The biopharmaceutical industry contributes substantially to volatile organic compounds(VOCs)emissions,causing growing concerns and social developmental conflicts.This study conducted an on-site investigation of the pr...The biopharmaceutical industry contributes substantially to volatile organic compounds(VOCs)emissions,causing growing concerns and social developmental conflicts.This study conducted an on-site investigation of the process-based emission of VOCs from three biopharmaceutical enterprises.In the workshops of the three enterprises,26 VOCs were detected,which could be sorted into 4 classes:hydrocarbons,aromatic hydrocarbons,oxygen-containing compounds,and nitrogen-containing compounds.Ketones were the main components of waste gases,accounting for 44.13%-77.85%of the overall VOCs.Process-based source profiles were compiled for each process unit,with the fermentation and extraction units of tiamulin fumarate being the main source of VOC emissions.Dimethyl heptanone,vinyl acetate,diethylamine,propylene glycol methyl ether(PGME),and benzene were screened as priority pollutants through a fuzzy comprehensive evaluation system.Ground level concentration simulation results of the Gauss plume diffusion model demonstrated that the diffusivity of VOCs in the atmosphere was relatively high,indicating potential non-carcinogenic and carcinogenic risks 1.5-2 km downwind.Furthermore,the process-based formation potentials of ozone and secondary organic aerosols(SOAs)were determined and indicated that N-methyl-2-pyrrolidone,dimethyl heptanone,and PGME should be preferentially controlled to reduce the ozone formation potential,whereas the control of benzene and chlorobenzene should be prioritized to reduce the generation of SOAs.Our results provide a basis for understanding the characteristics of VOC emission by biopharmaceutical industries and their diffusion,potentially allowing the development of measures to reduce health risks and secondary pollution.展开更多
Currently,most of the methods formineral materials analysis generate secondary pollution,which is detrimental to human health.For instance,traditionalmethods for sphalerite analysis in the zinc(Zn)smelting industry in...Currently,most of the methods formineral materials analysis generate secondary pollution,which is detrimental to human health.For instance,traditionalmethods for sphalerite analysis in the zinc(Zn)smelting industry including chemical titration,atomic absorption spectrometry,and inductively coupled atomic emission spectroscopy.Colored indicators and toxic heavy metals are used in the analytical processes,causing severe pollution.For some methods,liquid is transformed into gaseous plasma,which is more dangerous to human health.Due to large quantities of sphalerite being used,secondary pollution cannot be ignored.This study proposes a green analysis method for the detection of sphalerite based on colorimetry,which does not generate secondary pollution.The results show that the strong substitution ability of iron(Fe)for Zn contributes to their inverse correlation in contents.The lattice parameters decrease with the increasing Fe content,resulting in a darker coloration.Here,key colorimetry parameters of L*,a*,and b*show clear linear correlations with the Zn and Fe contents.Compared with traditional approaches,this new method is environmental friendly with high sensitivity and accuracy.The relative error and relative standard deviation were less than 10%and 5%,respectively.This study provides a significant reference for nonpollution determination of other mineral materials.展开更多
Since the discovery of polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs)in the process of municipal solid waste incineration(MSWI),a large number of researches have been conducted to reveal their formation ...Since the discovery of polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs)in the process of municipal solid waste incineration(MSWI),a large number of researches have been conducted to reveal their formation mechanisms and emission characteristics.As one of national priority control pollutants,chlorinated organics are inclined to transfer into PCDD/Fs in the heterogeneously catalyzed process,which has been considered to be one of great challenges in environmental catalysis.However,so far direct evidences to support such a conversion process are insufficient,and the reaction mechanisms are lack of exploration.This study investigated the catalytic elimination of chlorobenzene(CBz)over a range of industrially applied active species including Pt,Ru,V,Ce and Mn oxides,and explored their reaction byproducts,chlorine adsorption/desorption behaviors and PCDD/F formations.We found that all of these species could generate the PCDD/Fs,amongst which,Mn species were the most active for PCDD/F formation.Approximately 140 ng I-TEQg-1 PCDD/Fs were detected on the Mn-CNT surface after ageing at250℃for 30 h.Even using the dichloromethane(DCM)as a precursor,significant PCDD/Fs were still detected.The Ru and V species were shown to generate much less polychlorinated byproducts and PCDD/Fs,owning to their sufficiently high abilities in Cl desorption,which were through the semi-Deacon and Br(?)nsted H reactions,respectively.展开更多
The authors report the results of aethalometer black carbon(BC)aerosol measurements carried out over a rural(pristine)site,Panchgaon,Haryana State,India during the winter months of 2021-2022 and 2022-2023.They are com...The authors report the results of aethalometer black carbon(BC)aerosol measurements carried out over a rural(pristine)site,Panchgaon,Haryana State,India during the winter months of 2021-2022 and 2022-2023.They are compared with collocated and concurrent observations from the Air Quality Monitoring Station(AQMS),which provides synchronous air pollution and surface meteorological parameters.Secular variations in BC mass concentration are studied and explained with variations in local meteorological parameters.The biomass burning fire count retrievals from NASA-NOAA VIIRS satellite,and backward airmass trajectories from NOAA-ERL HYSPLIT Model analysis have also been utilized to explain the findings.They reveal that the north-west Indian region contributes maximum to the BC mass concentration over the study site during the study period.Moreover,the observed BC mass concentrations corroborate the synchronous fire count,primary and secondary pollutant concentrations.The results were found to aid the development of mitigation methods to achieve a sustainable climate system.展开更多
Here, we report the construction of magnetic core-shell microparticles for oil removal with thermal driving regeneration property. Water-in-oil-in water (W/O/W) emulsions from microfluidics are used as templates to pr...Here, we report the construction of magnetic core-shell microparticles for oil removal with thermal driving regeneration property. Water-in-oil-in water (W/O/W) emulsions from microfluidics are used as templates to prepare core-shell microparticles with magnetic holed poly (ethoxylated trimethylolpropane triacrylate) (PETPTA) shells each containing a thermal-sensitive poly (N-Isopropylacrylamide) (PNIPAM) core. The microparticles could adsorb oil from water due to the special structure and be collected with a magnetic field. Then, the oil-filled microparticles would be regenerated by thermal stimulus, in which the inner PNIPAM microgels work as thermal-sensitive pistons to force out the adsorbed oil. At the same time, the adsorbed oil would be recycled by distillation. Furthermore, the adsorption capacity of the microparticles for oil keeps very stable after 1st cycle. The adsorption and regeneration performances of the microparticles are greatly affected by the size of the holes on the outer PETPTA shells, which could be precisely controlled by regulating the interfacial forces in W/O/W emulsion templates. The optimized core-shell microparticles show excellent oil adsorption and thermal driving regeneration performances nearly without secondary pollution, and would be a reliable green adsorption material for kinds of oil.展开更多
As the main organic pollutant in municipal living waste , kitchen waste causes secondary pollution in the course of its being gathered and transported to the landfill by mixing with other refuse and by decomposition. ...As the main organic pollutant in municipal living waste , kitchen waste causes secondary pollution in the course of its being gathered and transported to the landfill by mixing with other refuse and by decomposition. This makes pollution prevention more difficult and raises the cost of landfill engineering. However, the amount of solid waste to be treated can be decreased and such pollution burden lessened by disposing of the solid waste in local municipal areas. The program in Beijing also shows that this works well with our situation in China and can accelerate marketization and public participation.展开更多
Secondary air pollutants,originating from gaseous pollutants and primary particulate matter emitted by natural sources and human activities,undergo complex atmospheric chemical reactions and multiphase processes.Secon...Secondary air pollutants,originating from gaseous pollutants and primary particulate matter emitted by natural sources and human activities,undergo complex atmospheric chemical reactions and multiphase processes.Secondary gaseous pollutants represented by ozone and secondary particulate matter,including sulfates,nitrates,ammonium salts,and secondary organic aerosols,are formed in the atmosphere,affecting air quality and human health.This paper summarizes the formation pathways and mechanisms of important atmospheric secondary pollutants.Meanwhile,different secondary pollutants’toxicological effects and corresponding health risks are evaluated.Studies have shown that secondary pollutants are generally more toxic than primary ones.However,due to their diverse source and complex generation mechanism,the study of the toxicological effects of secondary pollutants is still in its early stages.Therefore,this paper first introduces the formation mechanism of secondary gaseous pollutants and focuses mainly on ozone’s toxicological effects.In terms of particulate matter,secondary inorganic and organic particulate matters are summarized separately,then the contribution and toxicological effects of secondary components formed from primary carbonaceous aerosols are discussed.Finally,secondary pollutants generated in the indoor environment are briefly introduced.Overall,a comprehensive review of secondary air pollutants may shed light on the future toxicological and health effects research of secondary air pollutants.展开更多
This work presents an overall introduction to the Station for Observing Regional Processes of the EarthSystem - SORPES in Nanjing, East China, and gives an overview about main scientific findings instudies of air poll...This work presents an overall introduction to the Station for Observing Regional Processes of the EarthSystem - SORPES in Nanjing, East China, and gives an overview about main scientific findings instudies of air pollution-weather/climate interactions obtained since 2011. The main results summarizedin this paper include overall characteristics of trace gases and aerosols, chemical transformationmechanisms for secondary pollutants like O3, HONO andsecondary ingrganic aerosols, and the airpollution- weather/climate interactions and feedbacks in mixed air pollution plumes from sources likefossil fuel combustion, biomass burning and dust storms. The future outlook of the development plan on instrumentation, networking and data-sharing for the SORPES station is also discussed.展开更多
Urban and regional air pollutions are characterized by high concentrations of secondary pollutants such as photo-oxidants (mainly ozone) and fine particulate matter, which are formed through chemical reactions of th...Urban and regional air pollutions are characterized by high concentrations of secondary pollutants such as photo-oxidants (mainly ozone) and fine particulate matter, which are formed through chemical reactions of the primary pollutants emitted from various sources. The accumulation of these pollutants under stagnant meteorological conditions results in the formation of gray haze, reducing visibility and causing major impacts on human health and climate. In an air pollution complex, the co- existence of high concentrations of primary and secondary gaseous and particulate pollutants provides a large amount of reac- tants for heterogeneous reactions on the surface of fine particles; these reactions change the oxidizing capacity of the atmos- phere, as well as chemical compositions along with the physicochemical and optical properties of particulate matter, thereby accelerating formation of the air pollution complex and gray haze. Using in situ technologies, such as diffuse reflectance infra- red Fourier-transform spectroscopy and single-particle Raman spectroscopy, we systematically investigated the reaction kinet- ics and mechanisms of gaseous pollutants (i.e., NO2, SO2, 03, and formaldehyde) on the surfaces of the major components of atmospheric particles such as CaCO3, kaolinite, montmorillonite, NaC1, sea salt, A1203, and Tit2. We found that the main re- action products were sulfate, nitrate, or formate, which can change the hygroscopicity and light extinction parameters of those particles significantly. By analyzing the reaction kinetics of these heterogeneous reactions, we identified synergetic mechanisms of the three ternary reaction systems, ,i.e., NOE-particles-H2O, SO2-particles-O3, and organics/SO2-particles-UV illumination. These synergetic mechanisms can provide experimental and theoretical bases for understanding the feedback mechanisms and nonlinear processes in the formation of an air pollution complex and gray haze.展开更多
Integral to the urban ecosystem,greening trees provide many ecological benefits,but the active biogenic volatile organic compounds(BVOCs)they release contribute to the production of ozone and secondary organic aerosol...Integral to the urban ecosystem,greening trees provide many ecological benefits,but the active biogenic volatile organic compounds(BVOCs)they release contribute to the production of ozone and secondary organic aerosols,which harm ambient air quality.It is,therefore,necessary to understand the BVOC emission characteristics of dominant greening tree species and their relative contribution to secondary pollutants in various urban contexts.Consequently,this study utilized a dynamic enclosure system to collect BVOC samples of seven dominant greening tree species in urban Chengdu,Southwest China.Gas chromatography/mass spectrometry was used to analyze the BVOC components and standardized BVOC emission rates of each tree species were then calculated to assess their relative potential to form secondary pollutants.We found obvious differences in the composition of BVOCs emitted by each species.Ficus virens displayed a high isoprene emission rate at31.472μgC/(gdw(g dry weight)·hr),while Cinnamomum camphora emitted high volumes of D-Limonene at 93.574μgC/(gdw·hr).In terms of the BVOC emission rates by leaf area,C.camphora had the highest emission rate of total BVOCs at 13,782.59μgC/(m^(2)·hr),followed by Cedrus deodara with 5466.86μgC/(m^(2)·hr).Ginkgo biloba and Osmanthus fragrans mainly emitted oxygenated VOCs with lower overall emission rates.The high BVOC emitters like F.virens,C.camphora,and Magnolia grandiflora have high potential for significantly contributing to environmental secondary pollutants,so should be cautiously considered for future planting.This study provides important implications for improving urban greening efforts for subtropical Chinese urban contexts,like Chengdu.展开更多
To investigate the influence of haze on the chemical composition and formation processes of ambient aerosol particles,PM_(2.5) and size-segregated aerosol particles were collected daily during fall at an urban site ...To investigate the influence of haze on the chemical composition and formation processes of ambient aerosol particles,PM_(2.5) and size-segregated aerosol particles were collected daily during fall at an urban site of Gwangju,Korea.During the study period,the total concentration of secondary ionic species(SIS) contributed an average of 43.9% to the PM_(2.5) ,whereas the contribution of SIS to the PM_(2.5) during the haze period was 62.3%.The NO_3 and SO^(2-)_4 concentrations in PM_(2.5) during the haze period were highly elevated,being 13.4 and 5.0 times higher than those during non-haze period,respectively.The PM,NO^-_3,SO^(2-)_4,oxalate,water-soluble organic carbon(WSOC),and humic-like substances(HULIS) had tri-modal size distributions peaks at 0.32,1.0,and 5.2 μm during the non-haze and haze periods.However,during the non-haze period they exhibited dominant size distributions at the condensation mode peaking at 0.32 μm,while on October 21 when the heaviest haze event occurred,they had predominant droplet mode size distributions peaking at 1.00 μm.Moreover,strong correlations of WSOC and HULIS with SO^(2-)_4,oxalate,and K+at particle sizes of 〈 1.8 μm indicate that secondary processes and emissions from biomass burning could be responsible for WSOC and HULIS formations.It was found that the factors affecting haze formation could be the local stable synoptic conditions,including the weak surface winds and high surface pressures,the long-range transportation of haze from eastern China and upwind regions of the Korean peninsula,as well as the locally emitted and produced aerosol particles.展开更多
In the process of catalytic destruction of chlorinated volatile organic compounds(CVOCs),the catalyst is prone to chlorine poisoning and produce polychlorinated byproducts with high toxicity and persistence,bringing g...In the process of catalytic destruction of chlorinated volatile organic compounds(CVOCs),the catalyst is prone to chlorine poisoning and produce polychlorinated byproducts with high toxicity and persistence,bringing great risk to atmospheric environment and human health.To solve these problems,this work applied phosphate to modify K-OMS-2 catalysts.The physicochemical properties of catalysts were determined by using X-ray powder diffraction(XRD),scanning electron microscope(SEM),X-ray photoelectron spectroscopy(XPS),hydrogen temperature programmed reduction(H_(2)-TPR),pyridine adsorption Fouriertransform infrared(Py-IR)and water temperature programmed desorption(H_(2)O-TPD),and chlorobenzene was selected as a model pollutant to explore the catalytic performance and byproduct inhibition function of phosphating.Experimental results revealed that 1 wt.%phosphate modification yielded the best catalytic activity for chlorobenzene destruction,with the 90%conversion(T90)at approximately 247℃.The phosphating significantly decreased the types and yields of polychlorinated byproducts in effluent.After phosphating,we observed significant hydroxyl groups on catalyst surface,and the active centerwas transformed into Mn(IV)-O…H,which promoted the formation of HCl,and enhanced the dechlorination process.Furthermore,the enriched Lewis acid sites by phosphating profoundly enhanced the deep oxidation ability of the catalyst,which promoted a rapid oxidation of reaction intermediates,so as to reduce byproducts generation.This study provided an effective strategy for inhibiting the toxic byproducts for the catalytic destruction of chlorinated organics.展开更多
The potential release capacity of arsenic(As)from sediment was evaluated under a high level of exogenous organic matter(EOM)with both bioreactive and chemically reactive organic matters(OMs).The OMs were characterized...The potential release capacity of arsenic(As)from sediment was evaluated under a high level of exogenous organic matter(EOM)with both bioreactive and chemically reactive organic matters(OMs).The OMs were characterized by FI,HIX,BIX,and SUVA254 fluorescence indices showing the biological activities were kept at a high level during the experimental period.At the genus level,Fe/Mn/As-reducing bacteria(Geobacter,Pseudomonas,Bacillus,and Clostridium)and bacteria(Paenibacillus,Acidovorax,Delftia,and Sphingomonas)that can participate in metabolic transformation using EOM were identified.The reducing condition occurs which promoted As,Fe,and Mn releases at very high concentrations of OM.However,As release increased during the first 15-20 days,followed by a decline contributed by secondary iron precipitation.The degree of As release may be limited by the reactivity of Fe(hydro)oxides.The EOM infiltration enhances As and Mn releases in aqueous conditions causing the risk of groundwater pollution,which could occur in specific sites such as landfills,petrochemical sites,and managed aquifer recharge projects.展开更多
To date,investigations onto the regulation of reactants mass transfer has been paid much less attention in environmental catalysis.Herein,we demonstrated that by rationally designing the adsorption sites of multi-reac...To date,investigations onto the regulation of reactants mass transfer has been paid much less attention in environmental catalysis.Herein,we demonstrated that by rationally designing the adsorption sites of multi-reactants,the pollutant destruction efficiency,product selectivity,reaction stability and secondary pollution have been all affected in the catalytic chlorobenzene oxidation(CBCO).Experimental results revealed that the co-adsorption of chlo robenzene(CB)and gaseous O_(2)at the oxygen vacancies of CeO_(2)led to remarkably high CO_(2)generation,owning to their short mass transfer distance on the catalyst surface,while their separated adsorptions at Bronsted HZSM-5 and CeO_(2)vacancies resulted in a much lower CO_(2)generation,and produced significant polychlorinated byproducts in the off-gas.Howeve r,this separated adsorption model yielded superior long-term stability for the CeO_(2)/HZSM-5 catalyst,owning to the protection of CeO_(2)oxygen vacancies from Cl poisoning by the preferential adsorption of CB on the Bronsted acidic sites.This work unveils that design of environmental catalysts needs to consider both of the catalyst intrinsic property and reactant mass transfer;investigations of the latter could pave a new way for the development of highly efficient catalysts towards environmental pollution control.展开更多
This observational study investigates the variation of PM2.5 concentration and its ratio against PM10 concentration under different weather systems and pollution types. The study was conducted in Hangzhou on east Chin...This observational study investigates the variation of PM2.5 concentration and its ratio against PM10 concentration under different weather systems and pollution types. The study was conducted in Hangzhou on east China's Yangtze River Delta using data collected at seven ambient air quality monitoring stations around the metropolitan area between 2006 and 2008 and using weather information in the same period. Nine predominant weather systems affecting the city were classified through careful analysis of the 11- year surface and upper air weather charts from 1996 to 2006. Each observational day was then assigned to one of the nine weather systems. It was found that the PM2.5 concentration varied greatly for different weather systems, with the highest PM2.5 concentration associated with the post-cold-frontal system at 0.091 mg/m^3 and the lowest PM2.5 concentration with the easterlies system at 0.038 mg/m^3, although the PM2.5/PM10 ratio remained consistently above 0.5 for all systems. The post-cold-frontal system typically occurs in autumn and winter while the easterlies system is more a summer phenomenon. Among all types of pollution, the highest PM2.5 concentration of 0.117 mg/m^3 coincided with the large-scale continuous pollution events, suggesting that this type of pollution was more conducive to the formation of secondary particulate matters. The ratio of PM2.5/PM10 was above 0.5 in non-pollution days and all pollution types but one under the influence of dust storms when the ratio decreased to 0.3 or less. The outcomes of this study could be used to develop a rudimental predictive model of PM2.5 concentration based on weather system and pollution type.展开更多
基金financially supported by the National Natural Science Foundation of China (No.51878650)。
文摘The biopharmaceutical industry contributes substantially to volatile organic compounds(VOCs)emissions,causing growing concerns and social developmental conflicts.This study conducted an on-site investigation of the process-based emission of VOCs from three biopharmaceutical enterprises.In the workshops of the three enterprises,26 VOCs were detected,which could be sorted into 4 classes:hydrocarbons,aromatic hydrocarbons,oxygen-containing compounds,and nitrogen-containing compounds.Ketones were the main components of waste gases,accounting for 44.13%-77.85%of the overall VOCs.Process-based source profiles were compiled for each process unit,with the fermentation and extraction units of tiamulin fumarate being the main source of VOC emissions.Dimethyl heptanone,vinyl acetate,diethylamine,propylene glycol methyl ether(PGME),and benzene were screened as priority pollutants through a fuzzy comprehensive evaluation system.Ground level concentration simulation results of the Gauss plume diffusion model demonstrated that the diffusivity of VOCs in the atmosphere was relatively high,indicating potential non-carcinogenic and carcinogenic risks 1.5-2 km downwind.Furthermore,the process-based formation potentials of ozone and secondary organic aerosols(SOAs)were determined and indicated that N-methyl-2-pyrrolidone,dimethyl heptanone,and PGME should be preferentially controlled to reduce the ozone formation potential,whereas the control of benzene and chlorobenzene should be prioritized to reduce the generation of SOAs.Our results provide a basis for understanding the characteristics of VOC emission by biopharmaceutical industries and their diffusion,potentially allowing the development of measures to reduce health risks and secondary pollution.
基金National Natural Science Foundation of China,Grant/Award Numbers:52174385,41877392Fundamental Research Funds for the Central Universities,Tongji University,Grant/Award Number:22120220166。
文摘Currently,most of the methods formineral materials analysis generate secondary pollution,which is detrimental to human health.For instance,traditionalmethods for sphalerite analysis in the zinc(Zn)smelting industry including chemical titration,atomic absorption spectrometry,and inductively coupled atomic emission spectroscopy.Colored indicators and toxic heavy metals are used in the analytical processes,causing severe pollution.For some methods,liquid is transformed into gaseous plasma,which is more dangerous to human health.Due to large quantities of sphalerite being used,secondary pollution cannot be ignored.This study proposes a green analysis method for the detection of sphalerite based on colorimetry,which does not generate secondary pollution.The results show that the strong substitution ability of iron(Fe)for Zn contributes to their inverse correlation in contents.The lattice parameters decrease with the increasing Fe content,resulting in a darker coloration.Here,key colorimetry parameters of L*,a*,and b*show clear linear correlations with the Zn and Fe contents.Compared with traditional approaches,this new method is environmental friendly with high sensitivity and accuracy.The relative error and relative standard deviation were less than 10%and 5%,respectively.This study provides a significant reference for nonpollution determination of other mineral materials.
基金financially supported by the National Natural Science Foundation of China(Nos.21777140,21922607)the Outstanding Youth Project of Zhejiang Natural Science Foundation(No.LR19E080004)。
文摘Since the discovery of polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs)in the process of municipal solid waste incineration(MSWI),a large number of researches have been conducted to reveal their formation mechanisms and emission characteristics.As one of national priority control pollutants,chlorinated organics are inclined to transfer into PCDD/Fs in the heterogeneously catalyzed process,which has been considered to be one of great challenges in environmental catalysis.However,so far direct evidences to support such a conversion process are insufficient,and the reaction mechanisms are lack of exploration.This study investigated the catalytic elimination of chlorobenzene(CBz)over a range of industrially applied active species including Pt,Ru,V,Ce and Mn oxides,and explored their reaction byproducts,chlorine adsorption/desorption behaviors and PCDD/F formations.We found that all of these species could generate the PCDD/Fs,amongst which,Mn species were the most active for PCDD/F formation.Approximately 140 ng I-TEQg-1 PCDD/Fs were detected on the Mn-CNT surface after ageing at250℃for 30 h.Even using the dichloromethane(DCM)as a precursor,significant PCDD/Fs were still detected.The Ru and V species were shown to generate much less polychlorinated byproducts and PCDD/Fs,owning to their sufficiently high abilities in Cl desorption,which were through the semi-Deacon and Br(?)nsted H reactions,respectively.
文摘The authors report the results of aethalometer black carbon(BC)aerosol measurements carried out over a rural(pristine)site,Panchgaon,Haryana State,India during the winter months of 2021-2022 and 2022-2023.They are compared with collocated and concurrent observations from the Air Quality Monitoring Station(AQMS),which provides synchronous air pollution and surface meteorological parameters.Secular variations in BC mass concentration are studied and explained with variations in local meteorological parameters.The biomass burning fire count retrievals from NASA-NOAA VIIRS satellite,and backward airmass trajectories from NOAA-ERL HYSPLIT Model analysis have also been utilized to explain the findings.They reveal that the north-west Indian region contributes maximum to the BC mass concentration over the study site during the study period.Moreover,the observed BC mass concentrations corroborate the synchronous fire count,primary and secondary pollutant concentrations.The results were found to aid the development of mitigation methods to achieve a sustainable climate system.
基金This work was supported by the National Natural Science Foundation of China[grant numbers 21706219]。
文摘Here, we report the construction of magnetic core-shell microparticles for oil removal with thermal driving regeneration property. Water-in-oil-in water (W/O/W) emulsions from microfluidics are used as templates to prepare core-shell microparticles with magnetic holed poly (ethoxylated trimethylolpropane triacrylate) (PETPTA) shells each containing a thermal-sensitive poly (N-Isopropylacrylamide) (PNIPAM) core. The microparticles could adsorb oil from water due to the special structure and be collected with a magnetic field. Then, the oil-filled microparticles would be regenerated by thermal stimulus, in which the inner PNIPAM microgels work as thermal-sensitive pistons to force out the adsorbed oil. At the same time, the adsorbed oil would be recycled by distillation. Furthermore, the adsorption capacity of the microparticles for oil keeps very stable after 1st cycle. The adsorption and regeneration performances of the microparticles are greatly affected by the size of the holes on the outer PETPTA shells, which could be precisely controlled by regulating the interfacial forces in W/O/W emulsion templates. The optimized core-shell microparticles show excellent oil adsorption and thermal driving regeneration performances nearly without secondary pollution, and would be a reliable green adsorption material for kinds of oil.
文摘As the main organic pollutant in municipal living waste , kitchen waste causes secondary pollution in the course of its being gathered and transported to the landfill by mixing with other refuse and by decomposition. This makes pollution prevention more difficult and raises the cost of landfill engineering. However, the amount of solid waste to be treated can be decreased and such pollution burden lessened by disposing of the solid waste in local municipal areas. The program in Beijing also shows that this works well with our situation in China and can accelerate marketization and public participation.
基金This work was supported by the National Natural Science Foundation of China(No.92143301).
文摘Secondary air pollutants,originating from gaseous pollutants and primary particulate matter emitted by natural sources and human activities,undergo complex atmospheric chemical reactions and multiphase processes.Secondary gaseous pollutants represented by ozone and secondary particulate matter,including sulfates,nitrates,ammonium salts,and secondary organic aerosols,are formed in the atmosphere,affecting air quality and human health.This paper summarizes the formation pathways and mechanisms of important atmospheric secondary pollutants.Meanwhile,different secondary pollutants’toxicological effects and corresponding health risks are evaluated.Studies have shown that secondary pollutants are generally more toxic than primary ones.However,due to their diverse source and complex generation mechanism,the study of the toxicological effects of secondary pollutants is still in its early stages.Therefore,this paper first introduces the formation mechanism of secondary gaseous pollutants and focuses mainly on ozone’s toxicological effects.In terms of particulate matter,secondary inorganic and organic particulate matters are summarized separately,then the contribution and toxicological effects of secondary components formed from primary carbonaceous aerosols are discussed.Finally,secondary pollutants generated in the indoor environment are briefly introduced.Overall,a comprehensive review of secondary air pollutants may shed light on the future toxicological and health effects research of secondary air pollutants.
基金The work was supported by the National Natural Science Foundation of China (Grant Nos. D0512/91544231, D0512/ 41422504, and D0510/41505109), National Key Research and Development Program in China (No. 2016YFC0200506), and Jiangsu Provincial Science Fund (No. BK20140021). We thank L.F. Zheng, Z.N. Xu, L.S. Jin, E. Herrmann, Y.N. Xie, X.M. Qi, A. Virkkula, Z. Peng, Y.C. Shen, J.P. Wang, H. Shi, L. Wang, C.J. Zhu and H. Shi for their contributions on instrumental maintenance and field campaigns.
文摘This work presents an overall introduction to the Station for Observing Regional Processes of the EarthSystem - SORPES in Nanjing, East China, and gives an overview about main scientific findings instudies of air pollution-weather/climate interactions obtained since 2011. The main results summarizedin this paper include overall characteristics of trace gases and aerosols, chemical transformationmechanisms for secondary pollutants like O3, HONO andsecondary ingrganic aerosols, and the airpollution- weather/climate interactions and feedbacks in mixed air pollution plumes from sources likefossil fuel combustion, biomass burning and dust storms. The future outlook of the development plan on instrumentation, networking and data-sharing for the SORPES station is also discussed.
基金financially supported by the National Natural Science Foundation of China (20637020, 40490265 & 20077001)National Basic Research Program of China (2002CB410802)special fund of State Key Joint Laboratory of Environment Simulation and Pollution Control
文摘Urban and regional air pollutions are characterized by high concentrations of secondary pollutants such as photo-oxidants (mainly ozone) and fine particulate matter, which are formed through chemical reactions of the primary pollutants emitted from various sources. The accumulation of these pollutants under stagnant meteorological conditions results in the formation of gray haze, reducing visibility and causing major impacts on human health and climate. In an air pollution complex, the co- existence of high concentrations of primary and secondary gaseous and particulate pollutants provides a large amount of reac- tants for heterogeneous reactions on the surface of fine particles; these reactions change the oxidizing capacity of the atmos- phere, as well as chemical compositions along with the physicochemical and optical properties of particulate matter, thereby accelerating formation of the air pollution complex and gray haze. Using in situ technologies, such as diffuse reflectance infra- red Fourier-transform spectroscopy and single-particle Raman spectroscopy, we systematically investigated the reaction kinet- ics and mechanisms of gaseous pollutants (i.e., NO2, SO2, 03, and formaldehyde) on the surfaces of the major components of atmospheric particles such as CaCO3, kaolinite, montmorillonite, NaC1, sea salt, A1203, and Tit2. We found that the main re- action products were sulfate, nitrate, or formate, which can change the hygroscopicity and light extinction parameters of those particles significantly. By analyzing the reaction kinetics of these heterogeneous reactions, we identified synergetic mechanisms of the three ternary reaction systems, ,i.e., NOE-particles-H2O, SO2-particles-O3, and organics/SO2-particles-UV illumination. These synergetic mechanisms can provide experimental and theoretical bases for understanding the feedback mechanisms and nonlinear processes in the formation of an air pollution complex and gray haze.
基金supported by the National Natural Science Foundation of China(No.21906108)the Fundamental Research Funds for the Central Universities(No.YJ201937)+1 种基金Chengdu Science and Technology Bureau(No.2020-YF09-00051-SN)the Sichuan"1000 Plan"Scholar Program
文摘Integral to the urban ecosystem,greening trees provide many ecological benefits,but the active biogenic volatile organic compounds(BVOCs)they release contribute to the production of ozone and secondary organic aerosols,which harm ambient air quality.It is,therefore,necessary to understand the BVOC emission characteristics of dominant greening tree species and their relative contribution to secondary pollutants in various urban contexts.Consequently,this study utilized a dynamic enclosure system to collect BVOC samples of seven dominant greening tree species in urban Chengdu,Southwest China.Gas chromatography/mass spectrometry was used to analyze the BVOC components and standardized BVOC emission rates of each tree species were then calculated to assess their relative potential to form secondary pollutants.We found obvious differences in the composition of BVOCs emitted by each species.Ficus virens displayed a high isoprene emission rate at31.472μgC/(gdw(g dry weight)·hr),while Cinnamomum camphora emitted high volumes of D-Limonene at 93.574μgC/(gdw·hr).In terms of the BVOC emission rates by leaf area,C.camphora had the highest emission rate of total BVOCs at 13,782.59μgC/(m^(2)·hr),followed by Cedrus deodara with 5466.86μgC/(m^(2)·hr).Ginkgo biloba and Osmanthus fragrans mainly emitted oxygenated VOCs with lower overall emission rates.The high BVOC emitters like F.virens,C.camphora,and Magnolia grandiflora have high potential for significantly contributing to environmental secondary pollutants,so should be cautiously considered for future planting.This study provides important implications for improving urban greening efforts for subtropical Chinese urban contexts,like Chengdu.
基金supported by the Basic Science Research Programs through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(MOE)(NRF2014R1A1A4A01003896)the support from the BK21 Plus program through the NRF funded by the MOE
文摘To investigate the influence of haze on the chemical composition and formation processes of ambient aerosol particles,PM_(2.5) and size-segregated aerosol particles were collected daily during fall at an urban site of Gwangju,Korea.During the study period,the total concentration of secondary ionic species(SIS) contributed an average of 43.9% to the PM_(2.5) ,whereas the contribution of SIS to the PM_(2.5) during the haze period was 62.3%.The NO_3 and SO^(2-)_4 concentrations in PM_(2.5) during the haze period were highly elevated,being 13.4 and 5.0 times higher than those during non-haze period,respectively.The PM,NO^-_3,SO^(2-)_4,oxalate,water-soluble organic carbon(WSOC),and humic-like substances(HULIS) had tri-modal size distributions peaks at 0.32,1.0,and 5.2 μm during the non-haze and haze periods.However,during the non-haze period they exhibited dominant size distributions at the condensation mode peaking at 0.32 μm,while on October 21 when the heaviest haze event occurred,they had predominant droplet mode size distributions peaking at 1.00 μm.Moreover,strong correlations of WSOC and HULIS with SO^(2-)_4,oxalate,and K+at particle sizes of 〈 1.8 μm indicate that secondary processes and emissions from biomass burning could be responsible for WSOC and HULIS formations.It was found that the factors affecting haze formation could be the local stable synoptic conditions,including the weak surface winds and high surface pressures,the long-range transportation of haze from eastern China and upwind regions of the Korean peninsula,as well as the locally emitted and produced aerosol particles.
基金supported by the National Natural Science Foundation of China(Nos.21922607 and 22106133)the Outstanding Youth Project of Zhejiang Natural Science Foundation(No.LR19E080004).
文摘In the process of catalytic destruction of chlorinated volatile organic compounds(CVOCs),the catalyst is prone to chlorine poisoning and produce polychlorinated byproducts with high toxicity and persistence,bringing great risk to atmospheric environment and human health.To solve these problems,this work applied phosphate to modify K-OMS-2 catalysts.The physicochemical properties of catalysts were determined by using X-ray powder diffraction(XRD),scanning electron microscope(SEM),X-ray photoelectron spectroscopy(XPS),hydrogen temperature programmed reduction(H_(2)-TPR),pyridine adsorption Fouriertransform infrared(Py-IR)and water temperature programmed desorption(H_(2)O-TPD),and chlorobenzene was selected as a model pollutant to explore the catalytic performance and byproduct inhibition function of phosphating.Experimental results revealed that 1 wt.%phosphate modification yielded the best catalytic activity for chlorobenzene destruction,with the 90%conversion(T90)at approximately 247℃.The phosphating significantly decreased the types and yields of polychlorinated byproducts in effluent.After phosphating,we observed significant hydroxyl groups on catalyst surface,and the active centerwas transformed into Mn(IV)-O…H,which promoted the formation of HCl,and enhanced the dechlorination process.Furthermore,the enriched Lewis acid sites by phosphating profoundly enhanced the deep oxidation ability of the catalyst,which promoted a rapid oxidation of reaction intermediates,so as to reduce byproducts generation.This study provided an effective strategy for inhibiting the toxic byproducts for the catalytic destruction of chlorinated organics.
基金supported by the National Key Research and Development Program(2019YFC1806204)the National Natural Science Foundation of China(No.41907178).
文摘The potential release capacity of arsenic(As)from sediment was evaluated under a high level of exogenous organic matter(EOM)with both bioreactive and chemically reactive organic matters(OMs).The OMs were characterized by FI,HIX,BIX,and SUVA254 fluorescence indices showing the biological activities were kept at a high level during the experimental period.At the genus level,Fe/Mn/As-reducing bacteria(Geobacter,Pseudomonas,Bacillus,and Clostridium)and bacteria(Paenibacillus,Acidovorax,Delftia,and Sphingomonas)that can participate in metabolic transformation using EOM were identified.The reducing condition occurs which promoted As,Fe,and Mn releases at very high concentrations of OM.However,As release increased during the first 15-20 days,followed by a decline contributed by secondary iron precipitation.The degree of As release may be limited by the reactivity of Fe(hydro)oxides.The EOM infiltration enhances As and Mn releases in aqueous conditions causing the risk of groundwater pollution,which could occur in specific sites such as landfills,petrochemical sites,and managed aquifer recharge projects.
基金financially supported by the National Key R&D Program of China(No.2016YFC0202200)the National Natural Science Foundation of China(Nos.21777140,21922607)the Outstanding Youth Project of Zhejiang Natural Science Foundation(No.LR19E080004)。
文摘To date,investigations onto the regulation of reactants mass transfer has been paid much less attention in environmental catalysis.Herein,we demonstrated that by rationally designing the adsorption sites of multi-reactants,the pollutant destruction efficiency,product selectivity,reaction stability and secondary pollution have been all affected in the catalytic chlorobenzene oxidation(CBCO).Experimental results revealed that the co-adsorption of chlo robenzene(CB)and gaseous O_(2)at the oxygen vacancies of CeO_(2)led to remarkably high CO_(2)generation,owning to their short mass transfer distance on the catalyst surface,while their separated adsorptions at Bronsted HZSM-5 and CeO_(2)vacancies resulted in a much lower CO_(2)generation,and produced significant polychlorinated byproducts in the off-gas.Howeve r,this separated adsorption model yielded superior long-term stability for the CeO_(2)/HZSM-5 catalyst,owning to the protection of CeO_(2)oxygen vacancies from Cl poisoning by the preferential adsorption of CB on the Bronsted acidic sites.This work unveils that design of environmental catalysts needs to consider both of the catalyst intrinsic property and reactant mass transfer;investigations of the latter could pave a new way for the development of highly efficient catalysts towards environmental pollution control.
基金funded by the Hangzhou Key Sci_technology & Innovative Project(No.20092113A05)
文摘This observational study investigates the variation of PM2.5 concentration and its ratio against PM10 concentration under different weather systems and pollution types. The study was conducted in Hangzhou on east China's Yangtze River Delta using data collected at seven ambient air quality monitoring stations around the metropolitan area between 2006 and 2008 and using weather information in the same period. Nine predominant weather systems affecting the city were classified through careful analysis of the 11- year surface and upper air weather charts from 1996 to 2006. Each observational day was then assigned to one of the nine weather systems. It was found that the PM2.5 concentration varied greatly for different weather systems, with the highest PM2.5 concentration associated with the post-cold-frontal system at 0.091 mg/m^3 and the lowest PM2.5 concentration with the easterlies system at 0.038 mg/m^3, although the PM2.5/PM10 ratio remained consistently above 0.5 for all systems. The post-cold-frontal system typically occurs in autumn and winter while the easterlies system is more a summer phenomenon. Among all types of pollution, the highest PM2.5 concentration of 0.117 mg/m^3 coincided with the large-scale continuous pollution events, suggesting that this type of pollution was more conducive to the formation of secondary particulate matters. The ratio of PM2.5/PM10 was above 0.5 in non-pollution days and all pollution types but one under the influence of dust storms when the ratio decreased to 0.3 or less. The outcomes of this study could be used to develop a rudimental predictive model of PM2.5 concentration based on weather system and pollution type.