 10^（-6） for the Chinese dust,when BET areas are taken into account.HONO was observed as a product,and its formation and decomposition on Chinese mineral dust during the uptake processes were also studied.The complete dataset from this study was compiled with previous literature determinations.Atmospheric implications of the heterogeneous reaction between NO2 and mineral dust are also discussed,in an effort to understand this important heterogeneous process.展开更多
The heterogeneous uptake processes of sulfur dioxide on two types of Chinese mineral dust（Inner Mongolia desert dust and Xinjiang sierozem） were investigated using both Knudsen cell and smog chamber system. The temp...The heterogeneous uptake processes of sulfur dioxide on two types of Chinese mineral dust（Inner Mongolia desert dust and Xinjiang sierozem） were investigated using both Knudsen cell and smog chamber system. The temperature dependence of the uptake coefficients was studied over a range from 253 to 313 K using the Knudsen cell reactor, the initial uptake coefficients decreased with the increasing of temperature for these two mineral dust samples, whereas the steady state uptake coefficients of the Xinjiang sierozem increased with the temperature increasing, and these temperature dependence functions were obtained for the first time. In the smog chamber experiments at room temperature, the steady state uptake coefficients of SO2 decreased evidently with the increasing of sulfur dioxide initial concentration from 1.72 × 1012 to 6.15 × 1012mol/cm3. Humid air had effect on the steady state uptake coefficients of SO2 onto Inner Mongolia desert dust.Consequences about the understanding of the uptake processes onto mineral dust samples and the environmental implication were also discussed.展开更多
Understanding the formation mechanisms of secondary air pollution is very important for the formulation of air pollution control countermeasures in China.Thus,a large-scale outdoor atmospheric simulation smog chamber ...Understanding the formation mechanisms of secondary air pollution is very important for the formulation of air pollution control countermeasures in China.Thus,a large-scale outdoor atmospheric simulation smog chamber was constructed at Chinese Research Academy of Environmental Sciences(the CRAES Chamber),which was designed for simulating the atmospheric photochemical processes under the conditions close to the real atmospheric environment.The chamber consisted of a 56-m^(3) fluorinated ethylene propylene(FEP) Teflon film reactor,an electrically-driven stainless steel alloy shield,an auxiliary system,and multiple detection instrumentations.By performing a series of characterization experiments,we obtained basic parameters of the CRAES chamber,such as the mixing ability,the background reactivity,and the wall loss rates of gaseous compounds(propene,NO,NO_(2),ozone) and aerosols(ammonium sulfate).Oxidation experiments were also performed to study the formation of ozone and secondary organic aerosol(SOA),including α-pinene ozonolysis,propene and 1,3,5-trimethylbenzene photooxidation.Temperature and seed effects on the vapor wall loss and SOA yields were obtained in this work:higher temperature and the presence of seed could reduce the vapor wall loss;SOA yield was found to depend inversely on temperature,and the presence of seed could increase SOA yield.The seed was suggested to be used in the chamber to reduce the interaction between the gas phase and chamber walls.The results above showed that the CRAES chamber was reliable and could meet the demands for investigating tropospheric chemistry.展开更多
Heterogeneous reactions of nitrogen dioxide （NO2） on soils collected from Dalian （S 1） and Changsha （S2） were investigated over the relative humidity （RH） range of 5%-80% and temperature range of 278-328 K usi...Heterogeneous reactions of nitrogen dioxide （NO2） on soils collected from Dalian （S 1） and Changsha （S2） were investigated over the relative humidity （RH） range of 5%-80% and temperature range of 278-328 K using a horizontal coated-wall flow tube. The initial uptake coefficients of NO2 on S2 exhibited a decreasing trend from （10 ± 1.3） × 10-8 to （3.1 ± 0.5） x 10-8 with the relative humidity increasing from 5% to 80%. In the temperature effect studies, the initial uptake coefficients of S1 and S2 decreased from （10± 1.2） × 10-8 to （3.8 ± 0.5） × 10-8 and from （16± 2.2） × 10-8 to （3.8 ±0.4） × 10-8 when temperature increased from 278 to 288 K for S1 and from 278 to 308 K for S2, respectively. As the temperature continued to increase, the initial uptake coefficients of S1 and S2 returned to （7.9 ± 1.1）× 10-8 and （20 ± 3.1） × 10-8 at 313 and 328 K, respectively. This study shows that relative humidity could influence the uptake kinetics of NO2 on soil and temperature would impact the heterogeneous chemistry of NO2.展开更多
Anthropogenic emissions alter biogenic secondary organic aerosol(SOA)formation from naturally emitted volatileorganic compounds(BVOCs).We review the major laboratory and field findings with regard to effects of anthro...Anthropogenic emissions alter biogenic secondary organic aerosol(SOA)formation from naturally emitted volatileorganic compounds(BVOCs).We review the major laboratory and field findings with regard to effects of anthropogenicpollutants(NO_(x),anthropogenic aerosols,SO_(2),NH_(3))on biogenic SOA formation.NO_(x) participate in BVOC oxidationthrough changing the radical chemistry and oxidation capacity,leading to a complex SOA composition and yield sensitivitytowards NO_(x) level for different or even specific hydrocarbon precursors.Anthropogenic aerosols act as an importantintermedium for gas-particle partitioning and particle-phase reactions,processes of which are influenced by the particlephase state,acidity,water content and thus associated with biogenic SOA mass accumulation.SO_(2)modifies biogenic SOAformation mainly through sulfuric acid formation and accompanies new particle formation and acid-catalyzedheterogeneous reactions.Some new SO_(2)-involved mechanisms for organosulfate formation have also been proposed.NH_(3)/amines,as the most prevalent base species in the atmosphere,influence biogenic SOA composition and modify theoptical properties of SOA.The response of SOA formation behavior to these anthropogenic pollutants varies amongdifferent BVOCs precursors.Investigations on anthropogenic-biogenic interactions in some areas of China that aresimultaneously influenced by anthropogenic and biogenic emissions are summarized.Based on this review,somerecommendations are made for a more accurate assessment of controllable biogenic SOA formation and its contribution tothe total SOA budget.This study also highlights the importance of controlling anthropogenic pollutant emissions witheffective pollutant mitigation policies to reduce regional and global biogenic SOA formation.展开更多
Multiphase acid-catalyzed oxidation by hydrogen peroxide has been suggested to be a potential route to secondary organic aerosol formation from isoprene and its gas-phase oxidation products, but the lack of kinetics d...Multiphase acid-catalyzed oxidation by hydrogen peroxide has been suggested to be a potential route to secondary organic aerosol formation from isoprene and its gas-phase oxidation products, but the lack of kinetics data significantly limited the evaluation of this process in the atmosphere. Here we report the first measurement of the uptake of isoprene, methacrylic acid and methyl methacrylate into aqueous solutions of sulfuric acid and hydrogen peroxide. Isoprene cannot readily partition into the solution because of its high volatility and low solubility, which hinders its further liquid-phase oxidation. Both methacrylic acid and methyl methacrylate can enter the solutions and be oxidized by hydrogen peroxide, and steady-state uptake was observed with the acidity of solution above 30 wt.% and 70 wt.%, respectively. The steady-state uptake coefficient of methacrylic acid is much larger than that of methyl methacrylate for a solution with same acidity. These observations can be explained by the different reactivity of these two compounds caused by the different electron-withdrawing conjugation between carboxyl and ester groups. The atmospheric lifetimes were estimated based on the calculated steady-state uptake coefficients. These results demonstrate that the multiphase acid-catalyzed oxidation of methacrylic acid plays a role in secondary organic aerosol formation, but for isoprene and methyl methacrylate, this process is not important in the troposphere.展开更多
Acid-catalyzed heterogeneous oxidation with hydrogen peroxide（H2O2） has been suggested to be a potential pathway for secondary organic aerosol（SOA） formation from isoprene and its oxidation products. However, know...Acid-catalyzed heterogeneous oxidation with hydrogen peroxide（H2O2） has been suggested to be a potential pathway for secondary organic aerosol（SOA） formation from isoprene and its oxidation products. However, knowledge of the chemical mechanism and kinetics for this process is still incomplete. 3-Methyl-2-buten-1-ol（MBO321）, an aliphatic alcohol structurally similar to isoprene, is emitted by pine forests and widely used in the manufacturing industries. Herein the uptake of MBO321 into H2SO4-H2O2mixed solution was investigated using a flow-tube reactor coupled to a mass spectrometer. The reactive uptake coefficients（γ） were acquired for the first time and were found to increase rapidly with increasing acid concentration. Corresponding aqueous-phase reactions were performed to further study the mechanism of this acid-catalyzed reaction. MBO321 could convert to 2-methyl-3-buten-2-ol（MBO232） and yield isoprene in acidic media. Organic hydroperoxides（ROOHs） were found to be generated through the acid-catalyzed route,which could undergo a rearrangement reaction and result in the formation of acetone and acetaldehyde. Organosulfates, which have been proposed to be SOA tracer compounds in the atmosphere, were also produced during the oxidation process. These results suggest that the heterogeneous acid-catalyzed reaction of MBO321 with H2O2 may contribute to SOA mass under certain atmospheric conditions.展开更多
The reaction mechanism and kinetics of the simplest Criegee intermediate CH_(2)OO reaction with hydroperoxymethyl formate(HPMF)was investigated at high-level quantum chemistry calculations.HPMF has two reactive functi...The reaction mechanism and kinetics of the simplest Criegee intermediate CH_(2)OO reaction with hydroperoxymethyl formate(HPMF)was investigated at high-level quantum chemistry calculations.HPMF has two reactive functional groups,-C(O)OH and-OOH.The calculated results of thermodynamic data and rate constants indicated that the insertion reactions of CH_(2) OO with-OOH group of HPMF were more favorable than the reactions of CH_(2)OO with-C(O)OH group.The calculated overall rate constant was 2.33×10^(−13) cm^(3)/(moleculesec)at 298 K and the rate constants decreased as the temperature increased from 200 to 480 K.In addition,we also proved the polymerization reaction mechanism between CH_(2)OO and-OOH of HPMF.This theoretical study interpreted the previous experimental results,and supplied the structures of the intermediate products that couldn’t be detected during the experiment.展开更多
Atmospheric nanoparticles are crucial components contributing to fine particulate matter(PM_(2.5)),and therefore have significant effects on visibility,climate,and human health.Due to the unique role of atmospheric na...Atmospheric nanoparticles are crucial components contributing to fine particulate matter(PM_(2.5)),and therefore have significant effects on visibility,climate,and human health.Due to the unique role of atmospheric nanoparticles during the evolution process from gas-phase molecules to larger particles,a number of sophisticated experimental techniques have been developed and employed for online monitoring and characterization of the physical and chemical properties of atmospheric nanoparticles,helping us to better understand the formation and growth of new particles.In this paper,we firstly review these state-of-the-art techniques for investigating the formation and growth of atmospheric nanoparticles(e.g.,the gas-phase precursor species,molecular clusters,physicochemical properties,and chemical composition).Secondly,we present findings from recent field studies on the formation and growth of atmospheric nanoparticles,utilizing several advanced techniques.Further-more,perspectives are proposed for technique development and improvements in measuring atmospheric nanoparticles.展开更多
In this study, the temperature dependence of the heterogeneous uptake of acrylic acid on Arizona test dust （ATD） has been investigated within a temperature range of 255-315 K using a Knudsen cell reactor. Combined w...In this study, the temperature dependence of the heterogeneous uptake of acrylic acid on Arizona test dust （ATD） has been investigated within a temperature range of 255-315 K using a Knudsen cell reactor. Combined with diffuse reflectance infrared Fourier transform spectroscopy （DRIFTS） experiment, it was found that acrylic acid could adsorb on ATD via surface OH groups and convert to carboxylate on the particle surface. The kinetics study suggests that the initial true uptake coefficient （yt） of acrylic acid on ATD decreases from （4.02 ± 0.12） x 10-5 to （1.73 ± 0.05） x 10-5 with a temperature increase from 255 to 315 K. According to the temperature dependence of uptake coefficients, the enthalpy （AHobs） and entropy （ASobs） of uptake processes were determined to be -（9.60± 0.38） KJ/mol and -（121.55 ± 1.33） l.K/mol, respectively. The activation energy for desorption （Edes） was calculated to be （14.57 ± 0.60） KJ/mol. These results indicated that the heterogeneous uptake of acrylic acid on ATD surface was sensitive to temperature. The heterogeneous uptake on ATD could affect the concentration of acrylic acid in the atmosphere, especially at low temperature.展开更多
The heterogeneous uptake processes of hydrogen peroxide on Arizona test dust and two types of authentic Chinese mineral dusts, i.e., Inner Mongolia desert dust and Xinjiang calciferous dust, were investigated using a ...The heterogeneous uptake processes of hydrogen peroxide on Arizona test dust and two types of authentic Chinese mineral dusts, i.e., Inner Mongolia desert dust and Xinjiang calciferous dust, were investigated using a Knudsen cell reactor coupled with a quadrupole mass spectrometer. The uptake coefficients were measured as a function of the initial concentration of H_2O_2 from 2.6 × 10^（11） to 1.2 × 10^（12）molecules/cm^3, and the temperature dependence of the uptake coefficients was investigated over a range from 253 to 313 K. The concentration of H_2O_2 showed little effect on the uptake coefficients of these heterogeneous processes. As a function of temperature, the initial uptake coefficients decrease with increasing temperature, whereas the steady state uptake coefficients of Arizona test dust and Inner Mongolia desert dust increase with increasing temperature. Implications for the understanding of the uptake processes onto mineral dust samples were also discussed.展开更多
Unsaturated alcohols are a class of Biogenic volatile organic compounds(BVOCs)emitted in large quantities by plants when damaged or under adverse environmental conditions,and studies on their atmospheric degradation a...Unsaturated alcohols are a class of Biogenic volatile organic compounds(BVOCs)emitted in large quantities by plants when damaged or under adverse environmental conditions,and studies on their atmospheric degradation at night are still lacking.We used chamber experiments to study the gas-phase reactions of three unsaturated alcohols,E-2-penten-1-ol,Z-2-hexen-1-ol and Z-3-hepten-1-ol,with NO_(3)radicals(NO_(3)•)during the night.The rate constants of these reactions were(11.7±1.76)×10^(−13),(8.55±1.33)×10^(−13)and(6.08±0.47)×10^(−13)cm^(3)/(molecule·s)at 298K and 760 Torr,respectively.In contrast,the reaction rate of similar substances with ozone was about 10^(−18)cm^(3)/(molecule·s),which indicates that the reaction with NO_(3)•is themain oxidation pathway for unsaturated alcohols at night.Small molecule aldehydes and ketones were the main gas-phase organic products of the reaction of three aldehydes and ketones with NO_(3)•,and the total small molecule aldehydes and ketones yields can reach between 45%-60%.They mainly originate from the breakage of alkoxy radicals,and different breakage sites determine different product distributions.In addition,the SOA yields of the three unsaturated alcohols with NO_(3)•were 7.1%±1.0%,12.5%±1.9%and 30.0%±4.5%,respectively,whichweremuch higher than those of similarly structured substances with O_(3)or OH radicals(•OH).The results of high-resolution mass spectrometry shows that the main components of Secondary organic aerosol(SOA)of the three unsaturated alcohols are dimeric compounds containing several nitrate groups,which are formed through the polymerization of oxyalkyl radicals.展开更多
Nitrous acid(HONO)is a crucial source of OH radicals in the troposphere,significantly enhancing secondary pollutants like secondary organic aerosols(SOA)and peroxyacetyl nitrates(PAN).While prior research has examined...Nitrous acid(HONO)is a crucial source of OH radicals in the troposphere,significantly enhancing secondary pollutants like secondary organic aerosols(SOA)and peroxyacetyl nitrates(PAN).While prior research has examined HONO sources and their total impacts on secondary pollution,the specific enhancement capacity of each individual HONO source remains underexplored.This study uses observational data from 2015 to 2018 for HONO,SOA,and PAN across six sites in China,combined with WRF-Chem model adding six potential HONO sources to evaluate their capacity:traffic emissions(E_traffic),soil emissions(E_soil),indoor-outdoor exchange(E_indoor),nitrate photolysis(P_nit),and NO_(2) heterogeneous reactions on aerosol and ground surfaces(Het_a,Het_g).The simulated HONO contributions near the ground in urban Beijing were:12%from NO+OH(default source),10%-20%from E_traffic,1%-12%from P_nit,2%-10%from Het_a,and 50%-70% from Het_g.For SOA and PAN,we calculated incremental contributions enhanced by each HONO source and derived enhancement ratios(ERs)normalized against HONO’s contribution:~7 for P_nit,~2 for Het_a,~0.9 for Het_g,~0.8 for E_soil,~0.3 for E_traffic,and~0.1 for E_indoor.HONO sources’capacity to enhance secondary pollutants varies,being larger for aerosol-related sources.Vertical analysis on HONO concentration,spatial distribution,RO_(x) radical cycling rates,and OH enhancements revealed that aerosol-related HONO sources,especially P_nit,contribute more to secondary pollution.Future research should focus more on assessing real-world impacts of HONO sources,besides identifying their budgets.Additionally,uptake coefficient(γ)and nitrate photolysis frequency(J_(nitrate))critically affect HONO and secondary pollutant formation,necessitating further investigations.展开更多
A novel nanoadsorbent for the removal of heavy metal ions is reported.Cotton was first hydrolyzed to obtain cellulose nanocrystals（CNCs）.CNCs were then chemically modified with succinic anhydride to obtain SCNCs.The...A novel nanoadsorbent for the removal of heavy metal ions is reported.Cotton was first hydrolyzed to obtain cellulose nanocrystals（CNCs）.CNCs were then chemically modified with succinic anhydride to obtain SCNCs.The sodic nanoadsorbent（NaSCNCs） was further prepared by treatment of SCNCs with saturated NaHCO 3 aqueous solution.Batch experiments were carried out with SCNCs and NaSCNCs for the removal of Pb 2＋ and Cd 2＋.The effects of contact time,pH,initial adsorption concentration,coexisting ions and the regeneration performance were investigated.Kinetic studies showed that the adsorption equilibrium time of Pb 2＋ and Cd 2＋ was reached within 150 min on SCNCs and 5 min on NaSCNCs.The adsorption capacities of Pb 2＋ and Cd 2＋ on SCNCs and NaSCNCs increased with increasing pH.The adsorption isotherm was well fitted by the Langmuir model.The maximum adsorption capacities of SCNCs and NaSCNCs for Pb 2＋ and Cd 2＋ were 367.6 mg/g,259.7 mg/g and 465.1 mg/g,344.8 mg/g,respectively.SCNCs and NaSCNCs showed high selectivity and interference resistance from coexisting ions for the adsorption of Pb 2＋.NaSCNCs could be efficiently regenerated with a mild saturated NaCl solution with no loss of capacity after two recycles.The adsorption mechanisms of SCNCs and NaSCNCs were discussed.展开更多
The field observation of 54 non-methane hydrocarbon compounds(NMHCs)was conducted from September 1 to October 20 in 2020 during autumn in Haidian District,Beijing.The mean concentration of total NMHCs was 29.81±1...The field observation of 54 non-methane hydrocarbon compounds(NMHCs)was conducted from September 1 to October 20 in 2020 during autumn in Haidian District,Beijing.The mean concentration of total NMHCs was 29.81±11.39 ppbv during this period,and alkanes were the major components.There were typical festival effects of NMHCs with lower concentration during the National Day.Alkenes and aromatics were the dominant groups in ozone formation potential(OFP)and OH radical loss rate(L_(OH)).The positive matrix factorization(PMF)running results revealed that vehicular exhaust became the biggest source in urban areas,followed by liquefied petroleum gas(LPG)usage,solvent usage,and fuel evaporation.The box model coupled with master chemical mechanism(MCM)was applied to study the impacts of different NMHCs sources on ozone(O_(3))formation in an O_(3)episode.The simulation results indicated that reducing NMHCs concentration could effectively suppress O_(3)formation.Moreover,reducing traffic-related emissions of NMHCs was an effective way to control O_(3)pollution at an urban site in Beijing.展开更多
Atmospheric oxidizing capacity(AOC)is the fundamental driving factors of chemistry process(e.g.,the formation of ozone(O_(3))and secondary organic aerosols(SOA))in the troposphere.However,accurate quantification of AO...Atmospheric oxidizing capacity(AOC)is the fundamental driving factors of chemistry process(e.g.,the formation of ozone(O_(3))and secondary organic aerosols(SOA))in the troposphere.However,accurate quantification of AOC still remains uncertainty.In this study,a comprehensive field campaign was conducted during autumn 2019 in downtown of Beijing,where O_(3) and PM_(2.5) episodes had been experienced successively.The observation-based model(OBM)is used to quantify the AOC at O_(3) and PM_(2.5) episodes.The strong intensity of AOC is found at O_(3) and PM2.5 episodes,and hydroxyl radical(OH)is the dominating daytime oxidant for both episodes.The photolysis of O_(3) is main source of OH at O_(3) episode;the photolysis of nitrous acid(HONO)and formaldehyde(HCHO)plays important role in OH formation at PM_(2.5) episode.The radicals loss routines vary according to precursor pollutants,resulting in different types of air pollution.O_(3) budgets and sensitivity analysis indicates that O_(3) production is transition regime(both VOC and NOx-limited)at O3 episode.The heterogeneous reaction of hydroperoxy radicals(HO_(2))on aerosol surfaces has significant influence on OH and O_(3) production rates.The HO_(2) uptake coefficient(γHO_(2))is the determining factor and required accurate measurement in real atmospheric environment.Our findings could provide the important bases for coordinated control of PM_(2.5) and O_(3) pollution.展开更多
Atmospheric chemistry research has been growing rapidly in China in the last 25 years since the concept of the“air pollution complex”was first proposed by Professor Xiaoyan TANG in 1997.For papers published in 2021 ...Atmospheric chemistry research has been growing rapidly in China in the last 25 years since the concept of the“air pollution complex”was first proposed by Professor Xiaoyan TANG in 1997.For papers published in 2021 on air pollution(only papers included in the Web of Science Core Collection database were considered),more than 24000 papers were authored or co-authored by scientists working in China.In this paper,we review a limited number of representative and significant studies on atmospheric chemistry in China in the last few years,including studies on(1)sources and emission inventories,(2)atmospheric chemical processes,(3)interactions of air pollution with meteorology,weather and climate,(4)interactions between the biosphere and atmosphere,and(5)data assimilation.The intention was not to provide a complete review of all progress made in the last few years,but rather to serve as a starting point for learning more about atmospheric chemistry research in China.The advances reviewed in this paper have enabled a theoretical framework for the air pollution complex to be established,provided robust scientific support to highly successful air pollution control policies in China,and created great opportunities in education,training,and career development for many graduate students and young scientists.This paper further highlights that developing and low-income countries that are heavily affected by air pollution can benefit from these research advances,whilst at the same time acknowledging that many challenges and opportunities still remain in atmospheric chemistry research in China,to hopefully be addressed over the next few decades.展开更多
A distinctive kind of organic carbon aerosol that could absorb ultraviolet-visible radiation is called brown carbon(Br C),which has an important positive influence on radiative budget and climate change.In this work,w...A distinctive kind of organic carbon aerosol that could absorb ultraviolet-visible radiation is called brown carbon(Br C),which has an important positive influence on radiative budget and climate change.In this work,we reported the absorption properties and potential source of Br C based on a seven-wavelength aethalometer in the winter of 2018–2019 at an urban site of Sanmenxia in Fenwei Plain in central China.Specifically,the mean value of Br C absorption coefficient was 59.6±36.0 Mm^(-1) at 370 nm and contributed 37.7%to total absorption,which made a significant impact on visibility and regional environment.Absorption coefficients of Br C showed double-peak pattern,and Br C had shown small fluctuations under haze days compared with clean days.As for the sources of Br C,Br C absorption coefficients expressed strong correlations with element carbon aerosols and primary organic carbon aerosols,indicating that most of Br C originated from primary emissions.The linear correlations between trace metal elements(K,As,Fe,Mn,Zn,and Pb)and Br C absorption coefficients further referred that the major sources of Br C were primary emissions,like coal burning,biomass burning,and vehicle emissions.The moderate relationship between Br C absorption coefficients and secondary organic aerosols suggested that secondary production of Br C also played an important role.The 120 hr backward air mass trajectories analysis and concentration-weighted trajectories analysis were also used to investigate potential sources of Br C in and around this area,which inferred most parts of Br C were derived from local emissions.展开更多
To better characterize the optical properties of atmospheric aerosols, the multi-wavelength cavity ring-down aerosol extinction spectrometer(MCRD-AES) is developed and applied in this study. By using tunable light sou...To better characterize the optical properties of atmospheric aerosols, the multi-wavelength cavity ring-down aerosol extinction spectrometer(MCRD-AES) is developed and applied in this study. By using tunable light source and four parallel cavities, the MCRD-AES covers a wide and atmospherically relevant wavelength range from 360 to 663 nm. Four wavelengths(375 nm, 440 nm, 532 nm, and 620 nm) are particularly tested with ammonium sulfate and nigrosine. The refractive index values obtained from this study agree well with literature data. The stability and accuracy of the MCRD-AES are tested, and the minimum detectable extinction coefficient is 0.5 1/Mm. The high sensitivity, high precision, and wavelength changeable of MCRD-AES indicate its great application prospect in comprehensively quantifying the optical properties of atmospheric aerosols.展开更多
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 Basic Research Program (973) of Ministry of Science and Technology of China (No.2011CB403401)the National Natural Science Foundation of China (Nos.21190052,41173112,and 41475114)the Strategic Priority Research Program (B) of the Chinese Academy of Sciences (No.XDB05010400)
文摘Mineral dust is one of the major aerosols in the atmosphere.To assess its impact on trace atmospheric gases,in this work we present a laboratory study of the effect of temperature on the heterogeneous reaction of NO2 on the surface of ambient Chinese dust over the temperature range from 258 to 313 K.The results suggest that nitrogen dioxide could mainly be adsorbed on these types of Chinese mineral dust reversibly with little temperature dependence.Similar to a previous study on NO2 uptake on mineral aerosols,the uptake coefficients are mainly on the order of 10^（-6） for the Chinese dust,when BET areas are taken into account.HONO was observed as a product,and its formation and decomposition on Chinese mineral dust during the uptake processes were also studied.The complete dataset from this study was compiled with previous literature determinations.Atmospheric implications of the heterogeneous reaction between NO2 and mineral dust are also discussed,in an effort to understand this important heterogeneous process.
基金supported by the Strategic Priority Research Program(B)of the Chinese Academy of Sciences(No.XDB05010400)the National Basic Research Program(973)of Ministry of Science and Technology of China(No.2011CB403401)the National Natural Science Foundation of China(Major Program:21190052)(Nos.40925016,41173112)
文摘The heterogeneous uptake processes of sulfur dioxide on two types of Chinese mineral dust（Inner Mongolia desert dust and Xinjiang sierozem） were investigated using both Knudsen cell and smog chamber system. The temperature dependence of the uptake coefficients was studied over a range from 253 to 313 K using the Knudsen cell reactor, the initial uptake coefficients decreased with the increasing of temperature for these two mineral dust samples, whereas the steady state uptake coefficients of the Xinjiang sierozem increased with the temperature increasing, and these temperature dependence functions were obtained for the first time. In the smog chamber experiments at room temperature, the steady state uptake coefficients of SO2 decreased evidently with the increasing of sulfur dioxide initial concentration from 1.72 × 1012 to 6.15 × 1012mol/cm3. Humid air had effect on the steady state uptake coefficients of SO2 onto Inner Mongolia desert dust.Consequences about the understanding of the uptake processes onto mineral dust samples and the environmental implication were also discussed.
基金supported by the China Postdoctoral Science Foundation (No.2019M660752)the Beijing Municipal Science&Technology Commission (No.Z181100005418015),LAC/CMA (No.2019B08)+2 种基金the Fundamental Research Funds for Central Public Welfare Scientific Research Institutes of ChinaChinese Research Academy of Environmental Sciences (Nos.GYG5051201,2009GGQD18,2019YSKY-018,2019YSKY-012)the Chinese Academy of Sciences Strategic Leading Science and Technology Project (Class B)(No.XDB05010200)。
文摘Understanding the formation mechanisms of secondary air pollution is very important for the formulation of air pollution control countermeasures in China.Thus,a large-scale outdoor atmospheric simulation smog chamber was constructed at Chinese Research Academy of Environmental Sciences(the CRAES Chamber),which was designed for simulating the atmospheric photochemical processes under the conditions close to the real atmospheric environment.The chamber consisted of a 56-m^(3) fluorinated ethylene propylene(FEP) Teflon film reactor,an electrically-driven stainless steel alloy shield,an auxiliary system,and multiple detection instrumentations.By performing a series of characterization experiments,we obtained basic parameters of the CRAES chamber,such as the mixing ability,the background reactivity,and the wall loss rates of gaseous compounds(propene,NO,NO_(2),ozone) and aerosols(ammonium sulfate).Oxidation experiments were also performed to study the formation of ozone and secondary organic aerosol(SOA),including α-pinene ozonolysis,propene and 1,3,5-trimethylbenzene photooxidation.Temperature and seed effects on the vapor wall loss and SOA yields were obtained in this work:higher temperature and the presence of seed could reduce the vapor wall loss;SOA yield was found to depend inversely on temperature,and the presence of seed could increase SOA yield.The seed was suggested to be used in the chamber to reduce the interaction between the gas phase and chamber walls.The results above showed that the CRAES chamber was reliable and could meet the demands for investigating tropospheric chemistry.
基金supported by the Knowledge Innovation Program of the Chinese Academy of Sciences (No.KJCX2-EW-H01)the National Basic Research Program(973) of China (No. 2011CB403401)the National Natural Science Foundation of China (No. 21077109,41005070)
文摘Heterogeneous reactions of nitrogen dioxide （NO2） on soils collected from Dalian （S 1） and Changsha （S2） were investigated over the relative humidity （RH） range of 5%-80% and temperature range of 278-328 K using a horizontal coated-wall flow tube. The initial uptake coefficients of NO2 on S2 exhibited a decreasing trend from （10 ± 1.3） × 10-8 to （3.1 ± 0.5） x 10-8 with the relative humidity increasing from 5% to 80%. In the temperature effect studies, the initial uptake coefficients of S1 and S2 decreased from （10± 1.2） × 10-8 to （3.8 ± 0.5） × 10-8 and from （16± 2.2） × 10-8 to （3.8 ±0.4） × 10-8 when temperature increased from 278 to 288 K for S1 and from 278 to 308 K for S2, respectively. As the temperature continued to increase, the initial uptake coefficients of S1 and S2 returned to （7.9 ± 1.1）× 10-8 and （20 ± 3.1） × 10-8 at 313 and 328 K, respectively. This study shows that relative humidity could influence the uptake kinetics of NO2 on soil and temperature would impact the heterogeneous chemistry of NO2.
基金This work was supported by National Natural Science Foundation of China(Grant No.91644214)Youth Innovation Program of Universities in Shandong Province(Grant No.2019KJD007)Fundamental Research Fund of Shandong University(Grant No.2020QNQT012).
文摘Anthropogenic emissions alter biogenic secondary organic aerosol(SOA)formation from naturally emitted volatileorganic compounds(BVOCs).We review the major laboratory and field findings with regard to effects of anthropogenicpollutants(NO_(x),anthropogenic aerosols,SO_(2),NH_(3))on biogenic SOA formation.NO_(x) participate in BVOC oxidationthrough changing the radical chemistry and oxidation capacity,leading to a complex SOA composition and yield sensitivitytowards NO_(x) level for different or even specific hydrocarbon precursors.Anthropogenic aerosols act as an importantintermedium for gas-particle partitioning and particle-phase reactions,processes of which are influenced by the particlephase state,acidity,water content and thus associated with biogenic SOA mass accumulation.SO_(2)modifies biogenic SOAformation mainly through sulfuric acid formation and accompanies new particle formation and acid-catalyzedheterogeneous reactions.Some new SO_(2)-involved mechanisms for organosulfate formation have also been proposed.NH_(3)/amines,as the most prevalent base species in the atmosphere,influence biogenic SOA composition and modify theoptical properties of SOA.The response of SOA formation behavior to these anthropogenic pollutants varies amongdifferent BVOCs precursors.Investigations on anthropogenic-biogenic interactions in some areas of China that aresimultaneously influenced by anthropogenic and biogenic emissions are summarized.Based on this review,somerecommendations are made for a more accurate assessment of controllable biogenic SOA formation and its contribution tothe total SOA budget.This study also highlights the importance of controlling anthropogenic pollutant emissions witheffective pollutant mitigation policies to reduce regional and global biogenic SOA formation.
基金supported by the Knowledge Innovation Program of the Chinese Academy of Sciences (No.KJCX2-EW-H01)the National Basic Research Program(973) of Ministry of Science and Technology of China (No.2011CB403401)the National Natural Science Foundation of China (No.40925016, 40830101, 21077109,41005070, 41105085)
文摘Multiphase acid-catalyzed oxidation by hydrogen peroxide has been suggested to be a potential route to secondary organic aerosol formation from isoprene and its gas-phase oxidation products, but the lack of kinetics data significantly limited the evaluation of this process in the atmosphere. Here we report the first measurement of the uptake of isoprene, methacrylic acid and methyl methacrylate into aqueous solutions of sulfuric acid and hydrogen peroxide. Isoprene cannot readily partition into the solution because of its high volatility and low solubility, which hinders its further liquid-phase oxidation. Both methacrylic acid and methyl methacrylate can enter the solutions and be oxidized by hydrogen peroxide, and steady-state uptake was observed with the acidity of solution above 30 wt.% and 70 wt.%, respectively. The steady-state uptake coefficient of methacrylic acid is much larger than that of methyl methacrylate for a solution with same acidity. These observations can be explained by the different reactivity of these two compounds caused by the different electron-withdrawing conjugation between carboxyl and ester groups. The atmospheric lifetimes were estimated based on the calculated steady-state uptake coefficients. These results demonstrate that the multiphase acid-catalyzed oxidation of methacrylic acid plays a role in secondary organic aerosol formation, but for isoprene and methyl methacrylate, this process is not important in the troposphere.
基金project was supported by the Strategic Priority Research Program (B) of the Chinese Academy of Sciences (No. XDB05010400)the National Basic Research Program (973) of Ministry of Science and Technology of China (No. 2011CB403401)the National Natural Science Foundation of China (Major Program: 21190052) (Nos. 40925016, 41173112)
文摘Acid-catalyzed heterogeneous oxidation with hydrogen peroxide（H2O2） has been suggested to be a potential pathway for secondary organic aerosol（SOA） formation from isoprene and its oxidation products. However, knowledge of the chemical mechanism and kinetics for this process is still incomplete. 3-Methyl-2-buten-1-ol（MBO321）, an aliphatic alcohol structurally similar to isoprene, is emitted by pine forests and widely used in the manufacturing industries. Herein the uptake of MBO321 into H2SO4-H2O2mixed solution was investigated using a flow-tube reactor coupled to a mass spectrometer. The reactive uptake coefficients（γ） were acquired for the first time and were found to increase rapidly with increasing acid concentration. Corresponding aqueous-phase reactions were performed to further study the mechanism of this acid-catalyzed reaction. MBO321 could convert to 2-methyl-3-buten-2-ol（MBO232） and yield isoprene in acidic media. Organic hydroperoxides（ROOHs） were found to be generated through the acid-catalyzed route,which could undergo a rearrangement reaction and result in the formation of acetone and acetaldehyde. Organosulfates, which have been proposed to be SOA tracer compounds in the atmosphere, were also produced during the oxidation process. These results suggest that the heterogeneous acid-catalyzed reaction of MBO321 with H2O2 may contribute to SOA mass under certain atmospheric conditions.
基金supported by the National Key Research and Development Program of China(No.2016YFC0202200)the Na-tional Natural Science Foundation of China(No.42022039)+2 种基金Beijing National Laboratory for Molecular Sciences(No.BNLMS-CXXM-202011)Beijing Nova Program(No.2018113)the Youth Innovation Promotion Association CAS(No.2017042).
文摘The reaction mechanism and kinetics of the simplest Criegee intermediate CH_(2)OO reaction with hydroperoxymethyl formate(HPMF)was investigated at high-level quantum chemistry calculations.HPMF has two reactive functional groups,-C(O)OH and-OOH.The calculated results of thermodynamic data and rate constants indicated that the insertion reactions of CH_(2) OO with-OOH group of HPMF were more favorable than the reactions of CH_(2)OO with-C(O)OH group.The calculated overall rate constant was 2.33×10^(−13) cm^(3)/(moleculesec)at 298 K and the rate constants decreased as the temperature increased from 200 to 480 K.In addition,we also proved the polymerization reaction mechanism between CH_(2)OO and-OOH of HPMF.This theoretical study interpreted the previous experimental results,and supplied the structures of the intermediate products that couldn’t be detected during the experiment.
基金supported by the National Key Research and Development Program of China(No.2017YFC0209500)。
文摘Atmospheric nanoparticles are crucial components contributing to fine particulate matter(PM_(2.5)),and therefore have significant effects on visibility,climate,and human health.Due to the unique role of atmospheric nanoparticles during the evolution process from gas-phase molecules to larger particles,a number of sophisticated experimental techniques have been developed and employed for online monitoring and characterization of the physical and chemical properties of atmospheric nanoparticles,helping us to better understand the formation and growth of new particles.In this paper,we firstly review these state-of-the-art techniques for investigating the formation and growth of atmospheric nanoparticles(e.g.,the gas-phase precursor species,molecular clusters,physicochemical properties,and chemical composition).Secondly,we present findings from recent field studies on the formation and growth of atmospheric nanoparticles,utilizing several advanced techniques.Further-more,perspectives are proposed for technique development and improvements in measuring atmospheric nanoparticles.
基金supported by the National Natural Science Foundation of China(Nos.41405118 and 91544227)the Strategic Priority Research Program(B)of the Chinese Academy of Sciences(No.XDB05010400)+1 种基金the National Key Technology Support Plan Projects(No.2014BAC16B01)the Basic Scientific Research Progress of the Chinese Academy of Meteorological Sciences(No.2014Y007)
文摘In this study, the temperature dependence of the heterogeneous uptake of acrylic acid on Arizona test dust （ATD） has been investigated within a temperature range of 255-315 K using a Knudsen cell reactor. Combined with diffuse reflectance infrared Fourier transform spectroscopy （DRIFTS） experiment, it was found that acrylic acid could adsorb on ATD via surface OH groups and convert to carboxylate on the particle surface. The kinetics study suggests that the initial true uptake coefficient （yt） of acrylic acid on ATD decreases from （4.02 ± 0.12） x 10-5 to （1.73 ± 0.05） x 10-5 with a temperature increase from 255 to 315 K. According to the temperature dependence of uptake coefficients, the enthalpy （AHobs） and entropy （ASobs） of uptake processes were determined to be -（9.60± 0.38） KJ/mol and -（121.55 ± 1.33） l.K/mol, respectively. The activation energy for desorption （Edes） was calculated to be （14.57 ± 0.60） KJ/mol. These results indicated that the heterogeneous uptake of acrylic acid on ATD surface was sensitive to temperature. The heterogeneous uptake on ATD could affect the concentration of acrylic acid in the atmosphere, especially at low temperature.
基金supported by the Strategic Priority Research Program (B) of the Chinese Academy of Sciences (No.XDB05010400)the National Basic Research Program of China (973 Program) (No.2011CB403401) of Ministry of Science and Technology of China,the National Natural Science Foundation of China (Nos.41173112,21477134)
文摘The heterogeneous uptake processes of hydrogen peroxide on Arizona test dust and two types of authentic Chinese mineral dusts, i.e., Inner Mongolia desert dust and Xinjiang calciferous dust, were investigated using a Knudsen cell reactor coupled with a quadrupole mass spectrometer. The uptake coefficients were measured as a function of the initial concentration of H_2O_2 from 2.6 × 10^（11） to 1.2 × 10^（12）molecules/cm^3, and the temperature dependence of the uptake coefficients was investigated over a range from 253 to 313 K. The concentration of H_2O_2 showed little effect on the uptake coefficients of these heterogeneous processes. As a function of temperature, the initial uptake coefficients decrease with increasing temperature, whereas the steady state uptake coefficients of Arizona test dust and Inner Mongolia desert dust increase with increasing temperature. Implications for the understanding of the uptake processes onto mineral dust samples were also discussed.
基金supported by the National Key Research and Development Program of China(No.2020YFA0607800)the National Natural Science Foundation of China(Nos.42022039 and 42130606)Beijing National Laboratory for Molecular Sciences(No.BNLMS-CXXM-202011),the Youth Innovation Promotion Association of Chinese Academy of Sciences(No.Y2021013).
文摘Unsaturated alcohols are a class of Biogenic volatile organic compounds(BVOCs)emitted in large quantities by plants when damaged or under adverse environmental conditions,and studies on their atmospheric degradation at night are still lacking.We used chamber experiments to study the gas-phase reactions of three unsaturated alcohols,E-2-penten-1-ol,Z-2-hexen-1-ol and Z-3-hepten-1-ol,with NO_(3)radicals(NO_(3)•)during the night.The rate constants of these reactions were(11.7±1.76)×10^(−13),(8.55±1.33)×10^(−13)and(6.08±0.47)×10^(−13)cm^(3)/(molecule·s)at 298K and 760 Torr,respectively.In contrast,the reaction rate of similar substances with ozone was about 10^(−18)cm^(3)/(molecule·s),which indicates that the reaction with NO_(3)•is themain oxidation pathway for unsaturated alcohols at night.Small molecule aldehydes and ketones were the main gas-phase organic products of the reaction of three aldehydes and ketones with NO_(3)•,and the total small molecule aldehydes and ketones yields can reach between 45%-60%.They mainly originate from the breakage of alkoxy radicals,and different breakage sites determine different product distributions.In addition,the SOA yields of the three unsaturated alcohols with NO_(3)•were 7.1%±1.0%,12.5%±1.9%and 30.0%±4.5%,respectively,whichweremuch higher than those of similarly structured substances with O_(3)or OH radicals(•OH).The results of high-resolution mass spectrometry shows that the main components of Secondary organic aerosol(SOA)of the three unsaturated alcohols are dimeric compounds containing several nitrate groups,which are formed through the polymerization of oxyalkyl radicals.
基金supported by the National Natural Science Foundation of China(Nos.92044302,42075108,42107124,41822703,91544221,91844301,and 22222610)Beijing National Laboratory for Molecular Sciences(No.BNLMS-CXXM-202011)the Natural Science Foundation of Yunnan Province(No.202302AN360006)。
文摘Nitrous acid(HONO)is a crucial source of OH radicals in the troposphere,significantly enhancing secondary pollutants like secondary organic aerosols(SOA)and peroxyacetyl nitrates(PAN).While prior research has examined HONO sources and their total impacts on secondary pollution,the specific enhancement capacity of each individual HONO source remains underexplored.This study uses observational data from 2015 to 2018 for HONO,SOA,and PAN across six sites in China,combined with WRF-Chem model adding six potential HONO sources to evaluate their capacity:traffic emissions(E_traffic),soil emissions(E_soil),indoor-outdoor exchange(E_indoor),nitrate photolysis(P_nit),and NO_(2) heterogeneous reactions on aerosol and ground surfaces(Het_a,Het_g).The simulated HONO contributions near the ground in urban Beijing were:12%from NO+OH(default source),10%-20%from E_traffic,1%-12%from P_nit,2%-10%from Het_a,and 50%-70% from Het_g.For SOA and PAN,we calculated incremental contributions enhanced by each HONO source and derived enhancement ratios(ERs)normalized against HONO’s contribution:~7 for P_nit,~2 for Het_a,~0.9 for Het_g,~0.8 for E_soil,~0.3 for E_traffic,and~0.1 for E_indoor.HONO sources’capacity to enhance secondary pollutants varies,being larger for aerosol-related sources.Vertical analysis on HONO concentration,spatial distribution,RO_(x) radical cycling rates,and OH enhancements revealed that aerosol-related HONO sources,especially P_nit,contribute more to secondary pollution.Future research should focus more on assessing real-world impacts of HONO sources,besides identifying their budgets.Additionally,uptake coefficient(γ)and nitrate photolysis frequency(J_(nitrate))critically affect HONO and secondary pollutant formation,necessitating further investigations.
基金supported by the National Basic Research Program (973) of China (No. 2011CB933700) of Ministry of Science and Technology of China
文摘A novel nanoadsorbent for the removal of heavy metal ions is reported.Cotton was first hydrolyzed to obtain cellulose nanocrystals（CNCs）.CNCs were then chemically modified with succinic anhydride to obtain SCNCs.The sodic nanoadsorbent（NaSCNCs） was further prepared by treatment of SCNCs with saturated NaHCO 3 aqueous solution.Batch experiments were carried out with SCNCs and NaSCNCs for the removal of Pb 2＋ and Cd 2＋.The effects of contact time,pH,initial adsorption concentration,coexisting ions and the regeneration performance were investigated.Kinetic studies showed that the adsorption equilibrium time of Pb 2＋ and Cd 2＋ was reached within 150 min on SCNCs and 5 min on NaSCNCs.The adsorption capacities of Pb 2＋ and Cd 2＋ on SCNCs and NaSCNCs increased with increasing pH.The adsorption isotherm was well fitted by the Langmuir model.The maximum adsorption capacities of SCNCs and NaSCNCs for Pb 2＋ and Cd 2＋ were 367.6 mg/g,259.7 mg/g and 465.1 mg/g,344.8 mg/g,respectively.SCNCs and NaSCNCs showed high selectivity and interference resistance from coexisting ions for the adsorption of Pb 2＋.NaSCNCs could be efficiently regenerated with a mild saturated NaCl solution with no loss of capacity after two recycles.The adsorption mechanisms of SCNCs and NaSCNCs were discussed.
基金supported by the National Key Research and Development Program of China(No.2017YFC0210001)National Natural Science Foundation of China(Nos.42022039,21671089)+2 种基金the Scientific Research Fund of Liaoning Provincial Education Department(No.L2020002)Beijing National Laboratory for Molecular Sciences(No.BNLMS-CXXM-202011)the Youth Innovation Promotion Association CAS(No.2017042)
文摘The field observation of 54 non-methane hydrocarbon compounds(NMHCs)was conducted from September 1 to October 20 in 2020 during autumn in Haidian District,Beijing.The mean concentration of total NMHCs was 29.81±11.39 ppbv during this period,and alkanes were the major components.There were typical festival effects of NMHCs with lower concentration during the National Day.Alkenes and aromatics were the dominant groups in ozone formation potential(OFP)and OH radical loss rate(L_(OH)).The positive matrix factorization(PMF)running results revealed that vehicular exhaust became the biggest source in urban areas,followed by liquefied petroleum gas(LPG)usage,solvent usage,and fuel evaporation.The box model coupled with master chemical mechanism(MCM)was applied to study the impacts of different NMHCs sources on ozone(O_(3))formation in an O_(3)episode.The simulation results indicated that reducing NMHCs concentration could effectively suppress O_(3)formation.Moreover,reducing traffic-related emissions of NMHCs was an effective way to control O_(3)pollution at an urban site in Beijing.
基金supported by the National Key Research and Development Program of China (No. 2017YFC0210001)the National Natural Science Foundation of China (Nos. 41830106, 42022039)+1 种基金Beijing National Laboratory for Molecular Sciences (No. BNLMS-CXXM-202011)the Youth Innovation Promotion Association CAS (No. 2017042)
文摘Atmospheric oxidizing capacity(AOC)is the fundamental driving factors of chemistry process(e.g.,the formation of ozone(O_(3))and secondary organic aerosols(SOA))in the troposphere.However,accurate quantification of AOC still remains uncertainty.In this study,a comprehensive field campaign was conducted during autumn 2019 in downtown of Beijing,where O_(3) and PM_(2.5) episodes had been experienced successively.The observation-based model(OBM)is used to quantify the AOC at O_(3) and PM_(2.5) episodes.The strong intensity of AOC is found at O_(3) and PM2.5 episodes,and hydroxyl radical(OH)is the dominating daytime oxidant for both episodes.The photolysis of O_(3) is main source of OH at O_(3) episode;the photolysis of nitrous acid(HONO)and formaldehyde(HCHO)plays important role in OH formation at PM_(2.5) episode.The radicals loss routines vary according to precursor pollutants,resulting in different types of air pollution.O_(3) budgets and sensitivity analysis indicates that O_(3) production is transition regime(both VOC and NOx-limited)at O3 episode.The heterogeneous reaction of hydroperoxy radicals(HO_(2))on aerosol surfaces has significant influence on OH and O_(3) production rates.The HO_(2) uptake coefficient(γHO_(2))is the determining factor and required accurate measurement in real atmospheric environment.Our findings could provide the important bases for coordinated control of PM_(2.5) and O_(3) pollution.
基金funded by the National Natural Science Foundation of China(Grant No.91844000)。
文摘Atmospheric chemistry research has been growing rapidly in China in the last 25 years since the concept of the“air pollution complex”was first proposed by Professor Xiaoyan TANG in 1997.For papers published in 2021 on air pollution(only papers included in the Web of Science Core Collection database were considered),more than 24000 papers were authored or co-authored by scientists working in China.In this paper,we review a limited number of representative and significant studies on atmospheric chemistry in China in the last few years,including studies on(1)sources and emission inventories,(2)atmospheric chemical processes,(3)interactions of air pollution with meteorology,weather and climate,(4)interactions between the biosphere and atmosphere,and(5)data assimilation.The intention was not to provide a complete review of all progress made in the last few years,but rather to serve as a starting point for learning more about atmospheric chemistry research in China.The advances reviewed in this paper have enabled a theoretical framework for the air pollution complex to be established,provided robust scientific support to highly successful air pollution control policies in China,and created great opportunities in education,training,and career development for many graduate students and young scientists.This paper further highlights that developing and low-income countries that are heavily affected by air pollution can benefit from these research advances,whilst at the same time acknowledging that many challenges and opportunities still remain in atmospheric chemistry research in China,to hopefully be addressed over the next few decades.
基金supported by The National Key Research and Development Program of China(No.2017YFC0209500)the National Natural Science Foundation of China(Nos.91744204,41822703,and 91844301)National research program for key issues in air pollution control(No.DQGG-0103)。
文摘A distinctive kind of organic carbon aerosol that could absorb ultraviolet-visible radiation is called brown carbon(Br C),which has an important positive influence on radiative budget and climate change.In this work,we reported the absorption properties and potential source of Br C based on a seven-wavelength aethalometer in the winter of 2018–2019 at an urban site of Sanmenxia in Fenwei Plain in central China.Specifically,the mean value of Br C absorption coefficient was 59.6±36.0 Mm^(-1) at 370 nm and contributed 37.7%to total absorption,which made a significant impact on visibility and regional environment.Absorption coefficients of Br C showed double-peak pattern,and Br C had shown small fluctuations under haze days compared with clean days.As for the sources of Br C,Br C absorption coefficients expressed strong correlations with element carbon aerosols and primary organic carbon aerosols,indicating that most of Br C originated from primary emissions.The linear correlations between trace metal elements(K,As,Fe,Mn,Zn,and Pb)and Br C absorption coefficients further referred that the major sources of Br C were primary emissions,like coal burning,biomass burning,and vehicle emissions.The moderate relationship between Br C absorption coefficients and secondary organic aerosols suggested that secondary production of Br C also played an important role.The 120 hr backward air mass trajectories analysis and concentration-weighted trajectories analysis were also used to investigate potential sources of Br C in and around this area,which inferred most parts of Br C were derived from local emissions.
基金supported by the National Natural Science Foundation of China (No.41227805)the National Key Research and Development Program of China (No.2016YFC0202704)
文摘To better characterize the optical properties of atmospheric aerosols, the multi-wavelength cavity ring-down aerosol extinction spectrometer(MCRD-AES) is developed and applied in this study. By using tunable light source and four parallel cavities, the MCRD-AES covers a wide and atmospherically relevant wavelength range from 360 to 663 nm. Four wavelengths(375 nm, 440 nm, 532 nm, and 620 nm) are particularly tested with ammonium sulfate and nigrosine. The refractive index values obtained from this study agree well with literature data. The stability and accuracy of the MCRD-AES are tested, and the minimum detectable extinction coefficient is 0.5 1/Mm. The high sensitivity, high precision, and wavelength changeable of MCRD-AES indicate its great application prospect in comprehensively quantifying the optical properties of atmospheric aerosols.
