Air conditioning is a crucial participant in indoor air circulation and harmful microorganism transmission.To elucidate microbial contamination in air conditioning systems,bacteria,fungi,and pollens in residential air...Air conditioning is a crucial participant in indoor air circulation and harmful microorganism transmission.To elucidate microbial contamination in air conditioning systems,bacteria,fungi,and pollens in residential air conditioning(AC)filters in Shanghai were revealed.The concentrations of fungal ITS(1,972,037±5,025,505 copies/cm^(2))in most filter samples were considerably higher than the 16S rRNA gene(21,587±21,461 copies/cm^(2)).The multitudinous bacteria determined a higher richness,whereas the trend was not in line with fungi,owing to Aspergillus flourishing,with an average of 43.75%.Numerous bacteria that may often be prevalent in human skin,mucous membranes,and intestines,such as Enhydrobacter,Micrococcus,Staphylococcus,Streptococcus,and Haemophilus,were also discovered in AC filters.The pollens were affiliated with Streptophyta at phylum,and Humulus was the most abundant genus(mean value 67.84%),raising the possibility of allergic responses.This study provides a better understanding of the microbial characteristics of AC filters,enables more rational approaches for microbe contaminant control,and ultimately improves human health in megacities.展开更多
Five Cu-ZSM-5 catalysts were obtained by treating Na-ZSM-5 (Si/Al ratio = 15) with aqueous solutions of differ- ent Cu precursors (CuCl2, Cu(NO3)2, CuSO4, Cu(CH3COO)2, and ammoniacal copper (II) complex ion)...Five Cu-ZSM-5 catalysts were obtained by treating Na-ZSM-5 (Si/Al ratio = 15) with aqueous solutions of differ- ent Cu precursors (CuCl2, Cu(NO3)2, CuSO4, Cu(CH3COO)2, and ammoniacal copper (II) complex ion). After being pretreated in flowing He at 500 ℃ to form active Cu+, these catalysts exhibited quite different activities in cata- lytic decomposition of N2O. CZM-AC(II) (prepared by ammoniacal copper (II) complex ion) with 9.4 wt% Cu con- tent was the most active among these Cu-ZSM-5 catalysts, achieving almost complete N2I conversion at 400 ℃. CZM-CA (prepared using Cu( CH3COO)2 as the Cu precursor) with 2.8 wt% Cu content was the second most active catalyst among these Cu-ZSM-5 catalysts, achieving almost complete N2I conversion at 425 ℃. CZM-CC, CZM- CN, and CZM-CS prepared by using CuCl2, Cu(NO3)2, or CuSO4 as the Cu precursor with similar Cu contents (≈1.7 wt%) were the least active among these Cu-ZSM-5 catalysts, achieving ca. 90% N2O conversion at 500 ℃. XRD, ICP, SEM, TEM, EDX-mapping, and CO-IR experiments were conducted to characterize relevant samples. The superior activity of CZM-AC(II) can be attributed to the high contents of total Cu+ and dimeric Cu+ among these samples. The influence of co-fed O2 or H2O on the catalytic performance of typical samples was also studied.展开更多
Organic acids are important contributors to the acidity of atmospheric precipitation,but their existence in the Chinese atmosphere is largely unclear.In this study,twelve atmospheric gaseous organic acids,including C_...Organic acids are important contributors to the acidity of atmospheric precipitation,but their existence in the Chinese atmosphere is largely unclear.In this study,twelve atmospheric gaseous organic acids,including C_(1)-C_(9) alkanoic acids,methacrylic acid,pyruvic acid,and benzoic acid,were observed in the suburb of Wangdu,Hebei Province,a typical rural site in the northern China plain from 16^(th) December,2018 to 22^(nd) January,2019,using a Vocus■ Proton-Transfer-Reaction time-of-flight mass spectrometer(Vocus PTR-ToF).The quantification of C_(2)-C_(4) alkanoic acids by the Vocus PTR-ToF was calibrated according to the titration of a NaOH solution by C_(2)-C_(4) alkanoic acids from home-made permeation sources,and the other organic acids except for formic acid were quantified based on the k_(cap)-sensitivity linearity in the Vocus PTR-ToF,whereas formic acid was not quantified because our instrument setting led to a significant underestimation in its concentration.The average total concentration of eleven gaseous organic acids was 6.96±5.20 ppbv(parts per billion by volume).The average concentration of acetic acid was the highest(3.86±3.00 ppbv),followed by propanoic acid,butyric acid,and methacrylic acid.Domestic straw burning was likely the dominant source of the observed gaseous organic acids according to the good correlations between acetonitrile and organic acids and between particulate K+and organic acids,and traffic emissions could also have contributed.During episodes with continuously high concentrations of organic acids,short-distance transport dominated in Wangdu according to the backward trajectory analysis.Baoding,Shijiazhuang,and Hengshui areas were the main source areas based on potential source contribution function and concentration weighing track analysis.展开更多
Porous g-C3N4samples were obtained by simply calcining bulk g-C3N4in static air in a muffle oven.The photocatalytic performance of these samples was evaluated through the removal of aqueous organic dyes(methylene blu...Porous g-C3N4samples were obtained by simply calcining bulk g-C3N4in static air in a muffle oven.The photocatalytic performance of these samples was evaluated through the removal of aqueous organic dyes(methylene blue and methyl orange)and tetracycline hydrochloride under visible-light irradiation(λ〉420 nm).Compared to bulk g-C3N4,porous g-C3N4exhibited much better capability for removing these contaminants,especially under visible-light irradiation,due to the enlarged specific surface area and more efficient separation of photogenerated charge carries.In particular,porous g-C3N4obtained by calcining bulk g-C3N4in air at 525℃ showed the highest visible-light-driven catalytic activity among these samples.Superoxide radical anions(·O2^-)were found to be the primary active species responsible for photodegradation.展开更多
The experiment was carried out in a cylindrical dielectric barrier discharge(DBD)reactor assisted with a catalyst to decompose toluene under different humidity.In order to explore the synergistic effect on removing ...The experiment was carried out in a cylindrical dielectric barrier discharge(DBD)reactor assisted with a catalyst to decompose toluene under different humidity.In order to explore the synergistic effect on removing toluene in the catalysis-DBD reactor,this paper investigated the decomposition efficiency and the energy consumption in the catalysis-DBD and the non-catalyst DBD reactors under different humidity.The results showed that the catalysis-DBD reactor had a better performance than the non-catalysis one at the humidity ratio of 0.4%,and the removal efficiency of toluene could reach 88.6% in the catalysis-DBD reactor,while it was only 59.9% in the non-catalytic reactor.However,there was no significant difference in the removal efficiency of toluene between the two reactors when the humidities were 1.2% and 2.4%.Additionally,the degradation products were also analyzed in order to gain a better understanding of the mechanism of decomposing toluene in a catalysis-DBD reactor.展开更多
The α-pinene ozonolysis under the different environmental conditions were observed in a smog chamber. The second-order rate constant (k) was determined to be (7.25 ± 0.06) x 10^-17 cm^3/(molecule.sec) unde...The α-pinene ozonolysis under the different environmental conditions were observed in a smog chamber. The second-order rate constant (k) was determined to be (7.25 ± 0.06) x 10^-17 cm^3/(molecule.sec) under 20% of relative humidity (RH) and room temperature. RH showed a marked influence on the α-pinene ozonolysis. The value of k increased with KH increase, which was 1.6 times faster at RH = 80% than that at RH = 20%. Additionally, the value of k apparently changed in the presence of the aerosol particles. The diesel soot increased the k value. The fly ash prohibited the reaction, however, H2SO4-treated fly ash promoted the reaction. The information of products gained using FT-IR and SPAMS showed that pinonic acid, 10-hydroxy-pinonic acid and pinic acid could be generated during the α- pinene ozonolysis. Water molecules could take part in the formation of the products, and play a vital role in the degradation of α-pinene. The atmospheric residence time calculation showed that the ozonolysis in the atmosphere is an important way of the α-pinene consumption as compared to that reacted with OH during daytime. The results suggested that the degradation of α-pinene via the ozonization in the atmosphere may be affected greatly by RH, as well as the presence of aerosol particles. The ozonolysis reaction may be an important way of the a-pinene consumption during daytime.展开更多
Airborne bacteria play key roles in terrestrial and marine ecosystems and human health,yet our understanding of bacterial communities and their response to the environmental variables lags significantly behind that of...Airborne bacteria play key roles in terrestrial and marine ecosystems and human health,yet our understanding of bacterial communities and their response to the environmental variables lags significantly behind that of other components of PM_(2.5).Here,atmospheric fine particles obtained from urban and suburb Shanghai were analyzed by using the qPCR and Illumina Miseq sequencing.The bacteria with an average concentration of 2.12× 10^(3 )cells/m^(3),were dominated by Sphingomonas,Curvibacter,Acinetobacter,Bradyrhizobium,Methylobacterium,Halomonas,Aliihoeflea,and Phyllobacterium,which were related to the nitrogen,carbon,sulfur cycling and human health risk.Our results provide a global survey of bacterial community across urban,suburb,and high-altitude sites.In Shanghai(China),urban PM2.5 harbour more diverse and dynamic bacterial populations than that in the suburb.The structural equation model explained about 27%,41%,and 20%^78%of the variance found in bacteria diversity,concentration,and discrepant genera among urban and suburb sites.This work furthered the knowledge of diverse bacteria in a coastal Megacity in the Yangtze river delta and emphasized the potential impact of environmental variables on bacterial community structure.展开更多
Landfill biogas is a potential alternative for fossil fuel,but the containing impurities,volatile methyl siloxanes(simplified as siloxanes),often cause serious problems in gas turbines when applied to generate electri...Landfill biogas is a potential alternative for fossil fuel,but the containing impurities,volatile methyl siloxanes(simplified as siloxanes),often cause serious problems in gas turbines when applied to generate electricity.In this research,a collecting and analyzing method based on solvent adsorption and purge and trap-gas chromatography-mass spectrometry was established to determine the siloxanes in biogas from a landfill in Jinan,China,and adjacent ambient samples,such as soil,air,and leachate of the landfill.The results showed that,octamethylcyclotetrasiloxane(D4)and decamethylcyclopentasiloxane(D5)accounted for 63%of total siloxanes;and without considering D4 and D5,the order of detected siloxanes in concentration was found relating to Gibbs free energies of molecules,namely that higher abundant siloxane(except for D4 and D5)usually had lower Gibbs free energy.Additionally,the mass ratio between D4 and octamethyltrisiloxane(L3)in the bio gas varied with different garbage age in landfills,possibly revealing the breaking-down of larger siloxane molecules with time.The samples,which were collected from environmental samples adjacent to the landfill,such as soil,water,and air,presented much higher siloxane level than urban or rural area away from landfills.The current H2 S scrubber of the landfill biogas could decrease the total siloxanes from 10.7 to 5.75 mg/m^3 due to Fe2 O3 and a refrigerant drier in a purification system and cyclic siloxanes were more easily removed than linear ones.展开更多
The significant increase of NO_(x)concentration causes severe damages to environment and human health.Light-driven photocatalytic technique affords an ideal solution for the removal of NO_(x)at ambient conditions.To e...The significant increase of NO_(x)concentration causes severe damages to environment and human health.Light-driven photocatalytic technique affords an ideal solution for the removal of NO_(x)at ambient conditions.To enhance the performance of NO_(x)removal,1D,2D and 3D photocatalysts have been constructed as the light absorption and the separation of charge carriers can be manipulated through controlling the morphology of the photocatalyst.Related works mainly focused on the construction and modification of special morphologic photocatalyst,including element doping,heterostructure constructing,crystal facet exposing,defect sites introducing and so on.Moreover,the excellent performance of the photocatalytic NO_(x)removal creates great awareness of the application,which has promising practical applications in NO_(x)removal by paint(removing NO_(x)indoor and outdoor)and pavement(degrading vehicle exhausts).For these considerations,recent advances in special morphologic photocatalysts for NO_(x)removal was summarized and commented in this review.The purpose is to provide insights into understanding the relationship between morphology and photocatalytic performance,meanwhile,to promote the application of photocatalytic technology in NO_(x)degradation.展开更多
基金supported by the Ministry of Science and Technology of China (No.2023YFC3708203)Daikin Industrial Co.,LTD (No.2021-01888),Science&Technology Commission of Shanghai Municipality (No.21DZ1202300)Shanghai International Science and Technology Partnership Project (No.21230780200).
文摘Air conditioning is a crucial participant in indoor air circulation and harmful microorganism transmission.To elucidate microbial contamination in air conditioning systems,bacteria,fungi,and pollens in residential air conditioning(AC)filters in Shanghai were revealed.The concentrations of fungal ITS(1,972,037±5,025,505 copies/cm^(2))in most filter samples were considerably higher than the 16S rRNA gene(21,587±21,461 copies/cm^(2)).The multitudinous bacteria determined a higher richness,whereas the trend was not in line with fungi,owing to Aspergillus flourishing,with an average of 43.75%.Numerous bacteria that may often be prevalent in human skin,mucous membranes,and intestines,such as Enhydrobacter,Micrococcus,Staphylococcus,Streptococcus,and Haemophilus,were also discovered in AC filters.The pollens were affiliated with Streptophyta at phylum,and Humulus was the most abundant genus(mean value 67.84%),raising the possibility of allergic responses.This study provides a better understanding of the microbial characteristics of AC filters,enables more rational approaches for microbe contaminant control,and ultimately improves human health in megacities.
基金Supported by the National Natural Science Foundation of China(Grant No.21477022)
文摘Five Cu-ZSM-5 catalysts were obtained by treating Na-ZSM-5 (Si/Al ratio = 15) with aqueous solutions of differ- ent Cu precursors (CuCl2, Cu(NO3)2, CuSO4, Cu(CH3COO)2, and ammoniacal copper (II) complex ion). After being pretreated in flowing He at 500 ℃ to form active Cu+, these catalysts exhibited quite different activities in cata- lytic decomposition of N2O. CZM-AC(II) (prepared by ammoniacal copper (II) complex ion) with 9.4 wt% Cu con- tent was the most active among these Cu-ZSM-5 catalysts, achieving almost complete N2I conversion at 400 ℃. CZM-CA (prepared using Cu( CH3COO)2 as the Cu precursor) with 2.8 wt% Cu content was the second most active catalyst among these Cu-ZSM-5 catalysts, achieving almost complete N2I conversion at 425 ℃. CZM-CC, CZM- CN, and CZM-CS prepared by using CuCl2, Cu(NO3)2, or CuSO4 as the Cu precursor with similar Cu contents (≈1.7 wt%) were the least active among these Cu-ZSM-5 catalysts, achieving ca. 90% N2O conversion at 500 ℃. XRD, ICP, SEM, TEM, EDX-mapping, and CO-IR experiments were conducted to characterize relevant samples. The superior activity of CZM-AC(II) can be attributed to the high contents of total Cu+ and dimeric Cu+ among these samples. The influence of co-fed O2 or H2O on the catalytic performance of typical samples was also studied.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.21925601,91644213)the National Key R&D Program of China(No.2017YFC0209505).
文摘Organic acids are important contributors to the acidity of atmospheric precipitation,but their existence in the Chinese atmosphere is largely unclear.In this study,twelve atmospheric gaseous organic acids,including C_(1)-C_(9) alkanoic acids,methacrylic acid,pyruvic acid,and benzoic acid,were observed in the suburb of Wangdu,Hebei Province,a typical rural site in the northern China plain from 16^(th) December,2018 to 22^(nd) January,2019,using a Vocus■ Proton-Transfer-Reaction time-of-flight mass spectrometer(Vocus PTR-ToF).The quantification of C_(2)-C_(4) alkanoic acids by the Vocus PTR-ToF was calibrated according to the titration of a NaOH solution by C_(2)-C_(4) alkanoic acids from home-made permeation sources,and the other organic acids except for formic acid were quantified based on the k_(cap)-sensitivity linearity in the Vocus PTR-ToF,whereas formic acid was not quantified because our instrument setting led to a significant underestimation in its concentration.The average total concentration of eleven gaseous organic acids was 6.96±5.20 ppbv(parts per billion by volume).The average concentration of acetic acid was the highest(3.86±3.00 ppbv),followed by propanoic acid,butyric acid,and methacrylic acid.Domestic straw burning was likely the dominant source of the observed gaseous organic acids according to the good correlations between acetonitrile and organic acids and between particulate K+and organic acids,and traffic emissions could also have contributed.During episodes with continuously high concentrations of organic acids,short-distance transport dominated in Wangdu according to the backward trajectory analysis.Baoding,Shijiazhuang,and Hengshui areas were the main source areas based on potential source contribution function and concentration weighing track analysis.
基金Supported by the National Natural Science Foundation of China(Grant No.21477022)
文摘Porous g-C3N4samples were obtained by simply calcining bulk g-C3N4in static air in a muffle oven.The photocatalytic performance of these samples was evaluated through the removal of aqueous organic dyes(methylene blue and methyl orange)and tetracycline hydrochloride under visible-light irradiation(λ〉420 nm).Compared to bulk g-C3N4,porous g-C3N4exhibited much better capability for removing these contaminants,especially under visible-light irradiation,due to the enlarged specific surface area and more efficient separation of photogenerated charge carries.In particular,porous g-C3N4obtained by calcining bulk g-C3N4in air at 525℃ showed the highest visible-light-driven catalytic activity among these samples.Superoxide radical anions(·O2^-)were found to be the primary active species responsible for photodegradation.
基金supported by the Key Project which is sponsored by the Science and Technology Commission of Shanghai Municipality(No.13231201903)the Key Programs for Science and Technology Development sponsored by the Science and Technology Commission of Shanghai Municipality(Nos.13231201901 and 14DZ1208401)the Key Project sponsored by the State-owned Assets Supervision and Administration Commission of Shanghai,China(No.2013019)
文摘The experiment was carried out in a cylindrical dielectric barrier discharge(DBD)reactor assisted with a catalyst to decompose toluene under different humidity.In order to explore the synergistic effect on removing toluene in the catalysis-DBD reactor,this paper investigated the decomposition efficiency and the energy consumption in the catalysis-DBD and the non-catalyst DBD reactors under different humidity.The results showed that the catalysis-DBD reactor had a better performance than the non-catalysis one at the humidity ratio of 0.4%,and the removal efficiency of toluene could reach 88.6% in the catalysis-DBD reactor,while it was only 59.9% in the non-catalytic reactor.However,there was no significant difference in the removal efficiency of toluene between the two reactors when the humidities were 1.2% and 2.4%.Additionally,the degradation products were also analyzed in order to gain a better understanding of the mechanism of decomposing toluene in a catalysis-DBD reactor.
基金supported by the Ministry of Science and Technology of China(Nos.2016YFC0202700,2016YFE0112200,2014BAC22B01)the National Natural Science Foundation of China(Nos.21527814,21077025)the Marie Sklodowska Curie Actions(Nos.690958-MARSU-RISE-2015)
文摘The α-pinene ozonolysis under the different environmental conditions were observed in a smog chamber. The second-order rate constant (k) was determined to be (7.25 ± 0.06) x 10^-17 cm^3/(molecule.sec) under 20% of relative humidity (RH) and room temperature. RH showed a marked influence on the α-pinene ozonolysis. The value of k increased with KH increase, which was 1.6 times faster at RH = 80% than that at RH = 20%. Additionally, the value of k apparently changed in the presence of the aerosol particles. The diesel soot increased the k value. The fly ash prohibited the reaction, however, H2SO4-treated fly ash promoted the reaction. The information of products gained using FT-IR and SPAMS showed that pinonic acid, 10-hydroxy-pinonic acid and pinic acid could be generated during the α- pinene ozonolysis. Water molecules could take part in the formation of the products, and play a vital role in the degradation of α-pinene. The atmospheric residence time calculation showed that the ozonolysis in the atmosphere is an important way of the α-pinene consumption as compared to that reacted with OH during daytime. The results suggested that the degradation of α-pinene via the ozonization in the atmosphere may be affected greatly by RH, as well as the presence of aerosol particles. The ozonolysis reaction may be an important way of the a-pinene consumption during daytime.
基金by the Shanghai Sailing Program(19YF1403200)National Natural Science Foundation of China(Grant Nos.21906023,91843301,91743202,21527814)+2 种基金Ministry of Science and Technology of China(No.2016YFC0202700)Marie Skto-dowska-Curie Actions(690958-MARSU-RISE-2015)China Postdoctoral Science Foundation(No.2018M640331).
文摘Airborne bacteria play key roles in terrestrial and marine ecosystems and human health,yet our understanding of bacterial communities and their response to the environmental variables lags significantly behind that of other components of PM_(2.5).Here,atmospheric fine particles obtained from urban and suburb Shanghai were analyzed by using the qPCR and Illumina Miseq sequencing.The bacteria with an average concentration of 2.12× 10^(3 )cells/m^(3),were dominated by Sphingomonas,Curvibacter,Acinetobacter,Bradyrhizobium,Methylobacterium,Halomonas,Aliihoeflea,and Phyllobacterium,which were related to the nitrogen,carbon,sulfur cycling and human health risk.Our results provide a global survey of bacterial community across urban,suburb,and high-altitude sites.In Shanghai(China),urban PM2.5 harbour more diverse and dynamic bacterial populations than that in the suburb.The structural equation model explained about 27%,41%,and 20%^78%of the variance found in bacteria diversity,concentration,and discrepant genera among urban and suburb sites.This work furthered the knowledge of diverse bacteria in a coastal Megacity in the Yangtze river delta and emphasized the potential impact of environmental variables on bacterial community structure.
基金supported by the National Natural Science Foundation of China(No.21407097)Supported by Shandong Key Laboratory of Water Pollution Control and Resource Reuse(No.2019KF14)the Opening Project of Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP^3)(No.FDLAP17001)
文摘Landfill biogas is a potential alternative for fossil fuel,but the containing impurities,volatile methyl siloxanes(simplified as siloxanes),often cause serious problems in gas turbines when applied to generate electricity.In this research,a collecting and analyzing method based on solvent adsorption and purge and trap-gas chromatography-mass spectrometry was established to determine the siloxanes in biogas from a landfill in Jinan,China,and adjacent ambient samples,such as soil,air,and leachate of the landfill.The results showed that,octamethylcyclotetrasiloxane(D4)and decamethylcyclopentasiloxane(D5)accounted for 63%of total siloxanes;and without considering D4 and D5,the order of detected siloxanes in concentration was found relating to Gibbs free energies of molecules,namely that higher abundant siloxane(except for D4 and D5)usually had lower Gibbs free energy.Additionally,the mass ratio between D4 and octamethyltrisiloxane(L3)in the bio gas varied with different garbage age in landfills,possibly revealing the breaking-down of larger siloxane molecules with time.The samples,which were collected from environmental samples adjacent to the landfill,such as soil,water,and air,presented much higher siloxane level than urban or rural area away from landfills.The current H2 S scrubber of the landfill biogas could decrease the total siloxanes from 10.7 to 5.75 mg/m^3 due to Fe2 O3 and a refrigerant drier in a purification system and cyclic siloxanes were more easily removed than linear ones.
基金supported by the National Natural Science Foundation of China(Nos.21607027,52002142,51772118,and 51972134)the Opening Project of Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention(LAP3,No.FDLAP19007)+2 种基金and some Foundation of Anhui Province in China:Natural Science Foundation(Nos.1808085J24 and 2108085MB43)the University Natural Science Research Project(No.KJ2020A0126)the Cultivating Outstanding Talents(No.gxbjZD2020066).
文摘The significant increase of NO_(x)concentration causes severe damages to environment and human health.Light-driven photocatalytic technique affords an ideal solution for the removal of NO_(x)at ambient conditions.To enhance the performance of NO_(x)removal,1D,2D and 3D photocatalysts have been constructed as the light absorption and the separation of charge carriers can be manipulated through controlling the morphology of the photocatalyst.Related works mainly focused on the construction and modification of special morphologic photocatalyst,including element doping,heterostructure constructing,crystal facet exposing,defect sites introducing and so on.Moreover,the excellent performance of the photocatalytic NO_(x)removal creates great awareness of the application,which has promising practical applications in NO_(x)removal by paint(removing NO_(x)indoor and outdoor)and pavement(degrading vehicle exhausts).For these considerations,recent advances in special morphologic photocatalysts for NO_(x)removal was summarized and commented in this review.The purpose is to provide insights into understanding the relationship between morphology and photocatalytic performance,meanwhile,to promote the application of photocatalytic technology in NO_(x)degradation.