Fine particles associated with haze pollution threaten the health of over 400 million people in China. Owing to excellent non-destructive fingerprint recognition characteristics, Raman and surface-enhanced Raman scatt...Fine particles associated with haze pollution threaten the health of over 400 million people in China. Owing to excellent non-destructive fingerprint recognition characteristics, Raman and surface-enhanced Raman scattering(SERS) are often used to analyze the composition of fine particles to determine their physical and chemical properties as well as reaction mechanisms. However, there is no comprehensive Raman spectral library of fine particles. Furthermore, various studies that used SERS for fine-particle composition analysis showed that the uniqueness of the SERS substrates and different excitation wavelengths can produce a different spectrum for the same fine-particle component. To overcome this limitation, we conducted SERS experiments with a portable Raman spectrometer using two common SERS substrates(silver(Ag) foil and gold nanoparticles(Au NPs)) and a 785 nm laser. Herein, we introduced three main particle component types(sulfate-nitrate-ammonium(SNA), organic material, and soot) with a total of 39 chemical substances. We scanned the solid Raman, liquid Raman, and SERS spectra of these substances and constructed a fine-particle reference library containing 105 spectra. Spectral results indicated that for soot and SNA, the differences in characteristic peaks mainly originated from the solid-liquid phase transition;Ag foil had little effect on this difference, while the Au NPs caused a significant red shift in the peak positions of polycyclic aromatic hydrocarbons. Moreover, with various characteristic peak positions in the three types of spectra, we could quickly and correctly distinguish substances. We hope that this spectral library will aid in the future identification of fine particles.展开更多
Based on online observations of fine particulate matter(PM2.5) for five consecutive years from January 2013 to December 2017 in Beijing, combined with simultaneous measurement of gaseous precursors and meteorological ...Based on online observations of fine particulate matter(PM2.5) for five consecutive years from January 2013 to December 2017 in Beijing, combined with simultaneous measurement of gaseous precursors and meteorological parameters, the evolution and meteorological causes of fineparticle explosive growth(FPEG) events were analyzed. During the 5-year observation period,132 FPEG events were observed and these events were further divided into three types(3-, 6-, and 9-h events) according to their evolution duration. The majority of FPEG events were observed in winter under the conditions of higher gas precursor concentrations and unfavorable meteorological conditions. The average concentration of PM2.5 during winter FPEG events changed little from 2013 to 2016, whereas it decreased significantly in 2017, in accordance with the similar variation of gaseous species(SO2, NO2, and CO). In addition, the higher wind speeds and lowest relative humidity observed in 2017 were also conducive to the decrease in PM2.5. The evolutions of FPEG events and normal haze episodes were analyzed, revealing that the rate of increase in NO2 was much greater than that of SO2, suggesting more of a contribution from mobile sources than stationary sources. The polar Plot results suggest that the transportation from the southeast area of Beijing plays a major role in the formation of 3-h events, whereas local emissions is the main contributory factor for 9-h events and normal haze episodes. However, further quantitative analysis regarding the contributions of these factors is still needed.展开更多
基金supported by National Natural Science Foundation of China (Nos. 21707077, 21775042, and 21475134)the National Key Research and Development Program of China (No. 2017YFA0207003)+1 种基金the Special Fund of Beijing Key Laboratory of Indoor Air Quality Evaluation and Control (No. BZ0344KF2006)the Fundamental Research Funds for the Central Universities (No. 2020MS037)。
文摘Fine particles associated with haze pollution threaten the health of over 400 million people in China. Owing to excellent non-destructive fingerprint recognition characteristics, Raman and surface-enhanced Raman scattering(SERS) are often used to analyze the composition of fine particles to determine their physical and chemical properties as well as reaction mechanisms. However, there is no comprehensive Raman spectral library of fine particles. Furthermore, various studies that used SERS for fine-particle composition analysis showed that the uniqueness of the SERS substrates and different excitation wavelengths can produce a different spectrum for the same fine-particle component. To overcome this limitation, we conducted SERS experiments with a portable Raman spectrometer using two common SERS substrates(silver(Ag) foil and gold nanoparticles(Au NPs)) and a 785 nm laser. Herein, we introduced three main particle component types(sulfate-nitrate-ammonium(SNA), organic material, and soot) with a total of 39 chemical substances. We scanned the solid Raman, liquid Raman, and SERS spectra of these substances and constructed a fine-particle reference library containing 105 spectra. Spectral results indicated that for soot and SNA, the differences in characteristic peaks mainly originated from the solid-liquid phase transition;Ag foil had little effect on this difference, while the Au NPs caused a significant red shift in the peak positions of polycyclic aromatic hydrocarbons. Moreover, with various characteristic peak positions in the three types of spectra, we could quickly and correctly distinguish substances. We hope that this spectral library will aid in the future identification of fine particles.
基金This study was supported by The Ministry of Science and Technology of the people's Republic of China:[Grant Numbers 2017YFC0210000 and 2016YFC0202700]the National Natural Science Foundation of China:[Grant Number 41705110].
文摘Based on online observations of fine particulate matter(PM2.5) for five consecutive years from January 2013 to December 2017 in Beijing, combined with simultaneous measurement of gaseous precursors and meteorological parameters, the evolution and meteorological causes of fineparticle explosive growth(FPEG) events were analyzed. During the 5-year observation period,132 FPEG events were observed and these events were further divided into three types(3-, 6-, and 9-h events) according to their evolution duration. The majority of FPEG events were observed in winter under the conditions of higher gas precursor concentrations and unfavorable meteorological conditions. The average concentration of PM2.5 during winter FPEG events changed little from 2013 to 2016, whereas it decreased significantly in 2017, in accordance with the similar variation of gaseous species(SO2, NO2, and CO). In addition, the higher wind speeds and lowest relative humidity observed in 2017 were also conducive to the decrease in PM2.5. The evolutions of FPEG events and normal haze episodes were analyzed, revealing that the rate of increase in NO2 was much greater than that of SO2, suggesting more of a contribution from mobile sources than stationary sources. The polar Plot results suggest that the transportation from the southeast area of Beijing plays a major role in the formation of 3-h events, whereas local emissions is the main contributory factor for 9-h events and normal haze episodes. However, further quantitative analysis regarding the contributions of these factors is still needed.