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1.
    
The region along the Taihang Mountains in the North China Plain (NCP) is characterized by serious fine particle pollution. To clarify the formation mechanism and controlling factors, an observational study was conducted to investigate the physical and chemical properties of the fine particulate matter in Jiaozuo city, China. Mass concentrations of the water-soluble ions (WSIs) in PM2.5 and gaseous pollutant precursors were measured on an hourly basis from December 1, 2017, to February 27, 2018. The positive matrix factorization (PMF) method and the FLEXible PARTicle (FLEXPART) model were employed to identify the sources of PM2.5. The results showed that the average mass concentration of PM2.5 was 111 μg/m3 during the observation period. Among the major WSIs, sulfate, nitrate, and ammonium (SNA) constituted 62% of the total PM2.5 mass, and NO3? ranked the highest with an average contribution of 24.6%. NH4+ was abundant in most cases in Jiaozuo. According to chemical balance analysis, SO42?, NO3?, and Cl? might be present in the form of (NH4)2SO4, NH4NO3, NH4Cl, and KCl. The liquid-phase oxidation of SO2 and NO2 was severe during the haze period. The relative humidity and pH were the key factors influencing SO42- formation. We found that NO3? mainly stemmed from homogeneous gas-phase reactions in the daytime and originated from the hydrolysis of N2O5 in the nighttime, which was inconsistent with previous studies. The PMF model identified five sources of PM2.5: secondary origin (37.8%), vehicular emissions (34.7%), biomass burning (11.5%), coal combustion (9.4%), and crustal dust (6.6%).  相似文献   

2.
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Monolayer-ordered gold nanoring arrays were prepared by ion-sputtering method and used as surface enhanced Raman spectroscopy (SERS) substrates to test the individual atmospheric aerosols particle. Compared to other methods used for testing atmospheric aerosols particles, the collection and subsequent detection in our work is performed directly on the gold nanoring SERS substrate without any treatment of the analyte. The SERS performance can be tuned by changing the depth of the gold nanoring cavity as originating from coupling of dipolar modes at the inner and outer surfaces of the nanorings. The electric field exhibits uniform enhancement and polarization in the ordered Au nanoring substrate, which can improve the accuracy for detecting atmospheric aerosol particles. Combined with Raman mapping, the information about chemical composition of individual atmospheric aerosols particle and distribution of specific components can be presented visually. The results show the potential of SERS in enabling improved analysis of aerosol particle chemical composition, mixing state, and other related physicochemical properties.  相似文献   

3.
    
The coastal eco-city of Fuzhou in Southeastern China has experienced severe ozone (O3)episodes at times in recent years.In this study,three typical synoptic circulations types (CTs)that influenced more than 80%of O3polluted days in Fuzhou during 2014-2019 were identified using a subjective approach.The characteristics of meteorological conditions linked to photochemical formation and transport of O3under the three CTs were summarized.Comprehensive Air Quality Mod...  相似文献   

4.
    
Currently, the three-dimensional (3D) distribution and characteristics of air pollution cannot be understood based on the application of any single atmospheric monitoring technology. Long-term, high-precision and large-scale 3D atmospheric monitoring might become practical by combining heterogeneous modern technologies; for this purpose, the SpaceAir-Ground integrated system is a promising concept. In this system, optical remote sensing technologies employing fixed or mobile platforms are used a...  相似文献   

5.
    
China’s energy dependents on coal due to the abundance and low cost of coal.Coal provides a secure and stable energy source in China.Over-dependence on coal results in the emission of Hazardous Trace Elements (HTEs) including selenium (Se),mercury (Hg),lead(Pb),arsenic (As),etc.,from Coal-Fired Power Plants (CFPPs),which are the major toxic air pollutants causing widespread concern.For this reason,it is essential to provide a succinct analysis of the main HTEs emission control techniques while c...  相似文献   

6.
    
This study aimed to explore the adsorption performance of sludge-based activated carbon (SBC) towards dissolved organic matters (DOMs) removal from sewage, and investigated the modification effect of different types of chemicals on the structure of synthesized SBC. Waste activated sludge (WAS) was used as a carbon source, and HCl, HNO3, and NaOH were used as different types of chemicals to modify the SBC. With the aid of chemical activation, the modified SBC showed higher adsorption performances on DOMs removal with maximum adsorption of 29.05 mg/g and second-order constant (k) of 0.1367 (L/mol/sec) due to the surface elution of ash and minerals by chemicals. The surface elemental composition of MSBC suggested that the content of C-C and C-O functional groups on the surface of modified sludge-based activated carbon (MSBC) played an important role on the adsorption capacities of MSBC towards DOMs removal in sewage. Additionally, the residual molecular weight of DOMs in sewage was investigated using a 3-dimension fluorescence excitation-emission matrix (3D-EEM) and high-performance size exclusion chromatography (HP-SEC). Results showed that the chemical modification significantly improved the adsorption capacity of MSBC on humic acids (HA) and aromatic proteins (APN), and both of NaOH-MSBC and HCl-MSBC were effective for a wide range of different AMW DOMs removal from sewage, while the HNO3-MSBC exhibited poorly on AMW organics of 2,617 Da and 409 Da due to the reducing content of macropore. In brief, this study provides reference values for the impact of the chemicals of the activation stage before the SBCs application.  相似文献   

7.
    
A new state-of-the-art indoor smog chamber facility(CAPS-ZJU) has been constructed and characterized at Zhejiang University,which is designed for chemical mechanism evaluation under well-controlled conditions.A series of characterization experiments were performed to validate the well-established experimental protocols,including temperature variation pattern,light spectrum and equivalent intensity(JNO2),injection and mixing performance,as well as gases and particle wall loss.In additi...  相似文献   

8.
    
BiFeO3 (BFO), as a kind of narrow band-gap semiconductor material, has gradually emerged advantages in the application of photocatalysis. In this paper, Ca doped BFO nanoparticles Bi0.9Ca0.1FeO3 (BCFO) were prepared by sol-gel method. And BCFO and CdS nanocomposites with two morphologies were obtained by controlling the time of loading CdS under a low temperature liquid phase process. It is found that the band gap becomes narrower after doping Ca into BFO, which is conducive to the absorption of visible light. Among all the samples, the composite of CdS nanowires and BCFO nanoparticles obtained by reaction time of 10 min has the best photocatalytic performance. The degradation rate of Methyl Orange solution was 94% after 90 min under visible light irradiation, which was much higher than that of pure BCFO and CdS. Furthermore, significant enhancement in the degradation rate (100% degradation in 60 min) can be achieved in poled samples after electric polarization process. The highest degradation rate is due to the promoted separation of photogenerated carriers induced by the internal polarization field and the formation of S-scheme heterostructure between BCFO and CdS. Such BCFO-CdS nanocomposites may bring new insights into designing highly efficient photocatalyst.  相似文献   

9.
    
Criegee intermediates (CIs), also known as carbonyl oxide, are reactive intermediates that play an important role in the atmospheric chemistry. Investigation on the structures and reactivity of CIs is of fundamental importance in understanding the underlying mechanism of their atmospheric reactions. In sharp contrast to the intensively studied parent molecule (CH2OO) and the alkyl-substituted derivatives, the knowledge about the fluorinated analogue CF3C(H)OO is scarce. By carefully heating the triplet carbene CF3CH in an O2-doped Ar-matrix to 35 K, the elusive carbonyl oxide CF3C(H)OO in syn- and anti-conformations has been generated and characterized with infrared (IR) and ultraviolet-visible (UV-vis) spectroscopy. The spectroscopic identification is supported by 18O-labeling experiments and quantum chemical calculations at the B3LYP/6-311++G(3df,3pd) and MP2/6-311++G(2d,2p) levels. Upon the long-wavelength irradiation (λ > 680 nm), both conformers of CF3C(H)OO decompose to give trifluoroacetaldehyde CF3C(H)O and simultaneously rearrange to the isomeric dioxirane, cyclic-CF3CH(OO), which undergoes isomerization to the lowest-energy carboxylic acid CF3C(O)OH upon UV-light excitation at 365 nm. The O2-oxidation of CF3CH via the intermediacy of CF3C(H)OO and cyclic-CF3CH(OO) might provide new insight into the mechanism for the degradation of hydro-chlorofluorocarbon CF3CHCl2 (HCFC-123) in the atmosphere.  相似文献   

10.
    
The source apportionment of PM2.5 is essential for pollution prevention.In view of the weaknesses of individual models,we proposed an integrated chemical mass balancesource emission inventory(CMB-SEI) model to acquire more accurate results.First,the SEI of secondary component precursors(SO2,NOx,NH3,and VOCs) was compiled to acquire the emission ratios of these sources for the precursors.Then,a regular CMB simulation was executed to obtain the contribut...  相似文献   

11.
    
Given the high abundance of water in the atmosphere,the reaction of Criegee intermediates (CIs) with (H2O)2is considered to be the predominant removal pathway for CIs.However,recent experimental findings reported that the reactions of CIs with organic acids and carbonyls are faster than expected.At the same time,the interface behavior between CIs and carbonyls has not been reported so far.Here,the gas-phase and air-water interface behavior between Criegee intermediates and ...  相似文献   

12.
    
The chemical composition of acid rain and its impact on lake water chemistry in Chongqing,China,from 2000 to 2020 were studied in this study.The regional acid rain intensity is affected jointly by the acid gas emissions and the neutralization of alkaline substances.The pH of precipitation experienced three stages of fluctuating decline,continuous improvement,and a slight correction.Precipitation pH showed inflection points in 2010,mainly due to the total control actions of SO2and NO  相似文献   

13.
    
A novel La-Co-O-C (LC-C) composites were prepared via a facile co-hydrothermal route with oxides and glycerol and further optimized for methane catalytic activity and thermal stability via component regulation. It was demonstrated that Co3O4 phase was the main component in regulation. The combined results of X-ray photoelectron spectroscopy (XPS), temperature-programmed desorption of oxygen (O2-TPD), temperature-programmed reduction of hydrogen (H2-TPR), temperature-programmed desorption of ammonia/carbon dioxide (NH3/CO2-TPD) revealed that component regulation led to more oxygen vacancies and exposure of surface Co2+, lower surface basicity and optimized acidity, which were beneficial for adsorption of active oxygen species and activation of methane molecules, resulting in the excellent catalytic oxidation performance. Especially, the (3.5)LC-C (3.5 is Co-to-La molar ratio) showed the optimum activity and the T50 and T90 (the temperature at which the CH4 conversion rate was 50% and 90%, respectively) were 318 and 367°C, respectively. Using theoretical calculations and in situ diffuse reflection infrared Fourier transform spectroscopy characterization, it was also found that the catalytic mechanism changes from the “Rideal-Eley” mechanism to the “Two-term” mechanism depending on the temperature windows in which the reaction takes place. Besides, the use of the “Flynn-Wall-Ozawa” model in thermoanalytical kinetics revealed that component regulation simultaneously optimized the decomposition activation energy, further expanding the application scope of carbon-containing composites.  相似文献   

14.
    
In order to enhance the removal performance of graphitic carbon nitride (g-C3N4) on organic pollutant, a simultaneous process of adsorption and photocatalysis was achieved via the compounding of biochar and g-C3N4. In this study, g-C3N4 was obtained by a condensation reaction of melamine at 550°C. Then the g-C3N4/biochar composites were synthesized by ball milling biochar and g-C3N4 together, which was considered as a simple, economical, and green strategy. The characterization of resulting g-C3N4/biochar suggested that biochar and g-C3N4 achieved effective linkage. The adsorption and photocatalytic performance of the composites were evaluated with enrofloxacin (EFA) as a model pollutant. The result showed that all the g-C3N4/biochar composites displayed higher adsorption and photocatalytic performance to EFA than that of pure g-C3N4. The 50% g-C3N4/biochar performed best and removed 45.2% and 81.1% of EFA (10 mg/L) under darkness and light with a dosage of 1 mg/mL, while g-C3N4 were 19.0% and 27.3%, respectively. Besides, 50% g-C3N4/biochar showed the highest total organic carbon (TOC) removal efficiency (65.9%). Radical trapping experiments suggested that superoxide radical (?O2?) and hole (h+) were the main active species in the photocatalytic process. After 4 cycles, the composite still exhibited activity for catalytic removal of EFA.  相似文献   

15.
    
The removal of ammonia (NH3) emitted from agricultural and industrial activities is of great significance to protect human health and ecological environment. Photocatalytic NH3 oxidation to N2 under mild conditions is a promising strategy. However, developing visible light photocatalysts for NH3 oxidation is still in its infancy. Here, we fabricate N-TiO2 and Ag/AgCl/N-TiO2 photocatalysts by sol-gel and photodeposition methods, respectively. The introduction of N not only endows TiO2 with visible light response (absorption edge at 460 nm) but also results in the formation of heterophase junction (anatase and rutile). Thus, N-TiO2 shows 2.0 and 1.8 times higher than those over anatase TiO2 and commercial TiO2 for NH3 oxidation under full spectrum irradiation. Meanwhile, surface modification of Ag can simultaneously enhance visible light absorption (generating localized surface plasmon resonance effect) and charge separation efficiency. Therefore, the photocatalytic activity of Ag/AgCl/N-TiO2 is further improved. Furthermore, the presence of N and Ag also enhances the selectivity of N2 product owing to the change of reaction pathway. This work simultaneously regulates photocatalytic conversion efficiency and product selectivity, providing some guidance for developing highly efficient photocatalysts for NH3 elimination.  相似文献   

16.
    
To investigate the enhancing effect of Mn on the performance of simultaneous catalytic oxidation of AsH3 and PH3 by CuO-Al2O3 in a reducing atmosphere under micro-oxygen conditions, Cu-Mn modified γ-Al2O3 catalysts were prepared. The characteristics of the catalysts showed that Mn reduced the crystallinity of the active CuO component, increased the number of oxygen vacancies and acidic sites on the catalyst surface, enhanced the mobility of surface oxygen, and the interaction between copper and manganese promoted the redox cycling ability of the catalysts and improved their oxidation performance, which increased the conversion frequency (TOF) by 2.54 × 10−2 to 3.07 × 10−2 sec−1. On the other hand, the introduction of Mn reduced the production of phosphate and As2O3 on the catalyst surface by 30.96% and 44.9%, which reduced the coverage and inerting of the active sites by phosphate and As2O3, resulting in an 8 hr (6 hr) improvement in the stability of PH3 (AsH3) removal.  相似文献   

17.
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The health effects of trace metal elements in atmospheric fine particulate matter (PM2.5) are widely recognized, however, the emission factor profiles and chemical fractionation of metal elements in different sources were poorly understand. In this study, sixteen metal elements, including Cd, Pb, V, Zn, Ba, Sb, As, Fe, Sr, Cr, Rb, Co, Mn, Cu, Ni and Sn from biomass burning, bituminite and anthracite combustion, as well as dust, were quantified. The results show different emission sources were associated with distinct emission profiles, holding important implications for source apportionment of ambient particulate metals. Specifically, Fe was the dominant metal species (28-1922 mg/kg) for all samples, and was followed by different metals for different samples. For dust, Mn (39.9 mg/kgdust) had the second-highest emission factor, while for biomass burning, it was Cr and Ba (7.5 and 7.4 mg/kgbiomass, respectively). For bituminous coal combustion, the emission factor of Zn and Ba was 6.2 and 6.0 mg/kgbituminous, respectively, while for anthracite combustion the corresponding emission factor was 5.6 and 4.3 mg/kganthracite, respectively. Moreover, chemical fractionation (i.e., the exchangeable, reducible fraction, oxidizable, and residual fraction) and the bioavailability index (BI) values of the metal elements from different sources were further investigated to reveal the link between different emission sources and the potential health risk. The findings from this study hold important implications for source apportionment and source-specific particulate metal-associated health effects.  相似文献   

18.
    
Ultra-low emission (ULE) technology retrofits significantly impact the particulate-bound mercury (Hg) emissions from coal-fired power plants (CFPPs); however, the distribution and bioavailability of Hg in size-fractioned particulate matter (PM) around the ULE-retrofitted CFPPs are less understood. Here, total Hg and its chemical speciation in TSP (total suspended particles), PM10 (aerodynamic particle diameter ≤ 10 µm) and PM2.5 (aerodynamic particle diameter ≤ 2.5 µm) around a ULE-retrofitted CFPP in Guizhou Province were quantified. Atmospheric PM2.5 concentration was higher around this ULE-retrofitted CFPP than that in the intra-regional urban cities, and it had higher mass Hg concentration than other size-fractioned PM. Total Hg concentrations in PM had multifarious sources including CFPP, vehicle exhaust and biomass combustion, while they were significantly higher in autumn and winter than those in other seasons (P < 0.05). Regardless of particulate size, atmospheric PM-bound Hg had lower residual fractions (< 21%) while higher HCl-soluble fractions (> 40%). Mass concentrations of exchangeable, HCl-soluble, elemental, and residual Hg in PM2.5 were higher than those in other size-fractioned PM, and were markedly elevated in autumn and winter (P < 0.05). In PM2.5, HCl-soluble Hg presented a significantly positive relationship with elemental Hg (P < 0.05), while residual Hg showed the significantly positive relationships with HCl-soluble Hg and elemental Hg (P < 0.01). Overall, these results suggested that atmospheric PM-bound Hg around the ULE-retrofitted CFPP tends to accumulate in finer PM, and has higher bioavailable fractions, while has potential transformation between chemical speciation.  相似文献   

19.
    
With the rapid expansion of livestock production, the amount of livestock wastewater accumulated rapidly. Lack of biodegradable organic matter makes denitrification of livestock wastewater after anaerobic digestion more difficult. In this study, Myriophyllum aquaticum constructed wetlands(CWs) with efficient nitrogen removal performance were established under different carbon/nitrogen(C/N) ratios. Analysis of community composition reveals the change of M. aquaticum CWs in microbial community str...  相似文献   

20.
    
The tetC gene has been found to be one of the most widely distributed tetracycline resistance (tet) genes in various environmental niches, but the detailed dissemination mechanisms are still largely unknown. In the present study, 11 tetC-containing Aeromonas media strains were isolated from an aerobic biofilm reactor under oxytetracycline stresses, and the genome of one strain was sequenced using the PacBio RSII sequencing approach to reveal the genetic environment of tetC. The tetC gene was carried by an IS26 composite transposon, named Tn6434. The tetC-carrying Tn6434 structure was detected in all of the A. media strains either in a novel plasmid pAeme2 (n=9) or other DNA molecules (n=2) by PCR screening. The NCBI database searching result shows that this structure was also present in the plasmids or chromosomes of other 13 genera, indicating the transferability of Tn6434. Inverse PCR and sequencing confirmed that Tn6434 can form a circular intermediate and is able to incorporate into a preexisting IS26 element, suggesting that Tn6434 might be responsible for the dissemination of tetC between different DNA molecules. This study will be helpful in uncovering the spread mechanism of tet genes in water environments.  相似文献   

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