Photocatalytic degradation of gaseous pollutants on Bi-based semiconductors under solar lightirradiation has attracted significant attention.However,their application in gaseous straight-chainalkane purification is st...Photocatalytic degradation of gaseous pollutants on Bi-based semiconductors under solar lightirradiation has attracted significant attention.However,their application in gaseous straight-chainalkane purification is still rare.Here,a series of Bi/BiOBr composites were solvothermally synthe-sized and applied in solar-light-driven photocatalytic degradation of gaseous n-hexane.The charac-terization results revealed that both increasing number of functional groups of alcohol solvent(from methanol and ethylene glycol to glycerol)and solvothermal temperature(from 160 and 180to 200℃)facilitated the in-situ formation of metallic Bi nanospheres on BiOBr nanoplates withexposed(110)facets.Meanwhile,chemical bonding between Bi and BiOBr was observed on theseexposed facets that resulted in the formation of surface oxygen vacancy.Furthermore,the synergis-tic effect of optimum surface oxygen vacancy on exposed(110)facets led to a high visible light re-sponse,narrow band gap,great photocurrent,low recombination rate of the charge carriers,andstrong·O2-and h*formation,all of which resulted in the highest removal efficiency of 97.4%within120 min of 15 ppmv of n-hexane on Bi/BiOBr.Our findings efficiently broaden the application ofBi-based photocatalysis technology in the purification of gaseous straight-chain pollutants emittedby the petrochemical industry.展开更多
Surface defect modulation has emerged as a potential strategy for promoting the photocatalytic activity of photocatalysts for various applications, while the impact of the oxygen vacancy on bacterial inactivation is s...Surface defect modulation has emerged as a potential strategy for promoting the photocatalytic activity of photocatalysts for various applications, while the impact of the oxygen vacancy on bacterial inactivation is still debated. In this study, oxygen vacancies were introduced to tungsten trioxide nanosheets(WO3–x) via a microwave-assisted route. The as-prepared WO3–x nanosheets exhibited excellent visible-light-driven photocatalytic activity toward E. coli K-12 inactivation, and 6 log orders of the bacterial cells could be completely inactivated within 150 min. The obtained bacterial inactivation rate constant was 15.2 times higher than that of pristine WO3 without oxygen vacancies, suggesting that the surface oxygen vacancy could significantly promote the bacterial inactivation efficiency. The mechanism study indicated that the inactivation of bacterial cells occurs via a direct h+ oxidation pathway. In addition, the role of the oxygen vacancy was studied in detail;the oxygen vacancy was found to not only promote interfacial charge separation but also tune the band structure of WO3, thereby leading to increased h+ oxidation power. Finally, a possible oxygen vacancy-dominated photocatalytic bacterial inactivation mechanism is proposed. This work is expected to offer new insights into the microwave-assisted synthesis of defective photocatalysts and the use of the oxygen vacancy for promoting photocatalytic antibacterial activities.展开更多
Formaldehyde(HCHO) is a common indoor pollutant, long-term exposure to HCHO may harm human health. Its efficient removal at mild conditions is still challenging. The catalytic oxidation of HCHO molecules on a single a...Formaldehyde(HCHO) is a common indoor pollutant, long-term exposure to HCHO may harm human health. Its efficient removal at mild conditions is still challenging. The catalytic oxidation of HCHO molecules on a single atomic catalyst, Ti-decorated Ti3C2O2(Ti/Ti3C2O2) monolayer, is investigated by performing the first principles calculations in this work. It demonstrates that Ti atoms can be easily well dispersed at the form of single atom on Ti3C2O2 monolayer without aggregation. For HCHO catalytic oxidation, both Langmuir-Hinshelwood(LH) and Eley-Rideal(ER) mechanisms are considered. The results show that the step of HCHO dissociative adsorption on Ti/Ti3C2O2 with activated O2 can release high energy of 4.05 e V based on the ER mechanism, which can help to overcome the energy barrier(1.04 e V) of the subsequent reaction steps. The charge transfer from *OH group to CO molecule(dissociated from HCHO) not only promotes *OH group activation but also plays an important role in the H2 O generation along the ER mechanism. Therefore, HCHO can be oxidized easily on Ti/Ti3C2O2 monolayer, this work could provide significant guidance to develop effective non-noble metal catalysts for HCHO oxidation and broaden the applications of MXene-based materials.展开更多
Industrial coking facilities are an important emission source for volatile organic compounds(VOCs).This study analyzed the atmospheric VOC characteristics within an industrial coking facility and its surrounding envir...Industrial coking facilities are an important emission source for volatile organic compounds(VOCs).This study analyzed the atmospheric VOC characteristics within an industrial coking facility and its surrounding environment.Average concentrations of total VOCs(TVOCs)in the surrounding residential activity areas(R1 and R2),the coking facility(CF)and the control area(CA)were determined to be 138.5,47.8,550.0,and 15.0μg/m^(3),respectively.The cold drum process and coking and quenching areas within the coking facility were identified as the main polluting processes.The spatial variation in VOCs composition was analyzed,showing that VOCs in the coking facility and surrounding areas were mainly dominated by aromatic compounds such as BTX(benzene,toluene,and xylenes)and naphthalene,with concentrations being negatively correlated with the distance from the coking facility(p<0.01).The sources of VOCs in different functional areas across the monitoring area were analyzed,finding that coking emissions accounted for 73.5%,33.3% and 27.7% of TVOCs in CF,R1 and R2,respectively.These results demonstrated that coking emissions had a significant impact on VOC concentrations in the areas surrounding coking facility.This study evaluates the spatial variation in exposure to VOCs,providing important information for the influence of VOCs concentration posed by coking facility to surrounding residents and the development of strategies for VOC abatement.展开更多
Corona virus disease 2019(COVID-19)has exerted a profound adverse impact on human health.Studies have demonstrated that aerosol transmission is one of the major transmission routes of severe acute respiratory syndrome...Corona virus disease 2019(COVID-19)has exerted a profound adverse impact on human health.Studies have demonstrated that aerosol transmission is one of the major transmission routes of severe acute respiratory syndrome coronavirus 2(SARS-CoV-2).Pathogenic microorganisms such as SARS-CoV-2 can survive in the air and cause widespread infection among people.Early monitoring of pathogenic microorganism transmission in the atmosphere and accurate epidemic prediction are the frontier guarantee for preventing large-scale epidemic outbreaks.Monitoring of pathogenic microorganisms in the air,especially in densely populated areas,may raise the possibility to detect viruses before people are widely infected and contain the epidemic at an earlier stage.The multi-scale coupled accurate epidemic prediction system can provide support for governments to analyze the epidemic situation,allocate health resources,and formulate epidemic response policies.This review first elaborates on the effects of the atmospheric environment on pathogenic microorganism transmission,which lays a theoretical foundation for the monitoring and prediction of epidemic development.Secondly,the monitoring technique development and the necessity of monitoring pathogenic microorganisms in the atmosphere are summarized and emphasized.Subsequently,this review introduces the major epidemic prediction methods and highlights the significance to realize a multi-scale coupled epidemic prediction system by strengthening the multidisciplinary cooperation of epidemiology,atmospheric sciences,environmental sciences,sociology,demography,etc.By summarizing the achievements and challenges in monitoring and prediction of pathogenic microorganism transmission in the atmosphere,this review proposes suggestions for epidemic response,namely,the establishment of an integrated monitoring and prediction platform for pathogenic microorganism transmission in the atmosphere.展开更多
Environmental pollution is escalating due to rapid global development that often prioritizes human needs over planetary health.Despite global efforts to mitigate legacy pollutants,the continuous introduction of new su...Environmental pollution is escalating due to rapid global development that often prioritizes human needs over planetary health.Despite global efforts to mitigate legacy pollutants,the continuous introduction of new substances remains a major threat to both people and the planet.In response,global initiatives are focusing on risk assessment and regulation of emerging contaminants,as demonstrated by the ongoing efforts to establish the UN’s Intergovernmental Science-Policy Panel on Chemicals,Waste,and Pollution Prevention.This review identifies the sources and impacts of emerging contaminants on planetary health,emphasizing the importance of adopting a One Health approach.Strategies for monitoring and addressing these pollutants are discussed,underscoring the need for robust and socially equitable environmental policies at both regional and international levels.Urgent actions are needed to transition toward sustainable pollution management practices to safeguard our planet for future generations.展开更多
Acetylacetone(AcAc)is a typical class ofβ-diketones with broad industrial applications due to the property of the keto-enol isomers,but its isomerization and chemical reactions at the air-droplet interface are still ...Acetylacetone(AcAc)is a typical class ofβ-diketones with broad industrial applications due to the property of the keto-enol isomers,but its isomerization and chemical reactions at the air-droplet interface are still unclear.Hence,using combined molecular dynamics and quantum chemistry methods,the heterogeneous chemistry of AcAc at the air-droplet interface was investigated,including the attraction of AcAc isomers by the droplets,the distribution of isomers at the air-droplet interface,and the hydration reactions of isomers at the air-droplet interface.The results reveal that the preferential orientation of two AcAc isomers(keto-and enol-AcAc)to accumulate and accommodate at the acidic air-droplet interface.The isomerization of two AcAc isomers at the acidic air-droplet interface is more favorable than that at the neutral air-droplet interface because the“water bridge”structure is destroyed by H_(3)O^(+),especially for the isomerization from keto-Ac Ac to enol-AcAc.At the acidic air-droplet interface,the carbonyl or hydroxyl O-atoms of two AcAc isomers display an energetical preference to hydration.Keto-diol is the dominant products to accumulate at the air-droplet interface,and excessive keto-diol can enter the droplet interior to engage in the oligomerization.The photooxidation reaction of AcAc will increase the acidity of the air-droplet interface,which indirectly facilitate the uptake and formation of more keto-diol.Our results provide an insight into the heterogeneous chemistry ofβ-diketones and their influence on the environment.展开更多
There is an urgent need for developing cost-effective methods for the treatment of perfluorooctanoic acid(PFOA)due to its global emergence and potential risks.In this study,taking surface-defective BiOCl as an example...There is an urgent need for developing cost-effective methods for the treatment of perfluorooctanoic acid(PFOA)due to its global emergence and potential risks.In this study,taking surface-defective BiOCl as an example,a strategy of surface oxygen vacancy modulation was used to promote the photocatalytic defluorination efficiency of PFOA under simulated sunlight irradiation.The defective BiOCl was fabricated by a fast microwave solvothermal method,which was found to induce more surface oxygen vacancies than conventional solvothermal and precipitation methods.As a result,the asprepared BiOCl showed significantly enhanced defluorination efficiency,which was 2.7 and33.8 times higher than that of BiOCl fabricated by conventional solvothermal and precipitation methods,respectively.Mechanistic studies indicated that the defluorination of PFOA follows a direct hole(h^+)oxidation pathway with the aid of·OH,while the oxygen vacancies not only promote charge separation but also facilitate the intimate contact between the photocatalyst surface and PFOA by coordinating with its terminal carboxylate group in a bidentate or bridging mode.This work will provide a general strategy of oxygen vacancy modulation by microwave-assisted methods for efficient photocatalytic defluorination of PFOA in the environment using sunlight as the energy source.展开更多
Recent pandemic outbreak of the corona-virus disease 2019(COVID-19)has raised widespread concerns about the importance of the bioaerosols.They are atmospheric aerosol particles of biological origins,mainly including b...Recent pandemic outbreak of the corona-virus disease 2019(COVID-19)has raised widespread concerns about the importance of the bioaerosols.They are atmospheric aerosol particles of biological origins,mainly including bacteria,fungi,viruses,pollen,and cell debris.Bioaerosols can exert a substantial impact on ecosystems,climate change,air quality,and public health.Here,we review several relevant topics on bioaerosols,including sampling and detection techniques,characterization,effects on health and air quality,and control methods.However,very few studies have focused on the source apportionment and transport of bioaerosols.The knowledge of the sources and transport pathways of bioaerosols is essential for a comprehensive understanding of the role microorganisms play in the atmosphere and control the spread of epidemic diseases associated with them.Therefore,this review comprehensively summarizes the up to date progress on the source characteristics,source identification,and diffusion and transport process of bioaerosols.We intercompare three types of diffusion and transport models,with a special emphasis on a widely used mathematical model.This review also highlights the main factors affecting the source emission and transport process,such as biogeographic regions,land-use types,and environmental factors.Finally,this review outlines future perspectives on bioaerosols.展开更多
Formaldehyde(HCHO) is one kind of common indoor toxic pollutant,the catalytic oxidation degradation of formaldehyde at room temperature is desired.In this work,a new single atomic catalyst(SAC),Al doped graphene,for t...Formaldehyde(HCHO) is one kind of common indoor toxic pollutant,the catalytic oxidation degradation of formaldehyde at room temperature is desired.In this work,a new single atomic catalyst(SAC),Al doped graphene,for the catalytic oxidation of HCHO molecules was proposed through density function theory(DFT) calculations.It is found that Al atoms can be adsorbed on graphene stably without aggre s sion.Then HCHO can be effectively oxidized into CO2 and H2 O in the presence of O2 molecules on Al doped graphene with a low energy barrier of 0.82 eV and releasing energy of 2.29 eV with the pathway of HCHO→HCOOH→CO→CO2.The oxidation reaction can happen promptly with reaction time τ=56.9 s at the speed control step at room temperature.Therefore,this work proposed a high-performance catalyst Al-doped graphene without any noble metal for HCHO oxidation at ambient temperature,and corresponding oxidation pathway and mechanism are also deeply understood.展开更多
Fugitive emission has been becoming an important source of volatile organic compounds(VOCs) in pharmaceutical industry,but the exact contribution of fugitive emission remains incompletely understood.In present study,p...Fugitive emission has been becoming an important source of volatile organic compounds(VOCs) in pharmaceutical industry,but the exact contribution of fugitive emission remains incompletely understood.In present study,pollution characteristics,odorous activity and health risk of stack and fugitive emissions of VOCs from four functional units (e.g.,workshop,sewage treatment station,raw material storage and hazardous waste storage) of three representative pharmaceutical factories were investigated.Workshop was the dominant contributor to VOCs of fugitive emission in comparison with other functional units.Extreme high concentration of VOCs from fugitive emission in unsealed workshop (94.87 mg/m^(3))was observed relative to sealed one (1.18 mg/m^(3)),accounting for 31%and 5%of total VOCs,respectively.Fugitive emission of VOCs in the unsealed workshop mainly consisted of nhexane,1-hexene and dichloromethane.Odorous activity indexes and non-cancer hazard ratios of these VOCs from fugitive emission in the unsealed workshop were as high as that from stack exhaust.Furthermore,cancer risk of dichloromethane from fugitive emission and stack exhaust was up to (1.6-1.8)×10^(-5).Odorous activity or health risk index of the VOCs from fugitive emission was up to 13 or 11 times of the corresponding threshold value,posing remarkable health threat on pharmaceutical workers.Our?ndings highlighted the possibly underestimated contribution of fugitive emission on VOCs in the pharmaceutical industry.展开更多
Explore the photo-piezoelectric synergistic micro-mechanism by density functional theory(DFT)calculations at the electronic and atomic level is important.In this work,to understand the synergistic mechanism,atomic and...Explore the photo-piezoelectric synergistic micro-mechanism by density functional theory(DFT)calculations at the electronic and atomic level is important.In this work,to understand the synergistic mechanism,atomic and electronic properties of typical piezoelectric and photocatalytic material BaTiO_(3)were initially investigated with different strains.Subsequently,the adsorption of volatile organic compounds(VOCs)on the BaTiO_(3)(001)surface was determined during the piezoelectric process.In addition,the relationship between deformation ratio,the electronic structure and adsorption energy was understood in the deformation ratio range of 7%-12%for the optimal catalytic effect.The results of charge density differences and Born effective charge reveal the synergistic mechanism of piezoelectric photocatalysis.The built-in electric field formed by polarization results in the enhanced separation of charges,which makes the surface charges aggregation,enhancing the adsorption of VOCs,and benefiting the subsequent photocatalytic degradation.This work can provide significant theoretical guidance for the piezoelectric photocatalytic degradation of pollutants with the optimal strain range.展开更多
Rapid economic development and industrialization have left many risk sites around the world with significant or potential soil contamination due to industrial production or the shutdown or relocation of industrial fac...Rapid economic development and industrialization have left many risk sites around the world with significant or potential soil contamination due to industrial production or the shutdown or relocation of industrial facilities.Soil pollutants pose significant threats to human health,especially at sites used by the chemical,mining,and metalworking industries,among others[1].展开更多
The application of nanoscale zero-valent iron(nZVI) for the degradation of contaminants has been extensively investigated, however, few studies have focused on degradation in high salinity environments. In this study,...The application of nanoscale zero-valent iron(nZVI) for the degradation of contaminants has been extensively investigated, however, few studies have focused on degradation in high salinity environments. In this study, the ability of bare and carboxymethyl cellulose(CMC)-coated bimetallic Pd-nZVI particles to degrade 33′44′-tetrachlorobiphenyl in high saline water(SW) is examined with particular attention given to the effects of ethylenediaminetetraacetic acid(EDTA) on the rate of degradation. EDTA enhances the reactivity of Pd-nZVI in SW, with evidence provided to link this to the removal of the passivating layer. Additionally, a conceptual model is proposed which provides a quantitative description of the removal of these iron oxide layers in the presence of EDTA. An optimum EDTA to bare Pd-nZVI molar ratio of 0.1 exists, with insufficient EDTA unable to remove the passivating layer whilst excess EDTA results in Fe loss and enhanced agglomeration due to magnetic attraction of the bare Fe(0) particles. In contrast, CMCcoating of Pd-nZVI assemblages actually impedes degradation, despite the coated particles displaying a smaller average size compared to uncoated particles, with even the presence of EDTA in this case not significantly improving degradation. The reduced reactivity in the presence of CMC is primarily attributed to the effect of CMC on the association of Pd with nZVI particles. In particular, the presence of CMC reduced the total amount of Pd incorporated with the stabilized particles compared to the non-stabilized particles.Additionally, the presence of CMC results in less Pd present in its reactive zero-valent oxidation state.展开更多
Increasing attention has been paid to the air pollution more recently. Smog chamber has been proved as a necessary and effective tool to study atmospheric processes, including photochemical smog and haze formation. A ...Increasing attention has been paid to the air pollution more recently. Smog chamber has been proved as a necessary and effective tool to study atmospheric processes, including photochemical smog and haze formation. A novel smog chamber was designed to study the atmospheric photochemical reaction mechanism of typical volatile organic compounds(VOCs) as well as the aging of aerosols. The smog chamber system includes an enclosure equipped with black lights as the light source, two parallel reactors(2 m^3 of each) with separate control of light source and temperature, with a series of coupled instruments for online monitoring of gas phase and particle phase reactants and products. Chamber characterization, including air source stability, effective light intensity, temperature stability, as well as gas phase and particle phase wall losses, were carried out before further research. The results showed that our smog chamber systems developed by other domestic and international groups. It was also observed that the wall loss of aromatic VOCs varied with different functional groups as well as the isomerism. The results of preliminary simulation experiment from styrene-NO_x demonstrated that the chamber can be well utilized to simulate gas-particle conversion progresses in the atmosphere.展开更多
Personal care products(PCPs)inevitably come into contact with the skin in people’s daily life,potentially causing adverse effects on human health.The adverse effects can be exacerbated under UV irradiation but are ra...Personal care products(PCPs)inevitably come into contact with the skin in people’s daily life,potentially causing adverse effects on human health.The adverse effects can be exacerbated under UV irradiation but are rarely studied.In this study,to clearly understand the damage of representative PCPs to human skin and their photochemical transformation behaviors,fragrance tonalide(AHTN)was measured in the presence of amino acids as a basic building block of human tissue.The results showed that amino acids could decelerate the photochemical transformation rate of AHTN,increasing the likelihood of AHNT persisting on the skin surface and the health risk to the human being.Further,the interaction between amino acids and AHTN was investigated.AHTN could play bidirectional roles in damaging amino acids:the photosensitizer and reactive activator.As a photosensitizer,the ^(1)O_(2) generated from the AHTN photosensitization was partly employed to oxidative damage amino acids.Furthermore,by combining experiments with quantum chemical computation,the carbonyl group of the activator AHTN was found to be the active site to activate the N-containing group of amino acids.The activation mechanism was the electron transfer between AHTN and amino acids.Imines formed during the photochemical transformation of AHTN with histidine/glycine were the molecular initiating event for potential skin sensitization.This study reported for the first time that skin photosensitizer formation threatens human health during the photochemical transformation of AHTN.展开更多
Pathogenic microbes with antibiotic resistance can thrive on municipal solid waste as nutrients and be aerosolized and transported to vicinities during waste disposal processes.However,the characterization of pathogen...Pathogenic microbes with antibiotic resistance can thrive on municipal solid waste as nutrients and be aerosolized and transported to vicinities during waste disposal processes.However,the characterization of pathogenic bioaerosols and assessment of their exposure risks are lacking.Herein,particle size,concentration,activity,antibiotic resistance,and pathogenicity of airborne microorganisms were assessed in different sectors of a typical landfill.Results showed that active sector in downwind direction has the highest bioaerosol level(1234 CFU/m3),while residential area has the highest activity(14.82 mg/L).Botanical deodorizer from mist cannon can effectively remove bioaerosol.Most bioaerosols can be inhaled into respiratory system till bronchi with sizes ranging from 2.1−3.3 and 3.3−4.7μm.Pathogenic bacteria(Bacilli,Bacillus,and Burkholderia-Paraburkholderia)and allergenic fungi(Aspergillus,Cladosporium,and Curvularia)prevailed in landfill.Although high abundance of microbial volatile organic compounds(mVOCs)producing bioaerosols were detected,these mVOCs contributed little to odor issues in landfill.Notably,surrounding areas have higher levels of antibiotic-resistance genes(ARGs)than inner landfill with tetC,acrB,acrF,mdtF,and bacA as dominant ones.Most ARGs were significantly correlated with bacterial community,while environmental parameters mainly influenced fungal prevalence.These findings can assist in reducing and preventing respiratory allergy or infection risks in occupational environments relating to waste management.展开更多
Rational design and synthesis of highly efficient and robust photocatalysts with positive exciton splitting and interfacial charge transfer for environmental applications is critical.Herein,aiming at overcoming the co...Rational design and synthesis of highly efficient and robust photocatalysts with positive exciton splitting and interfacial charge transfer for environmental applications is critical.Herein,aiming at overcoming the common shortcomings of traditional photocatalysts such as weak photoresponsivity,rapid combination of photo-generated carriers and unstable structure,a novel Ag-bridged dual Z-scheme g-C_(3)N_(4)/BiOI/AgI plasmonic heterojunction was successfully synthesized using a facile method.Results showed that Ag-AgI nanoparticles and three-dimensional(3D)BiOI microspheres were decorated highly uniformly on the 3D porous g-C_(3)N_(4) nanosheet,resulting in a higher specific surface area and abundant active sites.The optimized 3D porous dual Z-scheme g-C_(3)N_(4)/BiOI/Ag-AgI manifested exceptional photocatalytic degradation efficiency of tetracycline(TC)in water with approximately 91.8%degradation efficiency within 165 min,outperforming majority of the reported g-C_(3)N_(4)-based photocatalysts.Moreover,g-C_(3)N_(4)/BiOI/Ag-AgI exhibited good stability in terms of activity and structure.In-depth radical scavenging and electron paramagnetic resonance(EPR)analyses confirmed the relative contributions of various scavengers.Mechanism analysis indicated that the improved photocatalytic performance and stability were ascribed to the highly ordered 3D porous framework,fast electron transfer of dual Z-scheme heterojunction,desirable photocatalytic performance of BiOI/AgI and synergistic effect of Ag plasmas.Therefore,the 3D porous Z-scheme g-C_(3)N_(4)/BiOI/Ag-AgI heterojunction had a good prospect for applications in water remediation.The current work provides new insight and useful guidance for designing novel structural photocatalysts for environment-related applications.展开更多
Organosulfate (OSA) nanoparticles,as secondary organic aerosol (SOA) compositions,are ubiquitous in urban and rural environments.Hence,we systemically investigated the mechanisms and kinetics of aqueous-phase reaction...Organosulfate (OSA) nanoparticles,as secondary organic aerosol (SOA) compositions,are ubiquitous in urban and rural environments.Hence,we systemically investigated the mechanisms and kinetics of aqueous-phase reactions of 1-butanol/1-decanol (BOL/DOL) and their roles in the formation of OSA nanoparticles by using quantum chemical and kinetic calculations.The mechanism results show that the aqueous-phase reactions of BOL/DOL start from initial protonation at alcoholic OH^(-)groups to form carbenium ions (CBs),which engage in the subsequent esterification or oligomerization reactions to form OSAs/organosulfites (OSIs) or dimers.The kinetic results reveal that dehydration to form CBs for BOL and DOL reaction systems is the rate-limiting step.Subsequently,about 18%of CBs occur via oligomerization to dimers,which are difficult to further oligomerize because all reactive sites are occupied.The rate constant of BOL reaction system is one order of magnitude larger than that of DOL reaction system,implying that relative short-chain alcohols are more prone to contribute OSAs/OSIs than long-chain alcohols.Our results reveal that typical long-chain alcohols contribute SOA formation via esterification rather than oligomerization because OSA/OSI produced by esterification engages in nanoparticle growth through enhancing hygroscopicity.展开更多
As more attention is being paid to the characteristics of atmospheric amines,there is also an increasing demand for reliable detection technologies.Herein,a method was developed for simultaneous detection of atmospher...As more attention is being paid to the characteristics of atmospheric amines,there is also an increasing demand for reliable detection technologies.Herein,a method was developed for simultaneous detection of atmospheric amines in both gaseous and particulate phases using gas chromatography-mass spectrometry(GC-MS).The amine samples were collected with and without phosphoric acid filters,followed by derivatization with benzenesulfonyl chloride under alkaline condition prior to GC-MS analysis.Furthermore,the method was optimized and validated for determining 14 standard amines.The detection limits ranged from0.0408-0.421μg/mL(for gaseous samples)and 0.163-1.69μg/mL(for particulate samples),respectively.The obtained recoveries ranged from 68.8%-180%and the relative standard deviation was less than 30%,indicating high precision and good reliability of the method.Seven amines were simultaneously detected in gaseous and particulate samples in an industrial park using the developed method successfully.Methylamine,dimethylamine and diethylamine together accounted for 76.7%and 75.6%of particulate and gaseous samples,respectively.By comparing the measured and predicted values of gas-particle partition fractions,it was found that absorption process of aqueous phase played a more important role in the gas-partition of amines than physical adsorption.Moreover,the reaction between unprotonated amines and acid(aq.)in water phase likely promoted water absorption.Higher measured partition fraction of dibutylamine was likely due to the reaction with gaseous HCl.The developed method would help provide a deeper understanding of gas-particle partitioning as well as atmospheric evolution of amines.展开更多
文摘Photocatalytic degradation of gaseous pollutants on Bi-based semiconductors under solar lightirradiation has attracted significant attention.However,their application in gaseous straight-chainalkane purification is still rare.Here,a series of Bi/BiOBr composites were solvothermally synthe-sized and applied in solar-light-driven photocatalytic degradation of gaseous n-hexane.The charac-terization results revealed that both increasing number of functional groups of alcohol solvent(from methanol and ethylene glycol to glycerol)and solvothermal temperature(from 160 and 180to 200℃)facilitated the in-situ formation of metallic Bi nanospheres on BiOBr nanoplates withexposed(110)facets.Meanwhile,chemical bonding between Bi and BiOBr was observed on theseexposed facets that resulted in the formation of surface oxygen vacancy.Furthermore,the synergis-tic effect of optimum surface oxygen vacancy on exposed(110)facets led to a high visible light re-sponse,narrow band gap,great photocurrent,low recombination rate of the charge carriers,andstrong·O2-and h*formation,all of which resulted in the highest removal efficiency of 97.4%within120 min of 15 ppmv of n-hexane on Bi/BiOBr.Our findings efficiently broaden the application ofBi-based photocatalysis technology in the purification of gaseous straight-chain pollutants emittedby the petrochemical industry.
文摘Surface defect modulation has emerged as a potential strategy for promoting the photocatalytic activity of photocatalysts for various applications, while the impact of the oxygen vacancy on bacterial inactivation is still debated. In this study, oxygen vacancies were introduced to tungsten trioxide nanosheets(WO3–x) via a microwave-assisted route. The as-prepared WO3–x nanosheets exhibited excellent visible-light-driven photocatalytic activity toward E. coli K-12 inactivation, and 6 log orders of the bacterial cells could be completely inactivated within 150 min. The obtained bacterial inactivation rate constant was 15.2 times higher than that of pristine WO3 without oxygen vacancies, suggesting that the surface oxygen vacancy could significantly promote the bacterial inactivation efficiency. The mechanism study indicated that the inactivation of bacterial cells occurs via a direct h+ oxidation pathway. In addition, the role of the oxygen vacancy was studied in detail;the oxygen vacancy was found to not only promote interfacial charge separation but also tune the band structure of WO3, thereby leading to increased h+ oxidation power. Finally, a possible oxygen vacancy-dominated photocatalytic bacterial inactivation mechanism is proposed. This work is expected to offer new insights into the microwave-assisted synthesis of defective photocatalysts and the use of the oxygen vacancy for promoting photocatalytic antibacterial activities.
文摘Formaldehyde(HCHO) is a common indoor pollutant, long-term exposure to HCHO may harm human health. Its efficient removal at mild conditions is still challenging. The catalytic oxidation of HCHO molecules on a single atomic catalyst, Ti-decorated Ti3C2O2(Ti/Ti3C2O2) monolayer, is investigated by performing the first principles calculations in this work. It demonstrates that Ti atoms can be easily well dispersed at the form of single atom on Ti3C2O2 monolayer without aggregation. For HCHO catalytic oxidation, both Langmuir-Hinshelwood(LH) and Eley-Rideal(ER) mechanisms are considered. The results show that the step of HCHO dissociative adsorption on Ti/Ti3C2O2 with activated O2 can release high energy of 4.05 e V based on the ER mechanism, which can help to overcome the energy barrier(1.04 e V) of the subsequent reaction steps. The charge transfer from *OH group to CO molecule(dissociated from HCHO) not only promotes *OH group activation but also plays an important role in the H2 O generation along the ER mechanism. Therefore, HCHO can be oxidized easily on Ti/Ti3C2O2 monolayer, this work could provide significant guidance to develop effective non-noble metal catalysts for HCHO oxidation and broaden the applications of MXene-based materials.
基金supported by the National Key R&D Program of China(Nos.2019YFC1804502 and 2019YFC1804503)the Guangdong Provincial Natural Science Fund for Distinguished Young Scholars(No.2022B1515020051)+2 种基金the National Natural Science Foundation of China(No.42077332)the Science and Technology Program of Guangzhou(No.202201010149)the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(No.2017BT01Z032)。
文摘Industrial coking facilities are an important emission source for volatile organic compounds(VOCs).This study analyzed the atmospheric VOC characteristics within an industrial coking facility and its surrounding environment.Average concentrations of total VOCs(TVOCs)in the surrounding residential activity areas(R1 and R2),the coking facility(CF)and the control area(CA)were determined to be 138.5,47.8,550.0,and 15.0μg/m^(3),respectively.The cold drum process and coking and quenching areas within the coking facility were identified as the main polluting processes.The spatial variation in VOCs composition was analyzed,showing that VOCs in the coking facility and surrounding areas were mainly dominated by aromatic compounds such as BTX(benzene,toluene,and xylenes)and naphthalene,with concentrations being negatively correlated with the distance from the coking facility(p<0.01).The sources of VOCs in different functional areas across the monitoring area were analyzed,finding that coking emissions accounted for 73.5%,33.3% and 27.7% of TVOCs in CF,R1 and R2,respectively.These results demonstrated that coking emissions had a significant impact on VOC concentrations in the areas surrounding coking facility.This study evaluates the spatial variation in exposure to VOCs,providing important information for the influence of VOCs concentration posed by coking facility to surrounding residents and the development of strategies for VOC abatement.
基金the Collaborative Research Project of the National Natural Science Foundation of China(L2224041)the Chinese Academy of Sciences(XK2022DXC005)+2 种基金Frontier of Interdisciplinary Research on Monitoring and Prediction of Pathogenic Microorganisms in the AtmosphereSelf-supporting Program of Guangzhou Laboratory(SRPG22-007)Fundamental Research Funds for the Central Universities(lzujbky-2022-kb09).
文摘Corona virus disease 2019(COVID-19)has exerted a profound adverse impact on human health.Studies have demonstrated that aerosol transmission is one of the major transmission routes of severe acute respiratory syndrome coronavirus 2(SARS-CoV-2).Pathogenic microorganisms such as SARS-CoV-2 can survive in the air and cause widespread infection among people.Early monitoring of pathogenic microorganism transmission in the atmosphere and accurate epidemic prediction are the frontier guarantee for preventing large-scale epidemic outbreaks.Monitoring of pathogenic microorganisms in the air,especially in densely populated areas,may raise the possibility to detect viruses before people are widely infected and contain the epidemic at an earlier stage.The multi-scale coupled accurate epidemic prediction system can provide support for governments to analyze the epidemic situation,allocate health resources,and formulate epidemic response policies.This review first elaborates on the effects of the atmospheric environment on pathogenic microorganism transmission,which lays a theoretical foundation for the monitoring and prediction of epidemic development.Secondly,the monitoring technique development and the necessity of monitoring pathogenic microorganisms in the atmosphere are summarized and emphasized.Subsequently,this review introduces the major epidemic prediction methods and highlights the significance to realize a multi-scale coupled epidemic prediction system by strengthening the multidisciplinary cooperation of epidemiology,atmospheric sciences,environmental sciences,sociology,demography,etc.By summarizing the achievements and challenges in monitoring and prediction of pathogenic microorganism transmission in the atmosphere,this review proposes suggestions for epidemic response,namely,the establishment of an integrated monitoring and prediction platform for pathogenic microorganism transmission in the atmosphere.
基金funded by the National Key Research and Development Program of China(2020YFC1807000)the Strategic Priority Research Program of the Chinese Academy of Sciences(no.XDA28030501)+9 种基金the National Natural Science Foundation of China(41991333,41977137,42090060)the International Atomic Energy Agency Research Project(D15022)the Youth Innovation Promotion Association of Chinese Academy of Sciences(2011225[Fang Wang],Y201859[H.Wang],2013201[J.Su],2021309[Y.Song],Y2022084[M.Ye])Chinese Academy of Sciences President’s International Fellowship Initiative(2020DC0005,2022DC0001,2024DC0009)the Institute of Soil Science,Chinese Academy of Sciences(ISSAS2419)the Research Group Linkage project from Alexander von Humboldt foundation,the Center for Health Impacts of Agriculture(CHIA)of Michigan State University,and the URI STEEP Superfund Center(grant#P42ES027706)Fang Wang was partly supported by the fellowship of Alexander von Humboldt for experienced researchers,and Shennong Young Talents of the Ministry of Agriculture and Rural Affairs,China(SNYCQN006-2022)J.P.and T.R.S.were supported by the Canada Research Chair program.B.W.B.was supported by a Royal Society of New Zealand Catalyst International Leaders fellowship.K.K.B.was supported by Innovation Fund Denmark and the European Commission Horizon 2020 financed under the ERA-NET Aquatic Pollutants Joint Transnational Call(REWA,GA no.869178)S.A.H.was partly supported by a grant from the National Institute of Environmental Health Sciences,National Institutes of Health grant number P42ES04911-29(Project 4)T.R.S.thanks CESAM by FCT/MCTES(UIDP/50017/2020+UIDB/50017/2020+LA/P/0094/2020)。
文摘Environmental pollution is escalating due to rapid global development that often prioritizes human needs over planetary health.Despite global efforts to mitigate legacy pollutants,the continuous introduction of new substances remains a major threat to both people and the planet.In response,global initiatives are focusing on risk assessment and regulation of emerging contaminants,as demonstrated by the ongoing efforts to establish the UN’s Intergovernmental Science-Policy Panel on Chemicals,Waste,and Pollution Prevention.This review identifies the sources and impacts of emerging contaminants on planetary health,emphasizing the importance of adopting a One Health approach.Strategies for monitoring and addressing these pollutants are discussed,underscoring the need for robust and socially equitable environmental policies at both regional and international levels.Urgent actions are needed to transition toward sustainable pollution management practices to safeguard our planet for future generations.
基金supported by the Guangdong Basic and Applied Basic Research Foundation(No.2019B151502064)the National Natural Science Foundation of China(Nos.42077189,42020104001,and 42277081)+3 种基金the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(No.2017BT01Z032)the Science and Technology Key Project of Guangdong ProvinceChina(No.2019B110206002)the Guangdong Provincial Key R&D Program(No.2022-GDUT-A0007)。
文摘Acetylacetone(AcAc)is a typical class ofβ-diketones with broad industrial applications due to the property of the keto-enol isomers,but its isomerization and chemical reactions at the air-droplet interface are still unclear.Hence,using combined molecular dynamics and quantum chemistry methods,the heterogeneous chemistry of AcAc at the air-droplet interface was investigated,including the attraction of AcAc isomers by the droplets,the distribution of isomers at the air-droplet interface,and the hydration reactions of isomers at the air-droplet interface.The results reveal that the preferential orientation of two AcAc isomers(keto-and enol-AcAc)to accumulate and accommodate at the acidic air-droplet interface.The isomerization of two AcAc isomers at the acidic air-droplet interface is more favorable than that at the neutral air-droplet interface because the“water bridge”structure is destroyed by H_(3)O^(+),especially for the isomerization from keto-Ac Ac to enol-AcAc.At the acidic air-droplet interface,the carbonyl or hydroxyl O-atoms of two AcAc isomers display an energetical preference to hydration.Keto-diol is the dominant products to accumulate at the air-droplet interface,and excessive keto-diol can enter the droplet interior to engage in the oligomerization.The photooxidation reaction of AcAc will increase the acidity of the air-droplet interface,which indirectly facilitate the uptake and formation of more keto-diol.Our results provide an insight into the heterogeneous chemistry ofβ-diketones and their influence on the environment.
基金supported by the National Natural Science Foundation of China (Nos. 21607028, 41425015 and 41573086)the Research Grant Council of Hong Kong Special Administrative Region (SAR) Government (No. GRF14100115)+3 种基金Science and Technology Project of Guangdong Province, China (No. 2017A050506049)Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program (No. 2017BT01Z032)Innovation Team Project of Guangdong Provincial Department of Education (No. 2017KCXTD012)Leading Scientific, Technical and Innovation Talents of Guangdong Special Support Program (No. 2016TX03Z094)
文摘There is an urgent need for developing cost-effective methods for the treatment of perfluorooctanoic acid(PFOA)due to its global emergence and potential risks.In this study,taking surface-defective BiOCl as an example,a strategy of surface oxygen vacancy modulation was used to promote the photocatalytic defluorination efficiency of PFOA under simulated sunlight irradiation.The defective BiOCl was fabricated by a fast microwave solvothermal method,which was found to induce more surface oxygen vacancies than conventional solvothermal and precipitation methods.As a result,the asprepared BiOCl showed significantly enhanced defluorination efficiency,which was 2.7 and33.8 times higher than that of BiOCl fabricated by conventional solvothermal and precipitation methods,respectively.Mechanistic studies indicated that the defluorination of PFOA follows a direct hole(h^+)oxidation pathway with the aid of·OH,while the oxygen vacancies not only promote charge separation but also facilitate the intimate contact between the photocatalyst surface and PFOA by coordinating with its terminal carboxylate group in a bidentate or bridging mode.This work will provide a general strategy of oxygen vacancy modulation by microwave-assisted methods for efficient photocatalytic defluorination of PFOA in the environment using sunlight as the energy source.
基金the National Natural Science Foundation of China(Grant No.51478045)the Fund Project of Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control(GKECHRC-07)+1 种基金the Fund Project of Shaanxi Key Laboratory of Land Consolidation(2018-ZD04)the Opening Fund of State Key Laboratory of Green Building in Western China(LSKF202008).
文摘Recent pandemic outbreak of the corona-virus disease 2019(COVID-19)has raised widespread concerns about the importance of the bioaerosols.They are atmospheric aerosol particles of biological origins,mainly including bacteria,fungi,viruses,pollen,and cell debris.Bioaerosols can exert a substantial impact on ecosystems,climate change,air quality,and public health.Here,we review several relevant topics on bioaerosols,including sampling and detection techniques,characterization,effects on health and air quality,and control methods.However,very few studies have focused on the source apportionment and transport of bioaerosols.The knowledge of the sources and transport pathways of bioaerosols is essential for a comprehensive understanding of the role microorganisms play in the atmosphere and control the spread of epidemic diseases associated with them.Therefore,this review comprehensively summarizes the up to date progress on the source characteristics,source identification,and diffusion and transport process of bioaerosols.We intercompare three types of diffusion and transport models,with a special emphasis on a widely used mathematical model.This review also highlights the main factors affecting the source emission and transport process,such as biogeographic regions,land-use types,and environmental factors.Finally,this review outlines future perspectives on bioaerosols.
基金National Natural Science Foundation of China (Nos.21777033,21607029 and 41425015)Science and Technology Planning Project of Guangdong Province (No. 2017B020216003)the Innovation Team Project of Guangdong Provincial Department of Education (No.2017KCXTD012)。
文摘Formaldehyde(HCHO) is one kind of common indoor toxic pollutant,the catalytic oxidation degradation of formaldehyde at room temperature is desired.In this work,a new single atomic catalyst(SAC),Al doped graphene,for the catalytic oxidation of HCHO molecules was proposed through density function theory(DFT) calculations.It is found that Al atoms can be adsorbed on graphene stably without aggre s sion.Then HCHO can be effectively oxidized into CO2 and H2 O in the presence of O2 molecules on Al doped graphene with a low energy barrier of 0.82 eV and releasing energy of 2.29 eV with the pathway of HCHO→HCOOH→CO→CO2.The oxidation reaction can happen promptly with reaction time τ=56.9 s at the speed control step at room temperature.Therefore,this work proposed a high-performance catalyst Al-doped graphene without any noble metal for HCHO oxidation at ambient temperature,and corresponding oxidation pathway and mechanism are also deeply understood.
基金supported by the National Key R&D Program of China (No. 2019YFC0214402)the National Nature Science Foundation of China (Nos. 41805103, 42177354, and 21777032)+1 种基金the Natural Science Foundation of Guangdong Province (No. 2021A1515011492)the Science and Technology Program of Guangzhou (No. 202102020451)。
文摘Fugitive emission has been becoming an important source of volatile organic compounds(VOCs) in pharmaceutical industry,but the exact contribution of fugitive emission remains incompletely understood.In present study,pollution characteristics,odorous activity and health risk of stack and fugitive emissions of VOCs from four functional units (e.g.,workshop,sewage treatment station,raw material storage and hazardous waste storage) of three representative pharmaceutical factories were investigated.Workshop was the dominant contributor to VOCs of fugitive emission in comparison with other functional units.Extreme high concentration of VOCs from fugitive emission in unsealed workshop (94.87 mg/m^(3))was observed relative to sealed one (1.18 mg/m^(3)),accounting for 31%and 5%of total VOCs,respectively.Fugitive emission of VOCs in the unsealed workshop mainly consisted of nhexane,1-hexene and dichloromethane.Odorous activity indexes and non-cancer hazard ratios of these VOCs from fugitive emission in the unsealed workshop were as high as that from stack exhaust.Furthermore,cancer risk of dichloromethane from fugitive emission and stack exhaust was up to (1.6-1.8)×10^(-5).Odorous activity or health risk index of the VOCs from fugitive emission was up to 13 or 11 times of the corresponding threshold value,posing remarkable health threat on pharmaceutical workers.Our?ndings highlighted the possibly underestimated contribution of fugitive emission on VOCs in the pharmaceutical industry.
基金supported by the National Natural Science Foundation of China(Nos.21777033 and 22006023)Natural Science Foundation of Guangdong Province(No.2019A1515010428)+1 种基金Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(No.2017BT01Z032)the Innovation Team Project of Guangdong Provincial Department of Education(No.2017KCXTD012)。
文摘Explore the photo-piezoelectric synergistic micro-mechanism by density functional theory(DFT)calculations at the electronic and atomic level is important.In this work,to understand the synergistic mechanism,atomic and electronic properties of typical piezoelectric and photocatalytic material BaTiO_(3)were initially investigated with different strains.Subsequently,the adsorption of volatile organic compounds(VOCs)on the BaTiO_(3)(001)surface was determined during the piezoelectric process.In addition,the relationship between deformation ratio,the electronic structure and adsorption energy was understood in the deformation ratio range of 7%-12%for the optimal catalytic effect.The results of charge density differences and Born effective charge reveal the synergistic mechanism of piezoelectric photocatalysis.The built-in electric field formed by polarization results in the enhanced separation of charges,which makes the surface charges aggregation,enhancing the adsorption of VOCs,and benefiting the subsequent photocatalytic degradation.This work can provide significant theoretical guidance for the piezoelectric photocatalytic degradation of pollutants with the optimal strain range.
基金This work was supported by the National Key Research and Development Project of China(2019YFC1804500).
文摘Rapid economic development and industrialization have left many risk sites around the world with significant or potential soil contamination due to industrial production or the shutdown or relocation of industrial facilities.Soil pollutants pose significant threats to human health,especially at sites used by the chemical,mining,and metalworking industries,among others[1].
基金funding provided by the Hundred Talent Program of Guangdong University of Technology,China(No.220418134)the National Natural Science Foundation of China(No.41807349)the Australian Research Council through Linkage Project(No.LP100100852)
文摘The application of nanoscale zero-valent iron(nZVI) for the degradation of contaminants has been extensively investigated, however, few studies have focused on degradation in high salinity environments. In this study, the ability of bare and carboxymethyl cellulose(CMC)-coated bimetallic Pd-nZVI particles to degrade 33′44′-tetrachlorobiphenyl in high saline water(SW) is examined with particular attention given to the effects of ethylenediaminetetraacetic acid(EDTA) on the rate of degradation. EDTA enhances the reactivity of Pd-nZVI in SW, with evidence provided to link this to the removal of the passivating layer. Additionally, a conceptual model is proposed which provides a quantitative description of the removal of these iron oxide layers in the presence of EDTA. An optimum EDTA to bare Pd-nZVI molar ratio of 0.1 exists, with insufficient EDTA unable to remove the passivating layer whilst excess EDTA results in Fe loss and enhanced agglomeration due to magnetic attraction of the bare Fe(0) particles. In contrast, CMCcoating of Pd-nZVI assemblages actually impedes degradation, despite the coated particles displaying a smaller average size compared to uncoated particles, with even the presence of EDTA in this case not significantly improving degradation. The reduced reactivity in the presence of CMC is primarily attributed to the effect of CMC on the association of Pd with nZVI particles. In particular, the presence of CMC reduced the total amount of Pd incorporated with the stabilized particles compared to the non-stabilized particles.Additionally, the presence of CMC results in less Pd present in its reactive zero-valent oxidation state.
基金supported by the Local Innovative and Research Team Project of Guangdong Pearl River Talents Program (No. 2017BT01Z032)the National Natural Science Foundation of China (Nos. 41731279 and 41425015 )+2 种基金the Key-Area Research and Development Program of Guangdong Province (No. 2019B110206002)The Innovation Team Project of Guangdong Provincial Department of Education (No. 2017KCXTD012)Guangdong Special Branch Plan of Science and Technology for Innovation leading scientists (2016TX03Z094)。
文摘Increasing attention has been paid to the air pollution more recently. Smog chamber has been proved as a necessary and effective tool to study atmospheric processes, including photochemical smog and haze formation. A novel smog chamber was designed to study the atmospheric photochemical reaction mechanism of typical volatile organic compounds(VOCs) as well as the aging of aerosols. The smog chamber system includes an enclosure equipped with black lights as the light source, two parallel reactors(2 m^3 of each) with separate control of light source and temperature, with a series of coupled instruments for online monitoring of gas phase and particle phase reactants and products. Chamber characterization, including air source stability, effective light intensity, temperature stability, as well as gas phase and particle phase wall losses, were carried out before further research. The results showed that our smog chamber systems developed by other domestic and international groups. It was also observed that the wall loss of aromatic VOCs varied with different functional groups as well as the isomerism. The results of preliminary simulation experiment from styrene-NO_x demonstrated that the chamber can be well utilized to simulate gas-particle conversion progresses in the atmosphere.
基金This work was supported by the National Key Research and Development Program of China(2019YFC1804503 and 2019YFC1804501)the Key-Area Research and Development Program of Guangdong Province(2020B1111350002)+2 种基金the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(2017BT01Z032)the National Natural Science Foundation of China(41977365 and 41425015)the Key Project of Guangdong-Guangxi Joint Fund(2020B1515420002).
文摘Personal care products(PCPs)inevitably come into contact with the skin in people’s daily life,potentially causing adverse effects on human health.The adverse effects can be exacerbated under UV irradiation but are rarely studied.In this study,to clearly understand the damage of representative PCPs to human skin and their photochemical transformation behaviors,fragrance tonalide(AHTN)was measured in the presence of amino acids as a basic building block of human tissue.The results showed that amino acids could decelerate the photochemical transformation rate of AHTN,increasing the likelihood of AHNT persisting on the skin surface and the health risk to the human being.Further,the interaction between amino acids and AHTN was investigated.AHTN could play bidirectional roles in damaging amino acids:the photosensitizer and reactive activator.As a photosensitizer,the ^(1)O_(2) generated from the AHTN photosensitization was partly employed to oxidative damage amino acids.Furthermore,by combining experiments with quantum chemical computation,the carbonyl group of the activator AHTN was found to be the active site to activate the N-containing group of amino acids.The activation mechanism was the electron transfer between AHTN and amino acids.Imines formed during the photochemical transformation of AHTN with histidine/glycine were the molecular initiating event for potential skin sensitization.This study reported for the first time that skin photosensitizer formation threatens human health during the photochemical transformation of AHTN.
基金This work was supported by the National Natural Science Foundation of China(Nos.U1901210,41877363,42130611,and 42177410)the Science and Technology Project of Guangdong Province,China(No.2021A0505030070)+2 种基金the Natural Science Foundation of Guangdong Province(No.2019A1515010599)the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(No.2017BT01Z032)the Young S&T Talent Training Program of Guangdong Provincial Association,China(No.2022QNRC23).
文摘Pathogenic microbes with antibiotic resistance can thrive on municipal solid waste as nutrients and be aerosolized and transported to vicinities during waste disposal processes.However,the characterization of pathogenic bioaerosols and assessment of their exposure risks are lacking.Herein,particle size,concentration,activity,antibiotic resistance,and pathogenicity of airborne microorganisms were assessed in different sectors of a typical landfill.Results showed that active sector in downwind direction has the highest bioaerosol level(1234 CFU/m3),while residential area has the highest activity(14.82 mg/L).Botanical deodorizer from mist cannon can effectively remove bioaerosol.Most bioaerosols can be inhaled into respiratory system till bronchi with sizes ranging from 2.1−3.3 and 3.3−4.7μm.Pathogenic bacteria(Bacilli,Bacillus,and Burkholderia-Paraburkholderia)and allergenic fungi(Aspergillus,Cladosporium,and Curvularia)prevailed in landfill.Although high abundance of microbial volatile organic compounds(mVOCs)producing bioaerosols were detected,these mVOCs contributed little to odor issues in landfill.Notably,surrounding areas have higher levels of antibiotic-resistance genes(ARGs)than inner landfill with tetC,acrB,acrF,mdtF,and bacA as dominant ones.Most ARGs were significantly correlated with bacterial community,while environmental parameters mainly influenced fungal prevalence.These findings can assist in reducing and preventing respiratory allergy or infection risks in occupational environments relating to waste management.
基金supported by the National Natural Science Foundation of China(Nos.22106020 and 42122056)the KeyArea Research and Development Program of Guangdong Province(No.2020B1111350002)+1 种基金the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(No.2017BT01Z032)the Guangdong Basic and Applied Basic Research Foundation(No.2020A1515110718).
文摘Rational design and synthesis of highly efficient and robust photocatalysts with positive exciton splitting and interfacial charge transfer for environmental applications is critical.Herein,aiming at overcoming the common shortcomings of traditional photocatalysts such as weak photoresponsivity,rapid combination of photo-generated carriers and unstable structure,a novel Ag-bridged dual Z-scheme g-C_(3)N_(4)/BiOI/AgI plasmonic heterojunction was successfully synthesized using a facile method.Results showed that Ag-AgI nanoparticles and three-dimensional(3D)BiOI microspheres were decorated highly uniformly on the 3D porous g-C_(3)N_(4) nanosheet,resulting in a higher specific surface area and abundant active sites.The optimized 3D porous dual Z-scheme g-C_(3)N_(4)/BiOI/Ag-AgI manifested exceptional photocatalytic degradation efficiency of tetracycline(TC)in water with approximately 91.8%degradation efficiency within 165 min,outperforming majority of the reported g-C_(3)N_(4)-based photocatalysts.Moreover,g-C_(3)N_(4)/BiOI/Ag-AgI exhibited good stability in terms of activity and structure.In-depth radical scavenging and electron paramagnetic resonance(EPR)analyses confirmed the relative contributions of various scavengers.Mechanism analysis indicated that the improved photocatalytic performance and stability were ascribed to the highly ordered 3D porous framework,fast electron transfer of dual Z-scheme heterojunction,desirable photocatalytic performance of BiOI/AgI and synergistic effect of Ag plasmas.Therefore,the 3D porous Z-scheme g-C_(3)N_(4)/BiOI/Ag-AgI heterojunction had a good prospect for applications in water remediation.The current work provides new insight and useful guidance for designing novel structural photocatalysts for environment-related applications.
基金financially supported by the Natural Science Foundation of Guangdong Province,China (No.2019B151502064)the National Natural Science Foundation of China (Nos.42077189 and 4201001008)+2 种基金the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program (No.2017BT01Z032)the Innovation Team Project of Guangdong Provincial Department of Education(No.2017KCXTD012)the Science and Technology Key Project of Guangdong Province,China (No.2019B110206002)。
文摘Organosulfate (OSA) nanoparticles,as secondary organic aerosol (SOA) compositions,are ubiquitous in urban and rural environments.Hence,we systemically investigated the mechanisms and kinetics of aqueous-phase reactions of 1-butanol/1-decanol (BOL/DOL) and their roles in the formation of OSA nanoparticles by using quantum chemical and kinetic calculations.The mechanism results show that the aqueous-phase reactions of BOL/DOL start from initial protonation at alcoholic OH^(-)groups to form carbenium ions (CBs),which engage in the subsequent esterification or oligomerization reactions to form OSAs/organosulfites (OSIs) or dimers.The kinetic results reveal that dehydration to form CBs for BOL and DOL reaction systems is the rate-limiting step.Subsequently,about 18%of CBs occur via oligomerization to dimers,which are difficult to further oligomerize because all reactive sites are occupied.The rate constant of BOL reaction system is one order of magnitude larger than that of DOL reaction system,implying that relative short-chain alcohols are more prone to contribute OSAs/OSIs than long-chain alcohols.Our results reveal that typical long-chain alcohols contribute SOA formation via esterification rather than oligomerization because OSA/OSI produced by esterification engages in nanoparticle growth through enhancing hygroscopicity.
基金supported from the National Natural Science Foundation of China(Nos.42020104001 and 41805103)Local Innovative and Research Team Project of Guangdong Pearl River Talents Program(No.2017BT01Z032)the Fund from Chemistry and Chemical Engineering Guangdong Laboratory(No.1922009)
文摘As more attention is being paid to the characteristics of atmospheric amines,there is also an increasing demand for reliable detection technologies.Herein,a method was developed for simultaneous detection of atmospheric amines in both gaseous and particulate phases using gas chromatography-mass spectrometry(GC-MS).The amine samples were collected with and without phosphoric acid filters,followed by derivatization with benzenesulfonyl chloride under alkaline condition prior to GC-MS analysis.Furthermore,the method was optimized and validated for determining 14 standard amines.The detection limits ranged from0.0408-0.421μg/mL(for gaseous samples)and 0.163-1.69μg/mL(for particulate samples),respectively.The obtained recoveries ranged from 68.8%-180%and the relative standard deviation was less than 30%,indicating high precision and good reliability of the method.Seven amines were simultaneously detected in gaseous and particulate samples in an industrial park using the developed method successfully.Methylamine,dimethylamine and diethylamine together accounted for 76.7%and 75.6%of particulate and gaseous samples,respectively.By comparing the measured and predicted values of gas-particle partition fractions,it was found that absorption process of aqueous phase played a more important role in the gas-partition of amines than physical adsorption.Moreover,the reaction between unprotonated amines and acid(aq.)in water phase likely promoted water absorption.Higher measured partition fraction of dibutylamine was likely due to the reaction with gaseous HCl.The developed method would help provide a deeper understanding of gas-particle partitioning as well as atmospheric evolution of amines.