Fine particles associated with haze pollution threaten the health of more than 400 million people in China. It is therefore of great importance to thoroughly investigate and understand their composition. To determine ...Fine particles associated with haze pollution threaten the health of more than 400 million people in China. It is therefore of great importance to thoroughly investigate and understand their composition. To determine the physicochemical properties in atmospheric fine particles at the micrometer level, we described a sensitive and feasible surface-enhanced Raman scattering(SERS) method using Ag foil as a substrate. This novel method enhanced the Raman signal intensities up to 10,000 a.u. for ν(NO_3^-) in fine particles.The SERS effect of Ag foil was further studied experimentally and theoretically and found to have an enhancement factor of the order of ～10~4. Size-fractionated real particle samples with aerodynamic diameters of 0.4–2.5 μm were successfully collected on a heavy haze day,allowing ready observation of morphology and identification of chemical components, such as soot, nitrates, and sulfates. These results suggest that the Ag-foil-based SERS technique can be effectively used to determine the microscopic characteristics of individual fine particles, which will help to understand haze formation mechanisms and formulate governance policies.展开更多
Investigating the heterogeneous reaction on individual atmospheric particles is important because it approximates actual atmospheric conditions and can aid in reducing artifacts in elucidating real mechanisms and proc...Investigating the heterogeneous reaction on individual atmospheric particles is important because it approximates actual atmospheric conditions and can aid in reducing artifacts in elucidating real mechanisms and processes,and determining real kinetic parameters of the atmosphere relevance.This study developed a Raman microspectrometry method to investigate heterogeneous reactions on individual particles.The method was applied to the reaction of NO2 with individual CaCO3 particles.It was demonstrated that Raman microspectrometry can obtain information on both chemical composition and microscopic morphology at the same time,as well as information on chemical characteristics,such as the phase,which is useful for studying reaction processes.Raman spectra of individual particles deposited on a substrate showed no interference by morphological resonance,which is helpful for obtaining high-quality spectra.Moreover,Raman microspectrometry was compared with other methods for investigating heterogeneous reactions on individual particles and was found to have several advantageous characteristics.展开更多
In recent decades, coastal ports have experienced rapid development and become an important economic and ecological hub in China. Atmospheric particle is a research hotspot in atmospheric environmental sciences in inl...In recent decades, coastal ports have experienced rapid development and become an important economic and ecological hub in China. Atmospheric particle is a research hotspot in atmospheric environmental sciences in inland regions. However, few studies on the atmospheric particle were conducted in coastal port areas in China, which indeed suffers atmospheric particle pollution. Lack of the physicochemical characteristics of fine particles serves as an obstacle toward the accurate control for air pollution in the coastal port area in China. Here, a field observation was conducted in an important coastal port city in Yangtze River Delta from March 6 to March 19, 2019. The average PM2.5 concentration was 63.7 ±27.8 μg/m^3 and NO3^-, SO4^2-, NH4^+, and organic matter accounted for ?60% of PM 2.5. Fe was the most abundant trace metal element and V as the ship emission indicator was detected. Transmission electron microscopy images showed that SK-rich, soot, Fe, SK-soot and SK-Fe were the major individual particles in the coastal port. V and soluble Fe were detected in sulfate coating of SK-Fe particles. We found that anthropogenic emissions, marine sea salt, and secondary atmosphere process were the major sources of fine particles. Backward trajectory analysis indicated that the dominant air masses were marine air mass, inland air mass from northern Zhejiang and inland-marine mixed air mass from Shandong and Shanghai during the sampling period. The findings can help us better understand the physicochemical properties of atmospheric fine particles in the coastal port of Eastern China.展开更多
Total suspended particulate （TSP） samples were collected at three sites along the coast of Qingdao, China, before and during a major dust storm in March, 2002. For comparison, PM10（particulate matter with aerodynam...Total suspended particulate （TSP） samples were collected at three sites along the coast of Qingdao, China, before and during a major dust storm in March, 2002. For comparison, PM10（particulate matter with aerodynamic diameters less than 10μm） samples were collected at one of the three sites. The morphological observation and compositional analysis of bulk and individual particles were performed by using scanning electron microscopy equipped with an energy dispersive X-ray system （SEM/EDX） for the TSP and PM10 samples. The results showed that the particles of different kinds of morphology had different elemental compositions, but the particles of similar morphology did not always have the same elemental composition for non-dust samples. The morphology and composition of non-dust particles were different at different sites. The fractal and spherical particles existed mainly in the coarse fraction for non-dust samples, while in the fine mode （〈 10μm） there were floccules formed by fine particles flocking together and containing crustal elements. Compared with the non-dust particles, the dust particles were more homogeneous in terms of morphology, particle size and composition. Particles with irregular shapes and well-distributed sizes dominated in the dust samples, containing crustal elements such as Mg, A1, Si, Ca, Fe, etc. The high sulfur content indicated that homogeneous and heterogeneous reactions took place on the surfaces of the dust particles in the specific environment of Qingdao.展开更多
In an urban-transit bus, fueled by biodiesel in Toledo, Ohio, single inhalable particle samples in October 2008 were collected and detected by scanning electron microscopy and energy dispersive X-ray spectrometry （SE...In an urban-transit bus, fueled by biodiesel in Toledo, Ohio, single inhalable particle samples in October 2008 were collected and detected by scanning electron microscopy and energy dispersive X-ray spectrometry （SEM/EDS）. Particle size analysis found bimodal distribution at 0.2 and 0.5 μm. The particle morphology was characterized by 14 different shape clusters： square, pentagon, hexagon, heptagon, octagon, nonagon, decagon, agglomerate, sphere, triangle, oblong, strip, line or stick, and unknown, by quantitative order. The square particles were common in the samples. Round and triangle particles are more, and pentagon, hexagon, heptagon, octagon, nonagon, decagon, strip, line or sticks are less. Agglomerate particles were found in abundance. The surface of most particles was coarse with a fractal edge that can provide a suitable chemical reaction bed in the polluted atmospheric environment. The three sorts of surface patterns of squares were smooth, semi-smooth, and coarse. The three sorts of square surface patterns represented the morphological characteristics of single inhalable particles in the air inside the bus in Toledo. The size and shape distribution results were compared to those obtained for a bus using ultra low sulfur diesel.展开更多
基金supported by the National Natural Science Foundation of China (Nos.21707077,81571130090)the National Key Research and Development Program (Nos.2017YFC0211500,2016YFC0202700,2017YFC0211601)+1 种基金the Science Fund for Creative Research Groups (No.21521064)the China Postdoctoral Science Foundation (No.2017M610923)
文摘Fine particles associated with haze pollution threaten the health of more than 400 million people in China. It is therefore of great importance to thoroughly investigate and understand their composition. To determine the physicochemical properties in atmospheric fine particles at the micrometer level, we described a sensitive and feasible surface-enhanced Raman scattering(SERS) method using Ag foil as a substrate. This novel method enhanced the Raman signal intensities up to 10,000 a.u. for ν(NO_3^-) in fine particles.The SERS effect of Ag foil was further studied experimentally and theoretically and found to have an enhancement factor of the order of ～10~4. Size-fractionated real particle samples with aerodynamic diameters of 0.4–2.5 μm were successfully collected on a heavy haze day,allowing ready observation of morphology and identification of chemical components, such as soot, nitrates, and sulfates. These results suggest that the Ag-foil-based SERS technique can be effectively used to determine the microscopic characteristics of individual fine particles, which will help to understand haze formation mechanisms and formulate governance policies.
基金financially supported by the National Natural Science Foundation of China (20637020, 40490265 & 20077001)National Basic Research Program of China (2002CB410802)special fund of State Key Joint Laboratory of Environment Simulation and Pollution Control
文摘Investigating the heterogeneous reaction on individual atmospheric particles is important because it approximates actual atmospheric conditions and can aid in reducing artifacts in elucidating real mechanisms and processes,and determining real kinetic parameters of the atmosphere relevance.This study developed a Raman microspectrometry method to investigate heterogeneous reactions on individual particles.The method was applied to the reaction of NO2 with individual CaCO3 particles.It was demonstrated that Raman microspectrometry can obtain information on both chemical composition and microscopic morphology at the same time,as well as information on chemical characteristics,such as the phase,which is useful for studying reaction processes.Raman spectra of individual particles deposited on a substrate showed no interference by morphological resonance,which is helpful for obtaining high-quality spectra.Moreover,Raman microspectrometry was compared with other methods for investigating heterogeneous reactions on individual particles and was found to have several advantageous characteristics.
基金supported by the National Natural Science Foundation of China (Nos. 41805099,91844301)the China Postdoctoral Science Foundation (No. 2018M632449)the Zhejiang Provincial Natural Science Foundation of China (No. LZ19D050001)。
文摘In recent decades, coastal ports have experienced rapid development and become an important economic and ecological hub in China. Atmospheric particle is a research hotspot in atmospheric environmental sciences in inland regions. However, few studies on the atmospheric particle were conducted in coastal port areas in China, which indeed suffers atmospheric particle pollution. Lack of the physicochemical characteristics of fine particles serves as an obstacle toward the accurate control for air pollution in the coastal port area in China. Here, a field observation was conducted in an important coastal port city in Yangtze River Delta from March 6 to March 19, 2019. The average PM2.5 concentration was 63.7 ±27.8 μg/m^3 and NO3^-, SO4^2-, NH4^+, and organic matter accounted for ?60% of PM 2.5. Fe was the most abundant trace metal element and V as the ship emission indicator was detected. Transmission electron microscopy images showed that SK-rich, soot, Fe, SK-soot and SK-Fe were the major individual particles in the coastal port. V and soluble Fe were detected in sulfate coating of SK-Fe particles. We found that anthropogenic emissions, marine sea salt, and secondary atmosphere process were the major sources of fine particles. Backward trajectory analysis indicated that the dominant air masses were marine air mass, inland air mass from northern Zhejiang and inland-marine mixed air mass from Shandong and Shanghai during the sampling period. The findings can help us better understand the physicochemical properties of atmospheric fine particles in the coastal port of Eastern China.
基金supported by the National Natural Science Foundation of China(Grant No.49976020).
文摘Total suspended particulate （TSP） samples were collected at three sites along the coast of Qingdao, China, before and during a major dust storm in March, 2002. For comparison, PM10（particulate matter with aerodynamic diameters less than 10μm） samples were collected at one of the three sites. The morphological observation and compositional analysis of bulk and individual particles were performed by using scanning electron microscopy equipped with an energy dispersive X-ray system （SEM/EDX） for the TSP and PM10 samples. The results showed that the particles of different kinds of morphology had different elemental compositions, but the particles of similar morphology did not always have the same elemental composition for non-dust samples. The morphology and composition of non-dust particles were different at different sites. The fractal and spherical particles existed mainly in the coarse fraction for non-dust samples, while in the fine mode （〈 10μm） there were floccules formed by fine particles flocking together and containing crustal elements. Compared with the non-dust particles, the dust particles were more homogeneous in terms of morphology, particle size and composition. Particles with irregular shapes and well-distributed sizes dominated in the dust samples, containing crustal elements such as Mg, A1, Si, Ca, Fe, etc. The high sulfur content indicated that homogeneous and heterogeneous reactions took place on the surfaces of the dust particles in the specific environment of Qingdao.
文摘In an urban-transit bus, fueled by biodiesel in Toledo, Ohio, single inhalable particle samples in October 2008 were collected and detected by scanning electron microscopy and energy dispersive X-ray spectrometry （SEM/EDS）. Particle size analysis found bimodal distribution at 0.2 and 0.5 μm. The particle morphology was characterized by 14 different shape clusters： square, pentagon, hexagon, heptagon, octagon, nonagon, decagon, agglomerate, sphere, triangle, oblong, strip, line or stick, and unknown, by quantitative order. The square particles were common in the samples. Round and triangle particles are more, and pentagon, hexagon, heptagon, octagon, nonagon, decagon, strip, line or sticks are less. Agglomerate particles were found in abundance. The surface of most particles was coarse with a fractal edge that can provide a suitable chemical reaction bed in the polluted atmospheric environment. The three sorts of surface patterns of squares were smooth, semi-smooth, and coarse. The three sorts of square surface patterns represented the morphological characteristics of single inhalable particles in the air inside the bus in Toledo. The size and shape distribution results were compared to those obtained for a bus using ultra low sulfur diesel.
