Particulate matter with diameters of 2.5 μm or smaller(PM_(2.5)) and ozone(O_3) are major pollutants in the urban atmosphere. PM_(2.5) can affect O_3 by altering the photolysis rate and heterogeneous reactions. Howev...Particulate matter with diameters of 2.5 μm or smaller(PM_(2.5)) and ozone(O_3) are major pollutants in the urban atmosphere. PM_(2.5) can affect O_3 by altering the photolysis rate and heterogeneous reactions. However, these two processes and their relative importance remain uncertain. In this paper, with Nanjing in China as the target city, we investigate the characteristics and mechanism of interactions between particles and O_3 based on ground observations and numerical modeling.In 2008, the average concentrations of PM_(2.5) and O_3 at Caochangmen station are 64.6 ± 47.4 μg m^(-3) and 24.6 ± 22.8 ppb,respectively, while at Pukou station they are 94.1 ± 63.4 μg m^(-3) and 16.9 ± 14.9 ppb. The correlation coefficient between PM_(2.5) and O_3 is -0.46. In order to understand the reaction between PM_(2.5) and O_3, we construct a box model, in which an aerosol optical property model, ultraviolet radiation model, gas phase chemistry model, and heterogeneous chemistry model,are coupled. The model is employed to investigate the relative contribution of the aforementioned two processes, which vary under different particle concentrations, scattering capability and VOCs/NOxratios(VOCs: volatile organic compounds;NOx: nitric oxide and nitrogen dioxide). Generally, photolysis rate effect can cause a greater O_3 reduction when the particle concentrations are higher, while heterogeneous reactions dominate O_3 reduction with low-level particle concentrations.Moreover, in typical VOC-sensitive regions, O_3 can even be increased by heterogeneous reactions. In Nanjing, both processes lead to O_3 reduction, and photolysis rate effect is dominant. Our study underscores the importance of photolysis rate effect and heterogeneous reactions for O_3, and such interaction processes should be fully considered in future atmospheric chemistry modeling.展开更多
Aerosol samples were collected in summer in Macao, a coastal city of the Pearl River Delta Region in China. Morphology, size, elemental composition, and mixing state of individual aerosol particles were determined by ...Aerosol samples were collected in summer in Macao, a coastal city of the Pearl River Delta Region in China. Morphology, size, elemental composition, and mixing state of individual aerosol particles were determined by scanning electron microscopy coupled energy dispersive X-ray （SEM/EDX） and transmission electron microscopy （TEM）. Based on the morphologies of 5711 aerosol particles, they consist of soot （32%）, mineral （17%）, secondary-（22%）, and unknown fine particles （29%）. The sizes of these particles were mostly distributed between 0.1 and 0.4 μm. Compositions of 202 mineral particles were obtained by SEM/EDX. Mineral particles were mainly classified into three types： Si-rich, Ca-rich, and Na-rich. The compositions of typical mineral particles can indicate their sources in sampling location. For example, mineral particles, collected along the main street, were associated with trace amounts of heavy metals, such as Zn, Ti, Mn, Ba, Pb, and As. TEM observations indicate that most Na-rich particles were aged sea salt particles （e.g., Na2SO4 and NaNO3） which formed through heterogeneous chemical reactions between sea salt and acidic gases. Additionally, aging time of soot was short in Macao due to high humidity, high temperature, and high levels of sunlight in Macao. Most of soot and fine mineral dust particles were internally mixed with secondary particles.展开更多
The Weather Research and Forecasting/Chemistry model （WRF-Chem） was updated by including pho- toexeited nitrogen dioxide （NO2） molecules, heterogeneous reactions on aerosol surfaces, and direct emissions of nitrou...The Weather Research and Forecasting/Chemistry model （WRF-Chem） was updated by including pho- toexeited nitrogen dioxide （NO2） molecules, heterogeneous reactions on aerosol surfaces, and direct emissions of nitrous acid （HONO） in the Carbon-Bond Mechanism Z （CBM-Z）. Five simulations were conducted to assess the effects of each new component and the three additional HONO sources on concentrations of major chemical components. We calculated percentage changes of major aerosol components and concentration ratios of gas NOy （NOyg） to NOy and particulate nitrates （NO3-） to NOy due to the three additional HONO sources in the North China Plain in August of 2007. Our results indicate that when the three additional HONO sources are included, WRF-Chem can reasonably reproduce the HONO observations. Heterogeneous reactions on aerosol surfaces are a key contributor to concentrations of HONO, nitrates （NO3-）, ammonium （NH＋）, and PM2.5 （concentration of particulate matter of ≤2.5 um in the ambient air） across the North China Plain. The three additional HONO sources produced a -5% -20% increase in monthly mean daytime concentration ratios of NO3-/NOy, a -15%- 52% increase in maximum hourly mean concentration ratios of NO3-/NOy, and a -10% -50% increase in monthly mean concentrations of NOx and NH＋ across large areas of the North China Plain. For the Bohai Bay, the largest hourly increases of NO3- exceeded 90%, of NH＋ exceeded 80%, and of PM2.5 exceeded 40%, due to the three additional HONO sources. This implies that the three additional HONO sources can aggravate regional air pollution, further impair visibility, and enhance the incidence of haze in some industrialized regions with high emissions of NOx and particulate matter under favorable meteorological conditions.展开更多
Fe3O4 catalyst supported on spherical γ-Al2O3 was prepared with and without ultrasonic treatment during the impregnation step,and the heterogeneous catalytic oxidation of dimethoate wastewater was conducted with Fent...Fe3O4 catalyst supported on spherical γ-Al2O3 was prepared with and without ultrasonic treatment during the impregnation step,and the heterogeneous catalytic oxidation of dimethoate wastewater was conducted with Fenton reagent.Then,the physical and chemical properties of the catalysts were analyzed by means of XRD,ICP-AES and SEM,especially the effect of Fe3O4 dispersity on γ-Al2O3.The results showed that the activity of the supported catalysts prepared with ultrasonic treatment for dimethoate was higher than those without ultrasonic treatment and the corresponding degradation rate doubled those of the catalyst obtained by impregnation.The probable cause was that for catalysts prepared with ultrasonic treatment,Fe3O4 was well dispersed on the catalyst surface with small particle size,or existed in non-crystalline amorphous state,and Fe content on the catalyst surface was higher than those without ultrasonic treatment.展开更多
基金supported by the National Key Basic Research & Development Program of China (Grant Nos. 2016YFC0203303, 2016YFC0208504 and 2014CB441203)the National Natural Science Foundation of China (Grant Nos. 91544230, 41575145 and 41621005)the EU 7th Framework Marie Curie Actions IRSES project: REQUA (Grant No. PIRSESGA-2013-612671)
文摘Particulate matter with diameters of 2.5 μm or smaller(PM_(2.5)) and ozone(O_3) are major pollutants in the urban atmosphere. PM_(2.5) can affect O_3 by altering the photolysis rate and heterogeneous reactions. However, these two processes and their relative importance remain uncertain. In this paper, with Nanjing in China as the target city, we investigate the characteristics and mechanism of interactions between particles and O_3 based on ground observations and numerical modeling.In 2008, the average concentrations of PM_(2.5) and O_3 at Caochangmen station are 64.6 ± 47.4 μg m^(-3) and 24.6 ± 22.8 ppb,respectively, while at Pukou station they are 94.1 ± 63.4 μg m^(-3) and 16.9 ± 14.9 ppb. The correlation coefficient between PM_(2.5) and O_3 is -0.46. In order to understand the reaction between PM_(2.5) and O_3, we construct a box model, in which an aerosol optical property model, ultraviolet radiation model, gas phase chemistry model, and heterogeneous chemistry model,are coupled. The model is employed to investigate the relative contribution of the aforementioned two processes, which vary under different particle concentrations, scattering capability and VOCs/NOxratios(VOCs: volatile organic compounds;NOx: nitric oxide and nitrogen dioxide). Generally, photolysis rate effect can cause a greater O_3 reduction when the particle concentrations are higher, while heterogeneous reactions dominate O_3 reduction with low-level particle concentrations.Moreover, in typical VOC-sensitive regions, O_3 can even be increased by heterogeneous reactions. In Nanjing, both processes lead to O_3 reduction, and photolysis rate effect is dominant. Our study underscores the importance of photolysis rate effect and heterogeneous reactions for O_3, and such interaction processes should be fully considered in future atmospheric chemistry modeling.
基金supported by the National Basic Research Program (973) of China (No.2006CB403701)the Macao Foundation for Development of Science and Technology (No.023/2006/A)+3 种基金the State Key Laboratory of Coal Resources and Safe Mining (China University of Mining and Technology) (No.SKLCRSM09KFB04)the China Postdoctoral Science Foundation Funded Project(No.20090461213)the Shandong Postdoctoral Science Innovation Foundation (No.200902016)the Independent Innovation Foundation of Shandong University
文摘Aerosol samples were collected in summer in Macao, a coastal city of the Pearl River Delta Region in China. Morphology, size, elemental composition, and mixing state of individual aerosol particles were determined by scanning electron microscopy coupled energy dispersive X-ray （SEM/EDX） and transmission electron microscopy （TEM）. Based on the morphologies of 5711 aerosol particles, they consist of soot （32%）, mineral （17%）, secondary-（22%）, and unknown fine particles （29%）. The sizes of these particles were mostly distributed between 0.1 and 0.4 μm. Compositions of 202 mineral particles were obtained by SEM/EDX. Mineral particles were mainly classified into three types： Si-rich, Ca-rich, and Na-rich. The compositions of typical mineral particles can indicate their sources in sampling location. For example, mineral particles, collected along the main street, were associated with trace amounts of heavy metals, such as Zn, Ti, Mn, Ba, Pb, and As. TEM observations indicate that most Na-rich particles were aged sea salt particles （e.g., Na2SO4 and NaNO3） which formed through heterogeneous chemical reactions between sea salt and acidic gases. Additionally, aging time of soot was short in Macao due to high humidity, high temperature, and high levels of sunlight in Macao. Most of soot and fine mineral dust particles were internally mixed with secondary particles.
基金supported by the National Natural Science Foundation of China (Grant Nos. 41175105 and 40905055)the Key Project of Chinese Academy of Sciences (Grant No. kzcx1-yw-06-04)
文摘The Weather Research and Forecasting/Chemistry model （WRF-Chem） was updated by including pho- toexeited nitrogen dioxide （NO2） molecules, heterogeneous reactions on aerosol surfaces, and direct emissions of nitrous acid （HONO） in the Carbon-Bond Mechanism Z （CBM-Z）. Five simulations were conducted to assess the effects of each new component and the three additional HONO sources on concentrations of major chemical components. We calculated percentage changes of major aerosol components and concentration ratios of gas NOy （NOyg） to NOy and particulate nitrates （NO3-） to NOy due to the three additional HONO sources in the North China Plain in August of 2007. Our results indicate that when the three additional HONO sources are included, WRF-Chem can reasonably reproduce the HONO observations. Heterogeneous reactions on aerosol surfaces are a key contributor to concentrations of HONO, nitrates （NO3-）, ammonium （NH＋）, and PM2.5 （concentration of particulate matter of ≤2.5 um in the ambient air） across the North China Plain. The three additional HONO sources produced a -5% -20% increase in monthly mean daytime concentration ratios of NO3-/NOy, a -15%- 52% increase in maximum hourly mean concentration ratios of NO3-/NOy, and a -10% -50% increase in monthly mean concentrations of NOx and NH＋ across large areas of the North China Plain. For the Bohai Bay, the largest hourly increases of NO3- exceeded 90%, of NH＋ exceeded 80%, and of PM2.5 exceeded 40%, due to the three additional HONO sources. This implies that the three additional HONO sources can aggravate regional air pollution, further impair visibility, and enhance the incidence of haze in some industrialized regions with high emissions of NOx and particulate matter under favorable meteorological conditions.
文摘Fe3O4 catalyst supported on spherical γ-Al2O3 was prepared with and without ultrasonic treatment during the impregnation step,and the heterogeneous catalytic oxidation of dimethoate wastewater was conducted with Fenton reagent.Then,the physical and chemical properties of the catalysts were analyzed by means of XRD,ICP-AES and SEM,especially the effect of Fe3O4 dispersity on γ-Al2O3.The results showed that the activity of the supported catalysts prepared with ultrasonic treatment for dimethoate was higher than those without ultrasonic treatment and the corresponding degradation rate doubled those of the catalyst obtained by impregnation.The probable cause was that for catalysts prepared with ultrasonic treatment,Fe3O4 was well dispersed on the catalyst surface with small particle size,or existed in non-crystalline amorphous state,and Fe content on the catalyst surface was higher than those without ultrasonic treatment.
