Wildfire events are increasing globally which may be partly associated with climate change,resulting in significant adverse impacts on local,regional air quality and global climate.In September 2020,a small wildfire(b...Wildfire events are increasing globally which may be partly associated with climate change,resulting in significant adverse impacts on local,regional air quality and global climate.In September 2020,a small wildfire(burned area:36.3 ha)event occurred in Souesmes(Loiret-Cher,Sologne,France),and its plume spread out over 200 km on the following day as observed by the MODIS satellite.Based on measurements at a suburban site(~50 km northwest of the fire location)in Orléans and backward trajectory analysis,young wildfire plumes were characterized.Significant increases in gaseous pollutants(CO,CH_(4),N_(2)O,VOCs,etc.)and particles(including black carbon)were found within the wildfire plumes,leading to a reduced air quality.Emission factors,defined as EF(X)=ΔX/ΔCO(where,X represents the target species),of various trace gases and black carbon within the young wildfire plumes were determined accordingly and compared with previous studies.Changes in the ambient ions(such as ammonium,sulfate,nitrate,chloride,and nitrite in the particle-and gasphase)and aerosol properties(e.g.,aerosol water content,aerosol p H)were also quantified and discussed.Moreover,we estimated the total carbon and climate-related species(e.g.,CO_(2),CH_(4),N_(2)O,and BC)emissions and compared them with fire emission inventories.Current biomass burning emission inventories have uncertainties in estimating small fire burned areas and emissions.For instance,we found that the Global Fire Assimilation System(GFAS)may underestimate emissions(e.g.,CO)of this small wildfire while other inventories(GFED and FINN)showed significant overestimation.Considering that it is the first time to record wildfire plumes in this region,related atmospheric implications are presented and discussed.展开更多
The atmospheric concentrations of carbonyls and BTEX (benzene,toluene,ethylbenzene,m,p-xylene and o-xylene) were measured simultaneously at a same sampling site in Beijing from September 2008 to August 2010.The aver...The atmospheric concentrations of carbonyls and BTEX (benzene,toluene,ethylbenzene,m,p-xylene and o-xylene) were measured simultaneously at a same sampling site in Beijing from September 2008 to August 2010.The average concentrations of the total measured carbonyls during autumn,winter,spring,and summer were 37.7,31.3,39.7,50.5 μg/m 3,respectively,and maximal values for their diurnal variations usually happened at noontime.In contrast to carbonyls,the average concentrations of the total measured BTEX during the four seasons were 27.2,31.9,23.2,19.1 μg/m 3,respectively,andminimal values for their diurnal variations always occurred in the early afternoon.The average concentration for carbonyls increased about 24% from September 2008–August 2009 to September 2009–August 2010,for BTEX,increased about 15%.Integrated life time cancer risks for three carcinogens (benzene,formaldehyde and acetaldehyde) in Beijing exceeded the value of 1E-06,and the hazard quotient (HQ) of non-cancer risk of exposure to formaldehyde exceeded unity.展开更多
As a secondary pollutant of photochemical pollution,peroxyacetyl nitrate(PAN)has attracted a close attention.A four-month campaign was conducted at a rural site in North China Plain(NCP)including the measurement of PA...As a secondary pollutant of photochemical pollution,peroxyacetyl nitrate(PAN)has attracted a close attention.A four-month campaign was conducted at a rural site in North China Plain(NCP)including the measurement of PAN,O_(3),NO_(x),PM_(2.5),oxygenated volatile organic compounds(OVOCs),photolysis rate constants of NO_(2)and O_(3)and meteorological parameters to investigate the wintertime characterization of photochemistry from November 2018 to February 2019.The results showed that the maximum and mean values of PAN were 4.38 and 0.93±0.67 ppbv during the campaign,respectively.The PAN under different PM_(2.5)concentrations from below 75μg/m^(3)up to 250μg/m^(3),showed different diurnal variation and formation rate.In the PM_(2.5)concentration range of above 250μg/m^(3),PAN had the largest daily mean value of 0.64 ppbv and the fastest production rate of 0.33 ppbv/hr.From the perspective of PAN’s production mechanism,the light intensity and precursors concentrations under different PM_(2.5)pollution levels indicated that there were sufficient light intensity and high volatile organic compounds(VOCs)and NO_(x)precursors concentration even under severe pollution level to generate a large amount of PAN.Moreover,the bimodal staggering phenomenon of PAN and PM_(2.5)provided a basis that PAN might aggravate haze through secondary organic aerosols(SOA)formation.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
Atmospheric carbonyls were measured at a semi-urban site in Orléans, France, from October 2010to July2011. Formaldehyde, acetaldehyde and acetone were found to be the most abundant carbonyls, with average concent...Atmospheric carbonyls were measured at a semi-urban site in Orléans, France, from October 2010to July2011. Formaldehyde, acetaldehyde and acetone were found to be the most abundant carbonyls, with average concentrations of 3.1, 1.0, 2.0 ppb, respectively in summer, 2.3, 0.7, 2.2 ppb, respectively in autumn, 2.2, 1.0, 2.1 ppb, respectively in spring,and 1.5, 0.7, 1.1 ppb, respectively in winter. Photo-oxidation of volatile organic compounds(VOCs) was found to make a remarkable contribution to atmospheric carbonyls in the semi-urban site based on the distinct seasonal and diurnal variations of the carbonyls, as well as the significantly positive correlations between the carbonyls and ozone. The significantly negative correlations between NO x and O_3 as well as the carbonyls and the positive correlations between wind speed and O_3 as well as the carbonyls implied that the carbonyls and O_3 at the semi-urban site were probably formed during air mass transport from neighboring cities.展开更多
The rate constants for the C1 atom reaction with three branched ketones have been measured at 298 ± 2 K and 760 Torr using the relative rate method in the absence of NO. The rate constants values obtained (in un...The rate constants for the C1 atom reaction with three branched ketones have been measured at 298 ± 2 K and 760 Torr using the relative rate method in the absence of NO. The rate constants values obtained (in units of 10^-10 cm^3/(molecule.sec)) are: k(2-methyl-3-pentanone) = 1.07 ± 0.26, k(3-methyl-2-pentanone) =1.21 ± 0.26, and k(4-methyl-2-pentanone) = 1.35 ± 0.27. Combining the chemical kinetic data obtained by this study with those reported for other ketones, a revised Structure Activity Relationship (SAR) parameter and R group reactivity (kR of R(O)R' and CHx (x = 1, 2, 3) group reactivity (kCHx) toward C1 atoms were proposed. In addition, the products from the three reactions in the presence of NO were also identified and quantified by using PTR-ToF-MS and GC-FID, and the yields of the identified products are: acetone (39% ± 8%) + ethanal (78% ± 12%), 2-butanone (22% ± 2%) + ethanal (75% ± 10%) + propanal (14% ± 1%) and acetone (26% ± 3%) + 2-methylpmpanal (24% ± 2%), for C1 atoms reaction with 2-methyl-3-pentanone, 3-methyl-2-pentanone and 4-methyl-2-pentanone, respectively. Based on the obtained results, the reaction mechanisms of C1 atoms with these three ketones are proposed.展开更多
Rate coefficients for the reaction of N03 radicals with 6 unsaturated volatile organic compounds(VOCs) in a 7300 L simulation chamber at ambient temperature and pressure have been determined by the relative rate metho...Rate coefficients for the reaction of N03 radicals with 6 unsaturated volatile organic compounds(VOCs) in a 7300 L simulation chamber at ambient temperature and pressure have been determined by the relative rate method.The resulting rate coefficients were determined for isoprene,2-carene,3-carene,methyl vinyl ketone(MVK),methacrolein(MACR)and crotonaldehyde(CA),as(6.6±0.8)×10-13,(1.8±0.6)×10-11,(8.7±0.5)×10-12,(1.24±1.04)×10-16,(3.3±0.9)×10-15 and(5.7±1.2)×10-15 cm3/(molecule·sec),respectively.The experiments indicate that NO3 radical reactions with all the studied unsaturated VOGs proceed through addition to the olefinic bond,however,it indicates that the introduction of a carbonyl group into unsaturated VOGs can deactivate the neighboring olefinic bond towards reaction with the NO3 radical,which is to be expected since the presence of these electronwithdrawing substituents will reduce the electron density in the π orbitals of the alkenes,and will therefore reduce the rate coefficient of these electrophilic addition reactions.In addition,we investigated the product formation from the reactions of 2-carene and 3-carene with the NO3 radical.Qualitative identification of an epoxide(C10H16OH+),caronaldehyde(C10H16O2 H+) and nitrooxy-ketone(C10H16O4 NH+) was achieved using a proton transfer reaction time-of-flight mass spectrometer(PTR-TOF-MS) and a reaction mechanism is proposed.展开更多
Air pollution as well as climate change and their possible effects on the environment, ecosystems and human health, are pressing challenges. Nowadays, it is dear that sustainable societal development cannot remain sol...Air pollution as well as climate change and their possible effects on the environment, ecosystems and human health, are pressing challenges. Nowadays, it is dear that sustainable societal development cannot remain solely wealth-oriented, but must take into account the present and future environmental issues. However, this approach is possible only if scientifically sound knowledge in all environmental areas becomes available to our societies and decision makers, which requires a firm scientific basis to our understanding of the processes guiding the atmospheric compositions.展开更多
The hygroscopicity and optical properties of alkylaminium sulfates (AASs) were investigated using a hygroscopicity tandem differential mobility analyzer coupled to a cavity ring-down spectrometer and a nephelometer....The hygroscopicity and optical properties of alkylaminium sulfates (AASs) were investigated using a hygroscopicity tandem differential mobility analyzer coupled to a cavity ring-down spectrometer and a nephelometer. AAS particles do not exhibit a deliquescence phenomenon and show a monotonic increase in diameter as the relative humidity (RH) ascends. Hygroscopic growth factors (GFs) for 40, 100 and 150 nm alkylaminium sulfate particles do not show an apparent Kelvin effect when RH is less than 45%, whereas GFs of the salt aerosols increase with initial particle size when RH is higher than 45%. Calculation using the Zdanovskii-Stokes-Robinson mixing rule suggests that hygroscopic growth of triethylaminium sulfate-ammonium sulfate mixtures is non-deliquescent, occurring at very low RH, implying that the displacement of ammonia by amine will significantly enhance the hygroscopicity of (NH4)2SO4 aerosols. In addition, light extinction of AAS particles is a combined effect of both scattering and absorption under dry conditions, but is dominated by scattering under wet conditions.展开更多
In the recent years, photocatalytic self-cleaning and "depolluting" materials have been suggested as a remediation technology mainly for NOx and aromatic VOCs in urban areas. A number of products incorporating the a...In the recent years, photocatalytic self-cleaning and "depolluting" materials have been suggested as a remediation technology mainly for NOx and aromatic VOCs in urban areas. A number of products incorporating the aforementioned technology have been made commercially available with the aim to improve urban air quality. These commercial products are based on the photocatalytic properties of a thin layer of TiO2 at the surface of the material (such as glass, pavement, etc.) or embedded in paints or concrete. The use of TiO2 photocatalysts as an emerging air pollution control technology has been reported in many locations worldwide. However, up to now, the effectiveness measured in situ and theexpected positive impact on air quality of this relatively new technology has only been demonstrated in a limited manner. Assessing and demonstrating the effectiveness of these depolluting techniques in real scale applications aims to create a real added value, in terms of policy making (i.e., implementing air quality strategies) and economics (by providing a demonstration of the actual performance of a new technique).展开更多
Airborne bacteria play key roles in terrestrial and marine ecosystems and human health,yet our understanding of bacterial communities and their response to the environmental variables lags significantly behind that of...Airborne bacteria play key roles in terrestrial and marine ecosystems and human health,yet our understanding of bacterial communities and their response to the environmental variables lags significantly behind that of other components of PM_(2.5).Here,atmospheric fine particles obtained from urban and suburb Shanghai were analyzed by using the qPCR and Illumina Miseq sequencing.The bacteria with an average concentration of 2.12× 10^(3 )cells/m^(3),were dominated by Sphingomonas,Curvibacter,Acinetobacter,Bradyrhizobium,Methylobacterium,Halomonas,Aliihoeflea,and Phyllobacterium,which were related to the nitrogen,carbon,sulfur cycling and human health risk.Our results provide a global survey of bacterial community across urban,suburb,and high-altitude sites.In Shanghai(China),urban PM2.5 harbour more diverse and dynamic bacterial populations than that in the suburb.The structural equation model explained about 27%,41%,and 20%^78%of the variance found in bacteria diversity,concentration,and discrepant genera among urban and suburb sites.This work furthered the knowledge of diverse bacteria in a coastal Megacity in the Yangtze river delta and emphasized the potential impact of environmental variables on bacterial community structure.展开更多
A sound scientific understanding of the factors affecting the environment is essential to guarantee the sustainable development of the world's economic and societal activities. Many environmental issues,such as air q...A sound scientific understanding of the factors affecting the environment is essential to guarantee the sustainable development of the world's economic and societal activities. Many environmental issues,such as air quality and climate展开更多
The heterogeneous degradation of nitrogen dioxide(NO2) on five samples of natural Icelandic volcanic particles has been investigated.Laboratory experiments were carried out under simulated atmospheric conditions using...The heterogeneous degradation of nitrogen dioxide(NO2) on five samples of natural Icelandic volcanic particles has been investigated.Laboratory experiments were carried out under simulated atmospheric conditions using a coated wall flow tube(CWFT).The CWFT reactor was coupled to a blue light nitrogen oxides analyzer(NOx analyzer),and a long path absorption photometer(LOPAP) to monitor in real time the concentrations of NO2,NO and HONO,respectively.Under dark and ambient relative humidity conditions,the steady state uptake coefficients of NO2 varied significantly between the volcanic samples probably due to differences in magma composition and morphological variation related with the density of surface OH groups.The irradiation of the surface with simulated sunlight enhanced the uptake coefficients by a factor of three indicating that photo-induced processes on the surface of the dust occur.Furthermore,the product yields of NO and HONO were determined under both dark and simulated sunlight conditions.The relative humidity was found to influence the distribution of gaseous products,promoting the formation of gaseous HONO.A detailed reaction mechanism is proposed that supports our experimental observations.Regarding the atmospheric implications,our results suggest that the NO2 degradation on volcanic particles and the corresponding formation of HONO is expected to be significant during volcanic dust storms or after a volcanic eruption.展开更多
One of the most important challenges the world is facing in this century is how to achieve sustained global development while balancing economic, societal and environmental considerations. It is clear that providing e...One of the most important challenges the world is facing in this century is how to achieve sustained global development while balancing economic, societal and environmental considerations. It is clear that providing everyone a healthy and wealthy society can only be achieved if upcoming policies and initiatives from policy makers are based on the most up-todate and validated scientific knowledge.展开更多
Clean air is essential to people's health and that of the environment.Since the industrial revolution,however,the quality of the air that people breathe has deteriorated considerably—mainly as a result of human acti...Clean air is essential to people's health and that of the environment.Since the industrial revolution,however,the quality of the air that people breathe has deteriorated considerably—mainly as a result of human activities.Rising industrial and energy production,the burning of fossil fuels and the dramatic rise in traffic all contribute to air pollution in our cities which,in turn,展开更多
基金supported by the VOLTAIRE project (ANR-10-LABX-100-01)funded by the ANR and the PIVOTS project provided by the Region Centre−Val de Loire (ARD 2020 program and CPER 2015−2020).
文摘Wildfire events are increasing globally which may be partly associated with climate change,resulting in significant adverse impacts on local,regional air quality and global climate.In September 2020,a small wildfire(burned area:36.3 ha)event occurred in Souesmes(Loiret-Cher,Sologne,France),and its plume spread out over 200 km on the following day as observed by the MODIS satellite.Based on measurements at a suburban site(~50 km northwest of the fire location)in Orléans and backward trajectory analysis,young wildfire plumes were characterized.Significant increases in gaseous pollutants(CO,CH_(4),N_(2)O,VOCs,etc.)and particles(including black carbon)were found within the wildfire plumes,leading to a reduced air quality.Emission factors,defined as EF(X)=ΔX/ΔCO(where,X represents the target species),of various trace gases and black carbon within the young wildfire plumes were determined accordingly and compared with previous studies.Changes in the ambient ions(such as ammonium,sulfate,nitrate,chloride,and nitrite in the particle-and gasphase)and aerosol properties(e.g.,aerosol water content,aerosol p H)were also quantified and discussed.Moreover,we estimated the total carbon and climate-related species(e.g.,CO_(2),CH_(4),N_(2)O,and BC)emissions and compared them with fire emission inventories.Current biomass burning emission inventories have uncertainties in estimating small fire burned areas and emissions.For instance,we found that the Global Fire Assimilation System(GFAS)may underestimate emissions(e.g.,CO)of this small wildfire while other inventories(GFED and FINN)showed significant overestimation.Considering that it is the first time to record wildfire plumes in this region,related atmospheric implications are presented and discussed.
基金supported by the National Natural Science Foundation of China (No. 41075094,40830101, 21177140,20977097)the National Basic Research and the Development Program (973) of China (No. 2010CB732304)+1 种基金the Special Fund for Environmental Research in the Public Interest (No. 201009001)the National Water Special Project (No. 2009ZX07210-009)
文摘The atmospheric concentrations of carbonyls and BTEX (benzene,toluene,ethylbenzene,m,p-xylene and o-xylene) were measured simultaneously at a same sampling site in Beijing from September 2008 to August 2010.The average concentrations of the total measured carbonyls during autumn,winter,spring,and summer were 37.7,31.3,39.7,50.5 μg/m 3,respectively,and maximal values for their diurnal variations usually happened at noontime.In contrast to carbonyls,the average concentrations of the total measured BTEX during the four seasons were 27.2,31.9,23.2,19.1 μg/m 3,respectively,andminimal values for their diurnal variations always occurred in the early afternoon.The average concentration for carbonyls increased about 24% from September 2008–August 2009 to September 2009–August 2010,for BTEX,increased about 15%.Integrated life time cancer risks for three carcinogens (benzene,formaldehyde and acetaldehyde) in Beijing exceeded the value of 1E-06,and the hazard quotient (HQ) of non-cancer risk of exposure to formaldehyde exceeded unity.
基金supported by the National Natural Science Foundation of China(Nos.91843301,91743202,41805091)Ministry of Science and Technology of China(No.2016YFC0202700)+1 种基金National research program for key issues in air pollution control(Nos.DQGG0103,DQGG0102)Marie Sk?odowska-Curie Actions(No.690958-MARSU-RISE-2015)
文摘As a secondary pollutant of photochemical pollution,peroxyacetyl nitrate(PAN)has attracted a close attention.A four-month campaign was conducted at a rural site in North China Plain(NCP)including the measurement of PAN,O_(3),NO_(x),PM_(2.5),oxygenated volatile organic compounds(OVOCs),photolysis rate constants of NO_(2)and O_(3)and meteorological parameters to investigate the wintertime characterization of photochemistry from November 2018 to February 2019.The results showed that the maximum and mean values of PAN were 4.38 and 0.93±0.67 ppbv during the campaign,respectively.The PAN under different PM_(2.5)concentrations from below 75μg/m^(3)up to 250μg/m^(3),showed different diurnal variation and formation rate.In the PM_(2.5)concentration range of above 250μg/m^(3),PAN had the largest daily mean value of 0.64 ppbv and the fastest production rate of 0.33 ppbv/hr.From the perspective of PAN’s production mechanism,the light intensity and precursors concentrations under different PM_(2.5)pollution levels indicated that there were sufficient light intensity and high volatile organic compounds(VOCs)and NO_(x)precursors concentration even under severe pollution level to generate a large amount of PAN.Moreover,the bimodal staggering phenomenon of PAN and PM_(2.5)provided a basis that PAN might aggravate haze through secondary organic aerosols(SOA)formation.
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 Region Centre of France, the Chinese National Natural Science Foundation (No.21307008)Changsha Science and Technology Project (No.K1403048-31)
文摘Atmospheric carbonyls were measured at a semi-urban site in Orléans, France, from October 2010to July2011. Formaldehyde, acetaldehyde and acetone were found to be the most abundant carbonyls, with average concentrations of 3.1, 1.0, 2.0 ppb, respectively in summer, 2.3, 0.7, 2.2 ppb, respectively in autumn, 2.2, 1.0, 2.1 ppb, respectively in spring,and 1.5, 0.7, 1.1 ppb, respectively in winter. Photo-oxidation of volatile organic compounds(VOCs) was found to make a remarkable contribution to atmospheric carbonyls in the semi-urban site based on the distinct seasonal and diurnal variations of the carbonyls, as well as the significantly positive correlations between the carbonyls and ozone. The significantly negative correlations between NO x and O_3 as well as the carbonyls and the positive correlations between wind speed and O_3 as well as the carbonyls implied that the carbonyls and O_3 at the semi-urban site were probably formed during air mass transport from neighboring cities.
基金supported by Labex Voltaire (ANR-10-LABX-100-01), ARD PIVOTS program (supported by the Centre-Val de Loire regional council)the European Union's Horizon 2020 Research and Innovation Programme through the EUROCHAMP2020 Infrastructure Activity under grant agreement No. 730997+1 种基金the China Scholarship Council for the financial supportsupported by the Natural Science Foundation of China (No. 41305124)
文摘The rate constants for the C1 atom reaction with three branched ketones have been measured at 298 ± 2 K and 760 Torr using the relative rate method in the absence of NO. The rate constants values obtained (in units of 10^-10 cm^3/(molecule.sec)) are: k(2-methyl-3-pentanone) = 1.07 ± 0.26, k(3-methyl-2-pentanone) =1.21 ± 0.26, and k(4-methyl-2-pentanone) = 1.35 ± 0.27. Combining the chemical kinetic data obtained by this study with those reported for other ketones, a revised Structure Activity Relationship (SAR) parameter and R group reactivity (kR of R(O)R' and CHx (x = 1, 2, 3) group reactivity (kCHx) toward C1 atoms were proposed. In addition, the products from the three reactions in the presence of NO were also identified and quantified by using PTR-ToF-MS and GC-FID, and the yields of the identified products are: acetone (39% ± 8%) + ethanal (78% ± 12%), 2-butanone (22% ± 2%) + ethanal (75% ± 10%) + propanal (14% ± 1%) and acetone (26% ± 3%) + 2-methylpmpanal (24% ± 2%), for C1 atoms reaction with 2-methyl-3-pentanone, 3-methyl-2-pentanone and 4-methyl-2-pentanone, respectively. Based on the obtained results, the reaction mechanisms of C1 atoms with these three ketones are proposed.
基金supported by Labex Voltaire(No.ANR-10-LABX100-01)the French National Research Agency(Agence Nationale de la Recherche)and the Research Grants Council(ANR-RGC)program(project ANR-16-CE01-0013)+2 种基金ARD PIVOTS program(Ambition Recherche Développement Plateformes d’Innovation,de Valorisation,d’Optimisation,Technologiques environnmentale S,supported by the centre-Val de Loire regional council)funding from the European Union’s Horizon 2020 research and innovation program through the EUROCHAMP-2020 Infrastructure Activity(No.730997)the Marie Sk?odowska Curie Actions Programme(No.690958)(MARSU)
文摘Rate coefficients for the reaction of N03 radicals with 6 unsaturated volatile organic compounds(VOCs) in a 7300 L simulation chamber at ambient temperature and pressure have been determined by the relative rate method.The resulting rate coefficients were determined for isoprene,2-carene,3-carene,methyl vinyl ketone(MVK),methacrolein(MACR)and crotonaldehyde(CA),as(6.6±0.8)×10-13,(1.8±0.6)×10-11,(8.7±0.5)×10-12,(1.24±1.04)×10-16,(3.3±0.9)×10-15 and(5.7±1.2)×10-15 cm3/(molecule·sec),respectively.The experiments indicate that NO3 radical reactions with all the studied unsaturated VOGs proceed through addition to the olefinic bond,however,it indicates that the introduction of a carbonyl group into unsaturated VOGs can deactivate the neighboring olefinic bond towards reaction with the NO3 radical,which is to be expected since the presence of these electronwithdrawing substituents will reduce the electron density in the π orbitals of the alkenes,and will therefore reduce the rate coefficient of these electrophilic addition reactions.In addition,we investigated the product formation from the reactions of 2-carene and 3-carene with the NO3 radical.Qualitative identification of an epoxide(C10H16OH+),caronaldehyde(C10H16O2 H+) and nitrooxy-ketone(C10H16O4 NH+) was achieved using a proton transfer reaction time-of-flight mass spectrometer(PTR-TOF-MS) and a reaction mechanism is proposed.
文摘Air pollution as well as climate change and their possible effects on the environment, ecosystems and human health, are pressing challenges. Nowadays, it is dear that sustainable societal development cannot remain solely wealth-oriented, but must take into account the present and future environmental issues. However, this approach is possible only if scientifically sound knowledge in all environmental areas becomes available to our societies and decision makers, which requires a firm scientific basis to our understanding of the processes guiding the atmospheric compositions.
基金supported by the National Natural Science Foundation of China(Nos.21190053,21177025,20937001)the Shanghai Science and Technology Commission of Shanghai Municipality(No.12DJ1400100,13XD1400700)+2 种基金the Priority Fields for Ph.D.Programs Foundation of Ministry of Education of China(No.20110071130003)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB05010200)FP7 Project(AMIS)(No.PIRSES-GA-2011)
文摘The hygroscopicity and optical properties of alkylaminium sulfates (AASs) were investigated using a hygroscopicity tandem differential mobility analyzer coupled to a cavity ring-down spectrometer and a nephelometer. AAS particles do not exhibit a deliquescence phenomenon and show a monotonic increase in diameter as the relative humidity (RH) ascends. Hygroscopic growth factors (GFs) for 40, 100 and 150 nm alkylaminium sulfate particles do not show an apparent Kelvin effect when RH is less than 45%, whereas GFs of the salt aerosols increase with initial particle size when RH is higher than 45%. Calculation using the Zdanovskii-Stokes-Robinson mixing rule suggests that hygroscopic growth of triethylaminium sulfate-ammonium sulfate mixtures is non-deliquescent, occurring at very low RH, implying that the displacement of ammonia by amine will significantly enhance the hygroscopicity of (NH4)2SO4 aerosols. In addition, light extinction of AAS particles is a combined effect of both scattering and absorption under dry conditions, but is dominated by scattering under wet conditions.
文摘In the recent years, photocatalytic self-cleaning and "depolluting" materials have been suggested as a remediation technology mainly for NOx and aromatic VOCs in urban areas. A number of products incorporating the aforementioned technology have been made commercially available with the aim to improve urban air quality. These commercial products are based on the photocatalytic properties of a thin layer of TiO2 at the surface of the material (such as glass, pavement, etc.) or embedded in paints or concrete. The use of TiO2 photocatalysts as an emerging air pollution control technology has been reported in many locations worldwide. However, up to now, the effectiveness measured in situ and theexpected positive impact on air quality of this relatively new technology has only been demonstrated in a limited manner. Assessing and demonstrating the effectiveness of these depolluting techniques in real scale applications aims to create a real added value, in terms of policy making (i.e., implementing air quality strategies) and economics (by providing a demonstration of the actual performance of a new technique).
基金by the Shanghai Sailing Program(19YF1403200)National Natural Science Foundation of China(Grant Nos.21906023,91843301,91743202,21527814)+2 种基金Ministry of Science and Technology of China(No.2016YFC0202700)Marie Skto-dowska-Curie Actions(690958-MARSU-RISE-2015)China Postdoctoral Science Foundation(No.2018M640331).
文摘Airborne bacteria play key roles in terrestrial and marine ecosystems and human health,yet our understanding of bacterial communities and their response to the environmental variables lags significantly behind that of other components of PM_(2.5).Here,atmospheric fine particles obtained from urban and suburb Shanghai were analyzed by using the qPCR and Illumina Miseq sequencing.The bacteria with an average concentration of 2.12× 10^(3 )cells/m^(3),were dominated by Sphingomonas,Curvibacter,Acinetobacter,Bradyrhizobium,Methylobacterium,Halomonas,Aliihoeflea,and Phyllobacterium,which were related to the nitrogen,carbon,sulfur cycling and human health risk.Our results provide a global survey of bacterial community across urban,suburb,and high-altitude sites.In Shanghai(China),urban PM2.5 harbour more diverse and dynamic bacterial populations than that in the suburb.The structural equation model explained about 27%,41%,and 20%^78%of the variance found in bacteria diversity,concentration,and discrepant genera among urban and suburb sites.This work furthered the knowledge of diverse bacteria in a coastal Megacity in the Yangtze river delta and emphasized the potential impact of environmental variables on bacterial community structure.
文摘A sound scientific understanding of the factors affecting the environment is essential to guarantee the sustainable development of the world's economic and societal activities. Many environmental issues,such as air quality and climate
基金the frame of Labex chemical and physical properties of the atmosphere(Labex Ca PPA)project,funded by agence nationale de la recherché(ANR)through the program d’investissements d’avenir(PIA)(No.ANR-11LABX-0005-01)contrat de planétat-région changement climatique dynamique de l’atmosphère impacts sur la biodiversitéet la santéhumaine(CPER CLIMIBIO)project,funded by the hauts-de-france regional council and the european regional development fund(ERDF)+1 种基金partly funded by the Czech Science Foundation under the’the role of high latitude dust in changing climate’(HLD-CHANGE)project(No.20-06168Y)the INSU LEFE-CHAT program for financial support
文摘The heterogeneous degradation of nitrogen dioxide(NO2) on five samples of natural Icelandic volcanic particles has been investigated.Laboratory experiments were carried out under simulated atmospheric conditions using a coated wall flow tube(CWFT).The CWFT reactor was coupled to a blue light nitrogen oxides analyzer(NOx analyzer),and a long path absorption photometer(LOPAP) to monitor in real time the concentrations of NO2,NO and HONO,respectively.Under dark and ambient relative humidity conditions,the steady state uptake coefficients of NO2 varied significantly between the volcanic samples probably due to differences in magma composition and morphological variation related with the density of surface OH groups.The irradiation of the surface with simulated sunlight enhanced the uptake coefficients by a factor of three indicating that photo-induced processes on the surface of the dust occur.Furthermore,the product yields of NO and HONO were determined under both dark and simulated sunlight conditions.The relative humidity was found to influence the distribution of gaseous products,promoting the formation of gaseous HONO.A detailed reaction mechanism is proposed that supports our experimental observations.Regarding the atmospheric implications,our results suggest that the NO2 degradation on volcanic particles and the corresponding formation of HONO is expected to be significant during volcanic dust storms or after a volcanic eruption.
文摘One of the most important challenges the world is facing in this century is how to achieve sustained global development while balancing economic, societal and environmental considerations. It is clear that providing everyone a healthy and wealthy society can only be achieved if upcoming policies and initiatives from policy makers are based on the most up-todate and validated scientific knowledge.
文摘Clean air is essential to people's health and that of the environment.Since the industrial revolution,however,the quality of the air that people breathe has deteriorated considerably—mainly as a result of human activities.Rising industrial and energy production,the burning of fossil fuels and the dramatic rise in traffic all contribute to air pollution in our cities which,in turn,