Acetaldehyde plays a significant role in atmospheric photochemical reactions and ozone formation.Previous studies have shown that acetaldehyde may rapidly be generated over short periods and impact ozone production,ye...Acetaldehyde plays a significant role in atmospheric photochemical reactions and ozone formation.Previous studies have shown that acetaldehyde may rapidly be generated over short periods and impact ozone production,yet the underlyingmechanism remains unclear.To better elucidate thesemechanisms,a field campaign was conducted in Dongying,a typical petrochemical city in China.The observed acetaldehyde concentration averaged 3.0±1.6 ppbv,with a peak around 09:00 local time.The diurnal variations of acetaldehyde were categorized into two types,with Category 1 exhibiting relatively high values and increasing sharply in concentration between 07:00 and 09:00 a.m.(refer to morning peak episode,MPE),and the remaining classified as Category 2.Category 1 was similar to previous studies at heavily polluted sites but differed fromcleaner locations.Using an observation-based chemical box model,we found that acetaldehyde contributed an average of 10.2%to the net ozone production rate.Combined with a positive matrix factorizationmodel,we identified secondary formation as the dominant source of acetaldehyde(45.0%),and the daytime production rate of acetaldehyde in Category 1 was significantly higher than that in Category 2.Cis-2-butene and trans-2-butene were identified as key precursors for the rapid acetaldehyde formation during the MEP,with the petroleum industry being their primary source.Volatile organic compounds(VOCs)from petroleum industry contributed over 60%to acetaldehyde formation during the morning peak.Our findings underscore the urgent need for targeted VOCs management strategies in petroleum sector tomitigate both carbonyl and ozone formation.展开更多
Fugitive emission from industrial sources may result in ozone formation and health risk,while the exact contribution of this source remains incompletely understood.In this study,emission characteristics,ozone formatio...Fugitive emission from industrial sources may result in ozone formation and health risk,while the exact contribution of this source remains incompletely understood.In this study,emission characteristics,ozone formation potential(OFP)and health risk of fugitive VOCs in7 representative industries were investigated.Chemical material industry was the dominant contributor to VOCs of fugitive emission in comparison with other industries.The OFP of VOCs from fugitive emission was in the range of 1.45×10^(3)-3.98×10^(5)μg/m^(3),with a higher value than that of organized emission in seven industries except for the coking industry and the chemical material industry,suggesting that fugitive VOCs should be taken into account while developing control strategies.Acetaldehyde,m,p-xylene,n-nonane,ethylene,vinyl chloridethe and other high OFP-contributing species were the major reactive species that should be targeted.Health risk assessment investigated non-cancer and cancer risks of fugitive VOCs in 7 industries were all above safe level(HR>1 and LCR>1×10^(-4)),posing remarkable health threats to human health.OVOCs were the main contributor to non-cancer risk,while halohydrocarbons and aromatics contributed most to cancer risks,posing remarkable health threat on human health.Our findings highlighted the contribution of fugitive VOCs on ozone formation and health risk was underestimated,indicating which should be considered in emission control strategies of industrial sources.展开更多
Fifteen heavy-duty diesel vehicles were tested on chassis dynamometer by using typical heavy duty driving cycle and fuel economy cycle. The air from the exhaust was sampled by 2,4- dinitrophenyhydrazine cartridge and ...Fifteen heavy-duty diesel vehicles were tested on chassis dynamometer by using typical heavy duty driving cycle and fuel economy cycle. The air from the exhaust was sampled by 2,4- dinitrophenyhydrazine cartridge and 23 carbonyl compounds were analyzed by high performance liquid chromatography. The average emission factor of carbonyls was 97.2 mg/km, higher than that of light-duty diesel vehicles and gasoline-powered vehicles. Formaldehyde, acetaldehyde, acetone and propionaidehyde were the species with the highest emission factors. Main influencing factors for carbonyl emissions were vehicle type, average speed and regulated emission standard, and the impact of vehicle loading was not evident in this study. National emission of carbonyls from diesel vehicles exhaust was calculated for China, 2011, based on both vehicle miles traveled and fuel consumption. Carbonyl emission of diesel vehicle was estimated to be 45.8 Gg, and was comparable to gasolinepowered vehicles （58.4 Gg）. The emissions of formaldehyde, acetaldehyde and acetone were 12.6, 6.9, 3.8 Gg, respectively. The ozone formation potential of carbonyls from diesel vehicles exhaust was 537 mg O3/km, higher than 497 mg O3/km of none-methane hydrocarbons emitted from diesel vehicles.展开更多
Observation-based method for O_(3)formation sensitivity research is an important tool to analyze the causes of ground-level O_(3)pollution,which has broad application potentials in determining the O_(3)pollution forma...Observation-based method for O_(3)formation sensitivity research is an important tool to analyze the causes of ground-level O_(3)pollution,which has broad application potentials in determining the O_(3)pollution formation mechanism and developing prevention and control strategies.This paper outlined the development history of research on O_(3)formation sensitivity based on observational methods,described the principle and applicability of the methodology,summarized the relative application results in China and provided recommendations on the prevention and control of O_(3)pollution in China based on relevant study results,and finally pointed out the shortcomings and future development prospects in this field in China.The overview study showed that the O_(3)formation sensitivity in some urban areas in China in recent years presented a gradual shifting tendency from the VOC-limited regime to the transition regime or the NO_(x)-limited regime due to the implementation of the O_(3)precursors emission reduction policies;O_(3)pollution control strategies and precursor control countermeasures should be formulated based on local conditions and the dynamic control capability of O_(3)pollution control measures should be improved.There are still some current deficiencies in the study field in China.Therefore,it is recommended that a stereoscopic monitoring network for atmospheric photochemical components should be further constructed and improved;the atmospheric chemical mechanisms should be vigorously developed,and standardized methods for determining the O_(3)formation sensitivity should be established in China in the near future.展开更多
Severe ground-level ozone(O_(3))pollution over major Chinese cities has become one of the most challenging problems,which have deleterious effects on human health and the sustainability of society.This study explored ...Severe ground-level ozone(O_(3))pollution over major Chinese cities has become one of the most challenging problems,which have deleterious effects on human health and the sustainability of society.This study explored the spatiotemporal distribution characteristics of ground-level O_(3) and its precursors based on conventional pollutant and meteorological monitoring data in Zhejiang Province from 2016 to 2021.Then,a high-performance convolutional neural network(CNN)model was established by expanding the moment and the concentration variations to general factors.Finally,the response mechanism of O_(3) to the variation with crucial influencing factors is explored by controlling variables and interpolating target variables.The results indicated that the annual average MDA8-90th concentrations in Zhejiang Province are higher in the northern and lower in the southern.When the wind direction(WD)ranges from east to southwest and the wind speed(WS)ranges between 2 and 3 m/sec,higher O_(3) concentration prone to occur.At different temperatures(T),the O_(3) concentration showed a trend of first increasing and subsequently decreasing with increasing NO_(2) concentration,peaks at the NO_(2) concentration around 0.02mg/m^(3).The sensitivity of NO_(2) to O_(3) formation is not easily affected by temperature,barometric pressure and dew point temperature.Additionally,there is a minimum IRNO_(2) at each temperature when the NO_(2) concentration is 0.03 mg/m^(3),and this minimum IRNO_(2) decreases with increasing temperature.The study explores the response mechanism of O_(3) with the change of driving variables,which can provide a scientific foundation and methodological support for the targeted management of O_(3) pollution.展开更多
Volatile organic compounds(VOCs)are the important precursors of the tropospheric ozone(O3)and secondary organic aerosols(SOA),both of which are known to harm human health and disrupt the earth’s climate system.In thi...Volatile organic compounds(VOCs)are the important precursors of the tropospheric ozone(O3)and secondary organic aerosols(SOA),both of which are known to harm human health and disrupt the earth’s climate system.In this study,VOC emission factors,O3 and SOA formation potentials were estimated for two types of industrial boilers:coal-fired boilers(n=3)and oil-fired boilers(n=3).Results showed that EVOCs concentrations were more than nine times higher for oil-fire d boilers compared to those for coal-fired boilers.Emission factors ofΣVOCs were found to be higher for oil-fired boilers(9.26-32.83 mg-VOC/kg)than for coal-fired boilers(1.57-4.13 mg-VOC/kg).Alkanes and aromatics were obtained as the most abundant groups in coal-fired boilers,while oxygenated organics and aromatics were the most contributing groups in oil-fired boilers.Benzene,n-hexane and o-ethyl toluene were the abundant VOC species in coal-fired boiler emissions,whereas toluene was the most abundant VOC species emitted from oil-fired boilers.O3 and SOA formation potentials were found 12 and 18 times,respectively,higher for oil-fired than for coal-fired boilers.Total OFP ranged from 3.99 to 11.39 mg-O3/kg for coal-fired boilers.For oil-fired boilers,total OFP ranged from 36.16 to 131.93 mg-O3/kg.Moreover,total secondary organic aerosol potential(SOAP)ranged from 65.4 to 122.5 mg-SOA/kg and 779.9 to 2252.5 mg-SOA/kg for the coal-fired and oil-fired boilers,respectively.展开更多
Toxic air pollutants(TAPs)are a class of airborne chemicals known or suspected to cause serious health issues.This study,applying positive matrix factorization and inhalation unit risk estimates of TAPs,quantifies the...Toxic air pollutants(TAPs)are a class of airborne chemicals known or suspected to cause serious health issues.This study,applying positive matrix factorization and inhalation unit risk estimates of TAPs,quantifies the changes in significant sources contributing to inhalation cancer risks(ICRs)from 2000 to 2020 in Hong Kong,China.Total ICR decreased from 1701 to 451 cases per million between 2000−2004 and 2016−2020,largely attributed to the reduction in diesel particulate matter(DPM),gasoline and solvent use-related volatile organic compounds(VOCs),and coal/biomass combustion-related polycyclic aromatic hydrocarbons and metal(loid)s.The regional contribution of VOCs associated with industrial and halogenated solvent sources increased substantially,representing the largest non-DPM ICR contributor(37%)in 2016−2020,stressing the need for a more comprehensive risk evaluation across the fast-growing and densely populated Greater Bay Area(GBA).ICRs in Hong Kong and the GBA will likely remain over 100 cases per million by 2050.The contributions to ozone formation potential of VOC/carbonyl sources were quantified,which show a notable shift from being solvent/gasoline-dominant in 2000−2004 to being more evenly shared by various sources in 2016−2020.Establishing a similar TAP monitoring network in the GBA is anticipated to provide the monitoring data needed to facilitate the development of more informed air quality management strategies.展开更多
Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previo...Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previous research,providing a long-term perspective on carbonyl compound variations and their environmental implica-tions.Atmospheric observations were conducted at Beijing(BJ)and Xianghe(XH)during the summer and winter months of 2018,2019,and 2023 to study the sources and impacts of carbonyl compounds in typical urban areas and peri‑urban areas.Notably,concentrations in the summer of 2023 increased compared to 2018 and 2019.The predominant carbonyl compounds—formaldehyde,acetaldehyde,and acetone—accounted for over 60%of the total.The mean values of OFP in BJ ranged from 18.55 to 58.61μg/m3,lower than those in XH(29.82 to 65.48μg/m3),with formaldehyde and acetaldehyde contributing over 80%of the total.SOAP exhibited a similar pattern,with values in XH(69.21 to 508.55μg/m3)significantly exceeding those in BJ(34.47 to 159.78μg/m3).The PMF model highlighted vehicle exhaust,secondary pollution,and biomass combustion as major sources of carbonyl compounds,emphasizing differences in source contributions between the two regions.This study’s com-parative analysis over different years and locations provides new insights into the dynamic changes in carbonyl compounds and their environmental importance.These results not only reinforce the importance of carbonyl compounds regulation but also offer a valuable reference for evaluating and refining emission control strategies during this period.展开更多
In this study,we conducted an observation experiment from May 1 to June 30,2018 in Zhengzhou,a major city in central China,where ground ozone(O3)pollution has become serious in recent years.The concentrations of O3 an...In this study,we conducted an observation experiment from May 1 to June 30,2018 in Zhengzhou,a major city in central China,where ground ozone(O3)pollution has become serious in recent years.The concentrations of O3 and its precursors,as well as H2O_(2) and meteorological data were obtained from the urban site(Yanchang,YC),suburban(Zhengzhou University,ZZU)and background sites(Ganglishuiku,GLSK).Result showed that the rates of O3 concentration exceeded Chinese National Air Quality Standard GradeⅡ(93.3 ppbv)were 59.0%,52.5%,and 55.7%at the above three sites with good consistency,respectively,indicating that O3 pollution is a regional problem in Zhengzhou.The daily peak O3 appeared at 15:00-16:00,which was opposite to VOCs,NOx,and CO and consistent with H2O_(2).The exhaustive statistical analysis of meteorological factors and chemical effects on O3 formation at YC was advanced.The high concentration of precursors,high temperature,low relative humidity,and moderately high wind speed together with the wind direction dominated by south and southeast wind contribute to urban O3 episodes in Zhengzhou.O3 formation analysis showed that reactive alkenes such as isoprene and cis-2-butene contributed most to O3 formation.The VOCs/NOx ratio and smog production model were used to determine O3-VOC-NOx sensitivity.The O3 formation in Zhengzhou during early summer was mainly under VOC-limited and transition regions alternately,which implies that the simultaneous emission reduction of alkenes and NOx is effective in reducing O3 pollution in Zhengzhou.展开更多
In recent years,many cities have taken measures to reduce volatile organic compounds(VOCs),an important precursor of ozone(O_(3)),to alleviate O_(3) pollution in China.116 VOC species were measured by online and offli...In recent years,many cities have taken measures to reduce volatile organic compounds(VOCs),an important precursor of ozone(O_(3)),to alleviate O_(3) pollution in China.116 VOC species were measured by online and offline methods in the urban area of Jiaozuo from May to October in 2021 to analyze the compositional characteristics.VOC sources were analyzed by a positive matrix factorization(PMF)model,and the sensitivity of ozone generation was determined by ozone isopleth plotting research(OZIPR)simulation.The results showed that the average volume concentration of total VOCs was 30.54 ppbv and showed a bimodal feature due to the rush-hour traffic in the morning and at nightfall.The most dominant VOC groups were oxygenated VOCs(OVOCs,29.3%)and alkanes(26.7%),and the most abundant VOC species were acetone and acetylene.However,based on the maximum incremental reactivity(MIR)method,the major VOC groups in terms of ozone formation potential(OFP)contribution were OVOCs(68.09μg/m^(3),31.5%),aromatics(62.90μg/m^(3),29.1%)and alkene/alkynes(54.90μg/m^(3),25.4%).This indicates that the control of OVOCs,aromatics and alkene/alkynes should take priority.Five sources of VOCs were quantified by PMF,including fixed sources of fossil fuel combustion(27.8%),industrial processes(25.9%),vehicle exhaust(19.7%),natural and secondary formation(13.9%)and solvent usage(12.7%).The empirical kinetic modeling approach(EKMA)curve obtained by OZIPR on O_(3) exceedance days indicated that the O_(3) sensitivity varied in different months.The results provide theoretical support for O_(3) pollution prevention and control in Jiaozuo.展开更多
On-site measurements of volatile organic compounds(VOCs)in different streams of flue gas were carried out on a real coal-fired power plant using sampling bags and SUMMA canisters to collect gas samples,filters to coll...On-site measurements of volatile organic compounds(VOCs)in different streams of flue gas were carried out on a real coal-fired power plant using sampling bags and SUMMA canisters to collect gas samples,filters to collect particle samples.Gas chromatography-flame ionization detector/mass spectrometry and gas chromatography-mass spectrometry was the offline analysis method.We found that the total mass concentration of the tested 102 VOC species at the outlet of wet flue gas desulfuration device was(13456±47)μg·m^(-3),which contained aliphatic hydrocarbons(57.9%),aromatic hydrocarbons(26.8%),halogen-containing species(14.5%),and a small amount of oxygen-containing and nitrogencontaining species.The most abundant species were 1-hexene,n-hexane and 2-methylpentane.The top ten species in terms of mass fraction(with a total mass fraction of 75.3%)were mainly hydrocarbons with a carbon number of 6 or higher and halogenated hydrocarbons with a lower carbon number.The mass concentration of VOC species in the particle phase was significantly lower than that in the gas phase.The change of VOC mass concentrations along the air pollution control devices indicates that conventional pollutant control equipment had a limited effect on VOC reduction.Ozone formation potential calculations showed that aromatic hydrocarbons contributed the highest ozone formation(46.4%)due to their relatively high mass concentrations and MIR(maximum increment reactivity)values.展开更多
Fine particulate matter(PM_(2.5))and ozone(O_(3))pollutions are prevalent air quality issues in China.Volatile organic compounds(VOCs)have significant impact on the formation of O_(3)and secondary organic aerosols(SOA...Fine particulate matter(PM_(2.5))and ozone(O_(3))pollutions are prevalent air quality issues in China.Volatile organic compounds(VOCs)have significant impact on the formation of O_(3)and secondary organic aerosols(SOA)contributing PM_(2.5).Herein,we investigated 54 VOCs,O_(3)and SOA in Tianjin from June 2017 to May 2019 to explore the non-linear relationship among O_(3),SOA and VOCs.The monthly patterns of VOCs and SOA concentrations were characterized by peak values during October to March and reached a minimum from April to September,but the observed O_(3)was exactly the opposite.Machine learning methods resolved the importance of individual VOCs on O_(3)and SOA that alkenes(mainly ethylene,propylene,and isoprene)have the highest importance to O_(3)formation;alkanes(C_(n),n≥6)and aromatics were the main source of SOA formation.Machine learning methods revealed and emphasized the importance of photochemical consumptions of VOCs to O_(3)and SOA formation.Ozone formation potential(OFP)and secondary organic aerosol formation potential(SOAFP)calculated by consumed VOCs quantitatively indicated that more than 80%of the consumed VOCs were alkenes which dominated the O_(3)formation,and the importance of consumed aromatics and alkenes to SOAFP were 40.84%and 56.65%,respectively.Therein,isoprene contributed the most to OFP at 41.45%regardless of the season,while aromatics(58.27%)contributed the most to SOAFP in winter.Collectively,our findings can provide scientific evidence on policymaking for VOCs controls on seasonal scales to achieve effective reduction in both SOA and O_(3).展开更多
Photodegradation technology has been widely applied in the purification of industrial aromatic hydrocarbons.However,whether this technology efficiently removes the pollutants to prevent secondary pollution and health ...Photodegradation technology has been widely applied in the purification of industrial aromatic hydrocarbons.However,whether this technology efficiently removes the pollutants to prevent secondary pollution and health risk is still unclear.Here,the photodegradation processes of three xylenes were compared under designed reaction atmospheres and light sources.Xe lamp showed poor photodegradation ability toward xylenes,no matter in N_(2) or N_(2)+O_(2)system,while much higher photodegradation performance of xylenes were obtained under ultraviolet(UV)and vacuum ultraviolet(VUV)irradiation,especially in N_(2)+O_(2)+VUV system,where 97.9%of m-xylene,99.0%of o-xylene or 87.5%of p-xylene with the initial concentration of 860 mg/m^(3) was removed within 240 min.The xylenes underwent three processes of photo-isomerization,photodecomposition and photo-oxidation to produce intermediates of aromatics,alkanes and carbonyls.Among them,the photo-isomerization products showed the highest concentration percentage(e.g.,≥50%in o-xylene system),confirming that photo-isomerization reaction was the dominated photodegradation process of xylenes.Moreover,these isomerized products not only contributed about 97%and91%to the formation potential of O3(OFP)and secondary organic aerosols(SOAFP),but also displayed obvious non-carcinogenic risk,although one of photodecomposition product—benzene showed the highest occupational exposure risk.Therefore,the secondary pollution and health risks of photodegradation products of xylenes were non-ignorable,although the OFP,SOAFP and health risks of the generated products reduced at least 4.5 times in comparison with that of the degraded xylenes.The findings are helpful for the appropriate application of this technology in the purification of industrial organic waste gas.展开更多
N-nitrosodimethylamine（NDMA） is an emerging disinfection by-product which is formed during water disinfection in the presence of amine-based precursors. Ranitidine, as one kind of amine-based pharmaceuticals, has be...N-nitrosodimethylamine（NDMA） is an emerging disinfection by-product which is formed during water disinfection in the presence of amine-based precursors. Ranitidine, as one kind of amine-based pharmaceuticals, has been identified as NDMA precursor with high NDMA molar conversion during chloramination. This study focused on the characterization of NDMA formation during ozonation of ranitidine. Influences of operational variables（ozone dose, pH value） and water matrix on NDMA generation as well as ranitidine degradation were evaluated. The results indicate high reactivity of ranitidine with ozone.Dimethylamine（DMA） and NDMA were generated due to ranitidine oxidation. High pH value caused more NDMA accumulation. NDMA formation was inhibited under acid conditions（pH ≤ 5） mainly due to the protonation of amines. Water matrix such as HCO-3and humic acid impacted NDMA generation due to UOH scavenging. Compared with UOH,ozone molecules dominated the productions of DMA and NDMA. However, UOH was a critical factor in NDMA degradation. Transformation products of ranitidine during ozonation were identified using gas chromatography–mass spectrometry. Among these products, just DMA and N,N-dimethylformamide could contribute to NDMA formation due to the DMA group in the molecular structures. The NDMA formation pathway from ranitidine ozonation was also proposed.展开更多
VOCs(Volatile organic compounds)exert a vital role in ozone and secondary organic aerosol production,necessitating investigations into their concentration,chemical characteristics,and source apportionment for the effe...VOCs(Volatile organic compounds)exert a vital role in ozone and secondary organic aerosol production,necessitating investigations into their concentration,chemical characteristics,and source apportionment for the effective implementation of measures aimed at preventing and controlling atmospheric pollution.FromJuly to October 2020,onlinemonitoringwas conducted in the main urban area of Shijiazhuang to collect data on VOCs and analyze their concentrations and reactivity.Additionally,the PMF(positive matrix factorization)method was utilized to identify the VOCs sources.Results indicated that the TVOCs(total VOCs)concentration was(96.7±63.4μg/m^3),with alkanes exhibiting the highest concentration of(36.1±26.4μg/m^3),followed by OVOCs(16.4±14.4μg/m^3).The key active components were alkenes and aromatics,among which xylene,propylene,toluene,propionaldehyde,acetaldehyde,ethylene,and styrene played crucial roles as reactive species.The sources derived from PMF analysis encompassed vehicle emissions,solvent and coating sources,combustion sources,industrial emissions sources,as well as plant sources,the contribution of which were 37.80%,27.93%,16.57%,15.24%,and 2.46%,respectively.Hence,reducing vehicular exhaust emissions and encouraging neighboring industries to adopt low-volatile organic solvents and coatings should be prioritized to mitigate VOCs levels.展开更多
Initial success has been achieved in Hong Kong in controlling primary air pollutants,but ambient ozone levels kept increasing during the past three decades.Volatile organic compounds(VOCs)are important for mitigating ...Initial success has been achieved in Hong Kong in controlling primary air pollutants,but ambient ozone levels kept increasing during the past three decades.Volatile organic compounds(VOCs)are important for mitigating ozone pollution as its major precursors.This study analyzed VOC characteristics of roadside,suburban,and rural sites in Hong Kong to investigate their compositions,concentrations,and source contributions.Herewe showthat the TVOC concentrations were 23.05±13.24,12.68±15.36,and 5.16±5.48 ppbv for roadside,suburban,and rural sites between May 2015 to June 2019,respectively.By using Positive Matrix Factorization(PMF)model,six sources were identified at the roadside site over five years:Liquefied petroleum gas(LPG)usage(33%–46%),gasoline evaporation(8%–31%),aged air mass(11%–28%),gasoline exhaust(5%–16%),diesel exhaust(2%–16%)and fuel filling(75–9%).Similarly,six sources were distinguished at the suburban site,including LPG usage(30%–33%),solvent usage(20%–26%),diesel exhaust(14%–26%),gasoline evaporation(8%–16%),aged air mass(4%–11%),and biogenic emissions(2%–5%).At the rural site,four sources were identified,including aged airmass(33%–51%),solvent usage(25%–30%),vehicular emissions(11%–28%),and biogenic emissions(6%–12%).The analysis further revealed that fuel filling and LPG usage were the primary contributors to OFP and OH reactivity at the roadside site,while solvent usage and biogenic emissions accounted for almost half of OFP and OH reactivity at the suburban and rural sites,respectively.These findings highlight the importance of identifying and characterizing VOC sources at different sites to help policymakers develop targeted measures for pollution mitigation in specific areas.展开更多
Ambient volatile organic compounds （VOCs） were sampled at six sites in Beijing in the summer of 2004 and analyzed by GCMS. The chemical reactivities of 73 quantified VOCs species were evaluated by OH loss rates （LO...Ambient volatile organic compounds （VOCs） were sampled at six sites in Beijing in the summer of 2004 and analyzed by GCMS. The chemical reactivities of 73 quantified VOCs species were evaluated by OH loss rates （LOH） and ozone formation potentials （OFPs）. Top 15 reactive species, mainly alkenes and aromatics, were identified by these two methods, and accounted for more than 70% of total reactivity of VOCs. In urban areas, isoprene was the most reactive species in term of OH loss rate, contributing 11.4% to the LOH of VOCs. While toluene, accounting for 9.4% of OFPs, appeared to have a long-time role in the photochemical processes. Tongzhou site is obviously influenced by local chemical industry, but the other five sites showed typical urban features influenced mainly by vehicular emissions.展开更多
Volatile organic compounds(VOCs)are major contributors to air pollution.Based on the emission characteristics of 99 VOCs that daily measured at 10 am in winter from 15 December 2015 to 17 January 2016 and in summer fr...Volatile organic compounds(VOCs)are major contributors to air pollution.Based on the emission characteristics of 99 VOCs that daily measured at 10 am in winter from 15 December 2015 to 17 January 2016 and in summer from 21 July to 25 August 2016 in Beijing,the environmental impact and health risk of VOC were assessed.In the winter polluted days,the secondary organic aerosol formation potential(SOAP)of VOC(199.70±15.05 mg/m^3)was significantly higher than that on other days.And aromatics were the primary contributor(98.03%)to the SOAP during the observation period.Additionally,the result of the ozone formation potential(OFP)showed that ethylene contributed the most to OFP in winter(26.00%and 27.64%on the normal and polluted days).In summer,however,acetaldehyde was the primary contributor to OFP(22.00%and 21.61%on the normal and polluted days).Simultaneously,study showed that hazard ratios and lifetime cancer risk values of acrolein,chloroform,benzene,1,2-dichloroethane,acetaldehyde and 1,3-butadiene exceeded the thresholds established by USEPA,thereby presenting a health risk to the residents.Besides,the ratio of toluene-to-benzene indicated that vehicle exhausts were the main source of VOC pollution in Beijing.The ratio of m-/p-xylene-toethylbenzene demonstrated that there were more prominent atmospheric photochemical reactions in summer than that in winter.Finally,according to the potential source contribution function(PSCF)results,compared with local pollution sources,the spread of pollution from long-distance VOCs had a greater impact on Beijing.展开更多
Cooking process can produce abundant volatile organic compounds(VOCs),which are harmful to environment and human health.Therefore,we conducted a comprehensive analysis in which VOCs emissions from multiple cuisines ha...Cooking process can produce abundant volatile organic compounds(VOCs),which are harmful to environment and human health.Therefore,we conducted a comprehensive analysis in which VOCs emissions from multiple cuisines have been sampled based on the simulation and acquisition platform,involving concentration characteristics,ozone formation potential(OFP)and purification efficiency assessments.VOCs emissions varied from 1828.5 to 14,355.1μg/m^(3),with the maximumand minimumvalues fromBarbecue and Family cuisine,respectively.Alkanes and alcohol had higher contributions to VOCs from Sichuan and Hunan cuisine(64.1%),Family cuisine(66.3%),Shandong cuisine(69.1%)and Cantonese cuisine(69.8%),with the dominant VOCs species of ethanol,isobutane and n-butane.In comparison,alcohols(79.5%)were abundant for Huaiyang cuisine,while alkanes(19.7%),alkenes(35.9%)and haloalkanes(22.9%)accounted for higher proportions from Barbecue.Specially,carbon tetrachloride,n-hexylene and 1-butene were the most abundant VOCs species for Barbecue,ranging from 8.8%to 14.6%.The highest OFP occurred in Barbecue.The sensitive species of OFP for Huaiyang cuisine were alcohols,while other cuisines were alkenes.Purification efficiency assessments shed light on the removal differences of individual and synergistic control technologies.VOCs emissions exhibited a strong dependence on the photocatalytic oxidation,with the removal efficiencies of 29.0%–54.4%.However,the high voltage electrostatic,wet purification and mechanical separation techniques played a mediocre or even counterproductive role in the VOCs reduction,meanwhile collaborative control technologies could not significantly improve the removal efficiency.Our results identifiedmore effective control technologies,which were conductive to alleviating air pollution from cooking emissions.展开更多
基金supported by the National Key Research and Development Program of the Ministry of Science of Technology of China(No.2022YFC3701101)the National Natural Science Foundation of China(No.42105106)+2 种基金China Postdoctoral Science Foundation(No.2021M691921)the Ministry of Ecology and Environment of the People’s Republic of China(No.DQGG202121)Dongying Ecological and Environmental Bureau(No.2021DFKY-0779).
文摘Acetaldehyde plays a significant role in atmospheric photochemical reactions and ozone formation.Previous studies have shown that acetaldehyde may rapidly be generated over short periods and impact ozone production,yet the underlyingmechanism remains unclear.To better elucidate thesemechanisms,a field campaign was conducted in Dongying,a typical petrochemical city in China.The observed acetaldehyde concentration averaged 3.0±1.6 ppbv,with a peak around 09:00 local time.The diurnal variations of acetaldehyde were categorized into two types,with Category 1 exhibiting relatively high values and increasing sharply in concentration between 07:00 and 09:00 a.m.(refer to morning peak episode,MPE),and the remaining classified as Category 2.Category 1 was similar to previous studies at heavily polluted sites but differed fromcleaner locations.Using an observation-based chemical box model,we found that acetaldehyde contributed an average of 10.2%to the net ozone production rate.Combined with a positive matrix factorizationmodel,we identified secondary formation as the dominant source of acetaldehyde(45.0%),and the daytime production rate of acetaldehyde in Category 1 was significantly higher than that in Category 2.Cis-2-butene and trans-2-butene were identified as key precursors for the rapid acetaldehyde formation during the MEP,with the petroleum industry being their primary source.Volatile organic compounds(VOCs)from petroleum industry contributed over 60%to acetaldehyde formation during the morning peak.Our findings underscore the urgent need for targeted VOCs management strategies in petroleum sector tomitigate both carbonyl and ozone formation.
基金supported by the National Natural Science Foundation of China (No.42177420)。
文摘Fugitive emission from industrial sources may result in ozone formation and health risk,while the exact contribution of this source remains incompletely understood.In this study,emission characteristics,ozone formation potential(OFP)and health risk of fugitive VOCs in7 representative industries were investigated.Chemical material industry was the dominant contributor to VOCs of fugitive emission in comparison with other industries.The OFP of VOCs from fugitive emission was in the range of 1.45×10^(3)-3.98×10^(5)μg/m^(3),with a higher value than that of organized emission in seven industries except for the coking industry and the chemical material industry,suggesting that fugitive VOCs should be taken into account while developing control strategies.Acetaldehyde,m,p-xylene,n-nonane,ethylene,vinyl chloridethe and other high OFP-contributing species were the major reactive species that should be targeted.Health risk assessment investigated non-cancer and cancer risks of fugitive VOCs in 7 industries were all above safe level(HR>1 and LCR>1×10^(-4)),posing remarkable health threats to human health.OVOCs were the main contributor to non-cancer risk,while halohydrocarbons and aromatics contributed most to cancer risks,posing remarkable health threat on human health.Our findings highlighted the contribution of fugitive VOCs on ozone formation and health risk was underestimated,indicating which should be considered in emission control strategies of industrial sources.
基金supported by the Natural Science Foundation for Outstanding Young Scholars(No.41125018)the National Commonweal Project of the Ministry of Environmental Protection(No.201009057)
文摘Fifteen heavy-duty diesel vehicles were tested on chassis dynamometer by using typical heavy duty driving cycle and fuel economy cycle. The air from the exhaust was sampled by 2,4- dinitrophenyhydrazine cartridge and 23 carbonyl compounds were analyzed by high performance liquid chromatography. The average emission factor of carbonyls was 97.2 mg/km, higher than that of light-duty diesel vehicles and gasoline-powered vehicles. Formaldehyde, acetaldehyde, acetone and propionaidehyde were the species with the highest emission factors. Main influencing factors for carbonyl emissions were vehicle type, average speed and regulated emission standard, and the impact of vehicle loading was not evident in this study. National emission of carbonyls from diesel vehicles exhaust was calculated for China, 2011, based on both vehicle miles traveled and fuel consumption. Carbonyl emission of diesel vehicle was estimated to be 45.8 Gg, and was comparable to gasolinepowered vehicles （58.4 Gg）. The emissions of formaldehyde, acetaldehyde and acetone were 12.6, 6.9, 3.8 Gg, respectively. The ozone formation potential of carbonyls from diesel vehicles exhaust was 537 mg O3/km, higher than 497 mg O3/km of none-methane hydrocarbons emitted from diesel vehicles.
基金supported by the National Research Program for Key Issues in Air Pollution Control(No.DQGG202121)the Beijing Municipal Science&Technology Commission(No.Z181100005418015)+1 种基金National Natural Science Foundation of China(No.42075094)the National Research Program for Key Issue in Air Pollution Control(No.DQGG2021101)。
文摘Observation-based method for O_(3)formation sensitivity research is an important tool to analyze the causes of ground-level O_(3)pollution,which has broad application potentials in determining the O_(3)pollution formation mechanism and developing prevention and control strategies.This paper outlined the development history of research on O_(3)formation sensitivity based on observational methods,described the principle and applicability of the methodology,summarized the relative application results in China and provided recommendations on the prevention and control of O_(3)pollution in China based on relevant study results,and finally pointed out the shortcomings and future development prospects in this field in China.The overview study showed that the O_(3)formation sensitivity in some urban areas in China in recent years presented a gradual shifting tendency from the VOC-limited regime to the transition regime or the NO_(x)-limited regime due to the implementation of the O_(3)precursors emission reduction policies;O_(3)pollution control strategies and precursor control countermeasures should be formulated based on local conditions and the dynamic control capability of O_(3)pollution control measures should be improved.There are still some current deficiencies in the study field in China.Therefore,it is recommended that a stereoscopic monitoring network for atmospheric photochemical components should be further constructed and improved;the atmospheric chemical mechanisms should be vigorously developed,and standardized methods for determining the O_(3)formation sensitivity should be established in China in the near future.
基金supported by the National Key Research and Development Program of China (Nos.2022YFC3702000 and 2022YFC3703500)the Key R&D Project of Zhejiang Province (No.2022C03146).
文摘Severe ground-level ozone(O_(3))pollution over major Chinese cities has become one of the most challenging problems,which have deleterious effects on human health and the sustainability of society.This study explored the spatiotemporal distribution characteristics of ground-level O_(3) and its precursors based on conventional pollutant and meteorological monitoring data in Zhejiang Province from 2016 to 2021.Then,a high-performance convolutional neural network(CNN)model was established by expanding the moment and the concentration variations to general factors.Finally,the response mechanism of O_(3) to the variation with crucial influencing factors is explored by controlling variables and interpolating target variables.The results indicated that the annual average MDA8-90th concentrations in Zhejiang Province are higher in the northern and lower in the southern.When the wind direction(WD)ranges from east to southwest and the wind speed(WS)ranges between 2 and 3 m/sec,higher O_(3) concentration prone to occur.At different temperatures(T),the O_(3) concentration showed a trend of first increasing and subsequently decreasing with increasing NO_(2) concentration,peaks at the NO_(2) concentration around 0.02mg/m^(3).The sensitivity of NO_(2) to O_(3) formation is not easily affected by temperature,barometric pressure and dew point temperature.Additionally,there is a minimum IRNO_(2) at each temperature when the NO_(2) concentration is 0.03 mg/m^(3),and this minimum IRNO_(2) decreases with increasing temperature.The study explores the response mechanism of O_(3) with the change of driving variables,which can provide a scientific foundation and methodological support for the targeted management of O_(3) pollution.
文摘Volatile organic compounds(VOCs)are the important precursors of the tropospheric ozone(O3)and secondary organic aerosols(SOA),both of which are known to harm human health and disrupt the earth’s climate system.In this study,VOC emission factors,O3 and SOA formation potentials were estimated for two types of industrial boilers:coal-fired boilers(n=3)and oil-fired boilers(n=3).Results showed that EVOCs concentrations were more than nine times higher for oil-fire d boilers compared to those for coal-fired boilers.Emission factors ofΣVOCs were found to be higher for oil-fired boilers(9.26-32.83 mg-VOC/kg)than for coal-fired boilers(1.57-4.13 mg-VOC/kg).Alkanes and aromatics were obtained as the most abundant groups in coal-fired boilers,while oxygenated organics and aromatics were the most contributing groups in oil-fired boilers.Benzene,n-hexane and o-ethyl toluene were the abundant VOC species in coal-fired boiler emissions,whereas toluene was the most abundant VOC species emitted from oil-fired boilers.O3 and SOA formation potentials were found 12 and 18 times,respectively,higher for oil-fired than for coal-fired boilers.Total OFP ranged from 3.99 to 11.39 mg-O3/kg for coal-fired boilers.For oil-fired boilers,total OFP ranged from 36.16 to 131.93 mg-O3/kg.Moreover,total secondary organic aerosol potential(SOAP)ranged from 65.4 to 122.5 mg-SOA/kg and 779.9 to 2252.5 mg-SOA/kg for the coal-fired and oil-fired boilers,respectively.
基金supported by the Hong Kong Environmental Protection Department(Project 20-00424)supported by a fellowship award from the Research Grants Council of the HKSAR,China(HKUST PDFS2223-6S10).
文摘Toxic air pollutants(TAPs)are a class of airborne chemicals known or suspected to cause serious health issues.This study,applying positive matrix factorization and inhalation unit risk estimates of TAPs,quantifies the changes in significant sources contributing to inhalation cancer risks(ICRs)from 2000 to 2020 in Hong Kong,China.Total ICR decreased from 1701 to 451 cases per million between 2000−2004 and 2016−2020,largely attributed to the reduction in diesel particulate matter(DPM),gasoline and solvent use-related volatile organic compounds(VOCs),and coal/biomass combustion-related polycyclic aromatic hydrocarbons and metal(loid)s.The regional contribution of VOCs associated with industrial and halogenated solvent sources increased substantially,representing the largest non-DPM ICR contributor(37%)in 2016−2020,stressing the need for a more comprehensive risk evaluation across the fast-growing and densely populated Greater Bay Area(GBA).ICRs in Hong Kong and the GBA will likely remain over 100 cases per million by 2050.The contributions to ozone formation potential of VOC/carbonyl sources were quantified,which show a notable shift from being solvent/gasoline-dominant in 2000−2004 to being more evenly shared by various sources in 2016−2020.Establishing a similar TAP monitoring network in the GBA is anticipated to provide the monitoring data needed to facilitate the development of more informed air quality management strategies.
基金supported by the National Natural Science Foundation of China(Nos.41905108 and 42130704).
文摘Carbonyl compounds play a pivotal role in the formation of secondary pollutants such as O_(3) and SOA,signifi-cantly impacting air quality and human health.This study extended the observation period compared to previous research,providing a long-term perspective on carbonyl compound variations and their environmental implica-tions.Atmospheric observations were conducted at Beijing(BJ)and Xianghe(XH)during the summer and winter months of 2018,2019,and 2023 to study the sources and impacts of carbonyl compounds in typical urban areas and peri‑urban areas.Notably,concentrations in the summer of 2023 increased compared to 2018 and 2019.The predominant carbonyl compounds—formaldehyde,acetaldehyde,and acetone—accounted for over 60%of the total.The mean values of OFP in BJ ranged from 18.55 to 58.61μg/m3,lower than those in XH(29.82 to 65.48μg/m3),with formaldehyde and acetaldehyde contributing over 80%of the total.SOAP exhibited a similar pattern,with values in XH(69.21 to 508.55μg/m3)significantly exceeding those in BJ(34.47 to 159.78μg/m3).The PMF model highlighted vehicle exhaust,secondary pollution,and biomass combustion as major sources of carbonyl compounds,emphasizing differences in source contributions between the two regions.This study’s com-parative analysis over different years and locations provides new insights into the dynamic changes in carbonyl compounds and their environmental importance.These results not only reinforce the importance of carbonyl compounds regulation but also offer a valuable reference for evaluating and refining emission control strategies during this period.
基金the National Key Research and Development Program of China(No.2017YFC0212403)。
文摘In this study,we conducted an observation experiment from May 1 to June 30,2018 in Zhengzhou,a major city in central China,where ground ozone(O3)pollution has become serious in recent years.The concentrations of O3 and its precursors,as well as H2O_(2) and meteorological data were obtained from the urban site(Yanchang,YC),suburban(Zhengzhou University,ZZU)and background sites(Ganglishuiku,GLSK).Result showed that the rates of O3 concentration exceeded Chinese National Air Quality Standard GradeⅡ(93.3 ppbv)were 59.0%,52.5%,and 55.7%at the above three sites with good consistency,respectively,indicating that O3 pollution is a regional problem in Zhengzhou.The daily peak O3 appeared at 15:00-16:00,which was opposite to VOCs,NOx,and CO and consistent with H2O_(2).The exhaustive statistical analysis of meteorological factors and chemical effects on O3 formation at YC was advanced.The high concentration of precursors,high temperature,low relative humidity,and moderately high wind speed together with the wind direction dominated by south and southeast wind contribute to urban O3 episodes in Zhengzhou.O3 formation analysis showed that reactive alkenes such as isoprene and cis-2-butene contributed most to O3 formation.The VOCs/NOx ratio and smog production model were used to determine O3-VOC-NOx sensitivity.The O3 formation in Zhengzhou during early summer was mainly under VOC-limited and transition regions alternately,which implies that the simultaneous emission reduction of alkenes and NOx is effective in reducing O3 pollution in Zhengzhou.
基金supported by the Research Project Entrusted by Henan Ecological Environment Monitoring and Safety Center,China(No.20201557)the Study of Collaborative Prevention and Control of Fine Particulate Matter and Ozone Pollution of Jiaozuo(No.DQGG202134)。
文摘In recent years,many cities have taken measures to reduce volatile organic compounds(VOCs),an important precursor of ozone(O_(3)),to alleviate O_(3) pollution in China.116 VOC species were measured by online and offline methods in the urban area of Jiaozuo from May to October in 2021 to analyze the compositional characteristics.VOC sources were analyzed by a positive matrix factorization(PMF)model,and the sensitivity of ozone generation was determined by ozone isopleth plotting research(OZIPR)simulation.The results showed that the average volume concentration of total VOCs was 30.54 ppbv and showed a bimodal feature due to the rush-hour traffic in the morning and at nightfall.The most dominant VOC groups were oxygenated VOCs(OVOCs,29.3%)and alkanes(26.7%),and the most abundant VOC species were acetone and acetylene.However,based on the maximum incremental reactivity(MIR)method,the major VOC groups in terms of ozone formation potential(OFP)contribution were OVOCs(68.09μg/m^(3),31.5%),aromatics(62.90μg/m^(3),29.1%)and alkene/alkynes(54.90μg/m^(3),25.4%).This indicates that the control of OVOCs,aromatics and alkene/alkynes should take priority.Five sources of VOCs were quantified by PMF,including fixed sources of fossil fuel combustion(27.8%),industrial processes(25.9%),vehicle exhaust(19.7%),natural and secondary formation(13.9%)and solvent usage(12.7%).The empirical kinetic modeling approach(EKMA)curve obtained by OZIPR on O_(3) exceedance days indicated that the O_(3) sensitivity varied in different months.The results provide theoretical support for O_(3) pollution prevention and control in Jiaozuo.
基金funded by the National Natural Science Foundation of China(52006079)the Natural Science Foundation of Hubei Province(2020CFB247)the National Key Research and Development Program of China(2018YFB0605201)。
文摘On-site measurements of volatile organic compounds(VOCs)in different streams of flue gas were carried out on a real coal-fired power plant using sampling bags and SUMMA canisters to collect gas samples,filters to collect particle samples.Gas chromatography-flame ionization detector/mass spectrometry and gas chromatography-mass spectrometry was the offline analysis method.We found that the total mass concentration of the tested 102 VOC species at the outlet of wet flue gas desulfuration device was(13456±47)μg·m^(-3),which contained aliphatic hydrocarbons(57.9%),aromatic hydrocarbons(26.8%),halogen-containing species(14.5%),and a small amount of oxygen-containing and nitrogencontaining species.The most abundant species were 1-hexene,n-hexane and 2-methylpentane.The top ten species in terms of mass fraction(with a total mass fraction of 75.3%)were mainly hydrocarbons with a carbon number of 6 or higher and halogenated hydrocarbons with a lower carbon number.The mass concentration of VOC species in the particle phase was significantly lower than that in the gas phase.The change of VOC mass concentrations along the air pollution control devices indicates that conventional pollutant control equipment had a limited effect on VOC reduction.Ozone formation potential calculations showed that aromatic hydrocarbons contributed the highest ozone formation(46.4%)due to their relatively high mass concentrations and MIR(maximum increment reactivity)values.
基金financially supported by the National Key Research and Development Program of China(No.2018 YFE0106900)supported by National Natural Science Foundation of China(Nos.42077191,41775149)+2 种基金Fundamental Research Funds for the Central Universities(No.63213072)National Research Program for Key Issues in Air Pollution Control(No.DQGG-05-30)the Blue Sky Foundation
文摘Fine particulate matter(PM_(2.5))and ozone(O_(3))pollutions are prevalent air quality issues in China.Volatile organic compounds(VOCs)have significant impact on the formation of O_(3)and secondary organic aerosols(SOA)contributing PM_(2.5).Herein,we investigated 54 VOCs,O_(3)and SOA in Tianjin from June 2017 to May 2019 to explore the non-linear relationship among O_(3),SOA and VOCs.The monthly patterns of VOCs and SOA concentrations were characterized by peak values during October to March and reached a minimum from April to September,but the observed O_(3)was exactly the opposite.Machine learning methods resolved the importance of individual VOCs on O_(3)and SOA that alkenes(mainly ethylene,propylene,and isoprene)have the highest importance to O_(3)formation;alkanes(C_(n),n≥6)and aromatics were the main source of SOA formation.Machine learning methods revealed and emphasized the importance of photochemical consumptions of VOCs to O_(3)and SOA formation.Ozone formation potential(OFP)and secondary organic aerosol formation potential(SOAFP)calculated by consumed VOCs quantitatively indicated that more than 80%of the consumed VOCs were alkenes which dominated the O_(3)formation,and the importance of consumed aromatics and alkenes to SOAFP were 40.84%and 56.65%,respectively.Therein,isoprene contributed the most to OFP at 41.45%regardless of the season,while aromatics(58.27%)contributed the most to SOAFP in winter.Collectively,our findings can provide scientific evidence on policymaking for VOCs controls on seasonal scales to achieve effective reduction in both SOA and O_(3).
基金supported by the National Natural Science Foundation of China (Nos.42177354 and 21777032)the National Key R&D Program of China (No.2019YFC0214402)the Guangdong Basic and Applied Basic Research oundation (No.2019B151502064)。
文摘Photodegradation technology has been widely applied in the purification of industrial aromatic hydrocarbons.However,whether this technology efficiently removes the pollutants to prevent secondary pollution and health risk is still unclear.Here,the photodegradation processes of three xylenes were compared under designed reaction atmospheres and light sources.Xe lamp showed poor photodegradation ability toward xylenes,no matter in N_(2) or N_(2)+O_(2)system,while much higher photodegradation performance of xylenes were obtained under ultraviolet(UV)and vacuum ultraviolet(VUV)irradiation,especially in N_(2)+O_(2)+VUV system,where 97.9%of m-xylene,99.0%of o-xylene or 87.5%of p-xylene with the initial concentration of 860 mg/m^(3) was removed within 240 min.The xylenes underwent three processes of photo-isomerization,photodecomposition and photo-oxidation to produce intermediates of aromatics,alkanes and carbonyls.Among them,the photo-isomerization products showed the highest concentration percentage(e.g.,≥50%in o-xylene system),confirming that photo-isomerization reaction was the dominated photodegradation process of xylenes.Moreover,these isomerized products not only contributed about 97%and91%to the formation potential of O3(OFP)and secondary organic aerosols(SOAFP),but also displayed obvious non-carcinogenic risk,although one of photodecomposition product—benzene showed the highest occupational exposure risk.Therefore,the secondary pollution and health risks of photodegradation products of xylenes were non-ignorable,although the OFP,SOAFP and health risks of the generated products reduced at least 4.5 times in comparison with that of the degraded xylenes.The findings are helpful for the appropriate application of this technology in the purification of industrial organic waste gas.
基金supported by the National Natural Science Foundation of China (Nos.50878165 and no.51608322)
文摘N-nitrosodimethylamine（NDMA） is an emerging disinfection by-product which is formed during water disinfection in the presence of amine-based precursors. Ranitidine, as one kind of amine-based pharmaceuticals, has been identified as NDMA precursor with high NDMA molar conversion during chloramination. This study focused on the characterization of NDMA formation during ozonation of ranitidine. Influences of operational variables（ozone dose, pH value） and water matrix on NDMA generation as well as ranitidine degradation were evaluated. The results indicate high reactivity of ranitidine with ozone.Dimethylamine（DMA） and NDMA were generated due to ranitidine oxidation. High pH value caused more NDMA accumulation. NDMA formation was inhibited under acid conditions（pH ≤ 5） mainly due to the protonation of amines. Water matrix such as HCO-3and humic acid impacted NDMA generation due to UOH scavenging. Compared with UOH,ozone molecules dominated the productions of DMA and NDMA. However, UOH was a critical factor in NDMA degradation. Transformation products of ranitidine during ozonation were identified using gas chromatography–mass spectrometry. Among these products, just DMA and N,N-dimethylformamide could contribute to NDMA formation due to the DMA group in the molecular structures. The NDMA formation pathway from ranitidine ozonation was also proposed.
基金supported by the Natural Science Foundation of Hebei Province(Nos.D2019106042,D2020304038,and D2021106002)the National Natural Science Foundation of China(No.22276099)+1 种基金the State Environmental Protection Key Laboratory of Formation and Prevention of Urban Air Pollution Complex(No.2021080544)the Environmental Monitoring Research Foundation of Jiangsu Province(No.2211).
文摘VOCs(Volatile organic compounds)exert a vital role in ozone and secondary organic aerosol production,necessitating investigations into their concentration,chemical characteristics,and source apportionment for the effective implementation of measures aimed at preventing and controlling atmospheric pollution.FromJuly to October 2020,onlinemonitoringwas conducted in the main urban area of Shijiazhuang to collect data on VOCs and analyze their concentrations and reactivity.Additionally,the PMF(positive matrix factorization)method was utilized to identify the VOCs sources.Results indicated that the TVOCs(total VOCs)concentration was(96.7±63.4μg/m^3),with alkanes exhibiting the highest concentration of(36.1±26.4μg/m^3),followed by OVOCs(16.4±14.4μg/m^3).The key active components were alkenes and aromatics,among which xylene,propylene,toluene,propionaldehyde,acetaldehyde,ethylene,and styrene played crucial roles as reactive species.The sources derived from PMF analysis encompassed vehicle emissions,solvent and coating sources,combustion sources,industrial emissions sources,as well as plant sources,the contribution of which were 37.80%,27.93%,16.57%,15.24%,and 2.46%,respectively.Hence,reducing vehicular exhaust emissions and encouraging neighboring industries to adopt low-volatile organic solvents and coatings should be prioritized to mitigate VOCs levels.
基金supported by Hong Kong Environment Protection Department(Quotation Ref.18-06532)Hong Kong Innovation and Technology Fund(ITS/193/20FP)Hong Kong Research Grants Council(No.26304921).
文摘Initial success has been achieved in Hong Kong in controlling primary air pollutants,but ambient ozone levels kept increasing during the past three decades.Volatile organic compounds(VOCs)are important for mitigating ozone pollution as its major precursors.This study analyzed VOC characteristics of roadside,suburban,and rural sites in Hong Kong to investigate their compositions,concentrations,and source contributions.Herewe showthat the TVOC concentrations were 23.05±13.24,12.68±15.36,and 5.16±5.48 ppbv for roadside,suburban,and rural sites between May 2015 to June 2019,respectively.By using Positive Matrix Factorization(PMF)model,six sources were identified at the roadside site over five years:Liquefied petroleum gas(LPG)usage(33%–46%),gasoline evaporation(8%–31%),aged air mass(11%–28%),gasoline exhaust(5%–16%),diesel exhaust(2%–16%)and fuel filling(75–9%).Similarly,six sources were distinguished at the suburban site,including LPG usage(30%–33%),solvent usage(20%–26%),diesel exhaust(14%–26%),gasoline evaporation(8%–16%),aged air mass(4%–11%),and biogenic emissions(2%–5%).At the rural site,four sources were identified,including aged airmass(33%–51%),solvent usage(25%–30%),vehicular emissions(11%–28%),and biogenic emissions(6%–12%).The analysis further revealed that fuel filling and LPG usage were the primary contributors to OFP and OH reactivity at the roadside site,while solvent usage and biogenic emissions accounted for almost half of OFP and OH reactivity at the suburban and rural sites,respectively.These findings highlight the importance of identifying and characterizing VOC sources at different sites to help policymakers develop targeted measures for pollution mitigation in specific areas.
基金National Natural Science Foundation of China(No.40575059 and No.20637001).
文摘Ambient volatile organic compounds （VOCs） were sampled at six sites in Beijing in the summer of 2004 and analyzed by GCMS. The chemical reactivities of 73 quantified VOCs species were evaluated by OH loss rates （LOH） and ozone formation potentials （OFPs）. Top 15 reactive species, mainly alkenes and aromatics, were identified by these two methods, and accounted for more than 70% of total reactivity of VOCs. In urban areas, isoprene was the most reactive species in term of OH loss rate, contributing 11.4% to the LOH of VOCs. While toluene, accounting for 9.4% of OFPs, appeared to have a long-time role in the photochemical processes. Tongzhou site is obviously influenced by local chemical industry, but the other five sites showed typical urban features influenced mainly by vehicular emissions.
基金supported by the National Key R&D Program of China(No.2016YFC0202500)the National Natural Science Foundation of China(Nos.21677163 and 21876193)+1 种基金the Chengdu Science and Technology Project(No.2018-ZM01-00019-SN)the Youth Innovation Promotion Association CAS。
文摘Volatile organic compounds(VOCs)are major contributors to air pollution.Based on the emission characteristics of 99 VOCs that daily measured at 10 am in winter from 15 December 2015 to 17 January 2016 and in summer from 21 July to 25 August 2016 in Beijing,the environmental impact and health risk of VOC were assessed.In the winter polluted days,the secondary organic aerosol formation potential(SOAP)of VOC(199.70±15.05 mg/m^3)was significantly higher than that on other days.And aromatics were the primary contributor(98.03%)to the SOAP during the observation period.Additionally,the result of the ozone formation potential(OFP)showed that ethylene contributed the most to OFP in winter(26.00%and 27.64%on the normal and polluted days).In summer,however,acetaldehyde was the primary contributor to OFP(22.00%and 21.61%on the normal and polluted days).Simultaneously,study showed that hazard ratios and lifetime cancer risk values of acrolein,chloroform,benzene,1,2-dichloroethane,acetaldehyde and 1,3-butadiene exceeded the thresholds established by USEPA,thereby presenting a health risk to the residents.Besides,the ratio of toluene-to-benzene indicated that vehicle exhausts were the main source of VOC pollution in Beijing.The ratio of m-/p-xylene-toethylbenzene demonstrated that there were more prominent atmospheric photochemical reactions in summer than that in winter.Finally,according to the potential source contribution function(PSCF)results,compared with local pollution sources,the spread of pollution from long-distance VOCs had a greater impact on Beijing.
基金supported by the Open Research Fund Program of State Environmental Protection Key Laboratory of Food Chain Pollution Control(No.FC2021YB03)the Research Foundation for Youth Scholars of Beijing Technology and Business University(No.QNJJ2021-32).
文摘Cooking process can produce abundant volatile organic compounds(VOCs),which are harmful to environment and human health.Therefore,we conducted a comprehensive analysis in which VOCs emissions from multiple cuisines have been sampled based on the simulation and acquisition platform,involving concentration characteristics,ozone formation potential(OFP)and purification efficiency assessments.VOCs emissions varied from 1828.5 to 14,355.1μg/m^(3),with the maximumand minimumvalues fromBarbecue and Family cuisine,respectively.Alkanes and alcohol had higher contributions to VOCs from Sichuan and Hunan cuisine(64.1%),Family cuisine(66.3%),Shandong cuisine(69.1%)and Cantonese cuisine(69.8%),with the dominant VOCs species of ethanol,isobutane and n-butane.In comparison,alcohols(79.5%)were abundant for Huaiyang cuisine,while alkanes(19.7%),alkenes(35.9%)and haloalkanes(22.9%)accounted for higher proportions from Barbecue.Specially,carbon tetrachloride,n-hexylene and 1-butene were the most abundant VOCs species for Barbecue,ranging from 8.8%to 14.6%.The highest OFP occurred in Barbecue.The sensitive species of OFP for Huaiyang cuisine were alcohols,while other cuisines were alkenes.Purification efficiency assessments shed light on the removal differences of individual and synergistic control technologies.VOCs emissions exhibited a strong dependence on the photocatalytic oxidation,with the removal efficiencies of 29.0%–54.4%.However,the high voltage electrostatic,wet purification and mechanical separation techniques played a mediocre or even counterproductive role in the VOCs reduction,meanwhile collaborative control technologies could not significantly improve the removal efficiency.Our results identifiedmore effective control technologies,which were conductive to alleviating air pollution from cooking emissions.
