During 2005, the filter samples of ambient PM10 from five sites and the source samples of particulate matter were collected in Kaifeng, Henan Province of China. Nineteen elements, water-soluble ions, total carbon (TC...During 2005, the filter samples of ambient PM10 from five sites and the source samples of particulate matter were collected in Kaifeng, Henan Province of China. Nineteen elements, water-soluble ions, total carbon (TC) and organic carbon (OC) contained in samples were analyzed. Seven contributive source types were identified and their contributions to ambient PM10 were estimated by chemical mass balance (CMB) receptor model. Weak associations between the concentrations of organic carbon and element carbon (EC) were observed during the sampling periods, indicating that there was secondary organic aerosol pollution in the urban atmosphere. An indirect method of "OC/EC minimum ratio" was applied to estimate the concentration of secondary organic carbon (SOC). The results showed that SOC contributed 26.2%, 32.4% and 18.0% of TC in spring, summer-fall and winter, respectively, and the annual average SOC concentration was 7.07 μg/m^3, accounting for 5.73% of the total mass in ambient PM10. The carbon species concentrations in ambient PM10 were recalculated by subtracting SOC concentrations from measured concentrations of TC and OC to increase the compatibility of source and receptor measurements for CMB model.展开更多
Seven soil profiles developed on calcium carbonate–rich slope deposits in the Polish Carpathians were studied in order to:i)determine the micromorphological features of heterogeneous soils formed in a carbonate depos...Seven soil profiles developed on calcium carbonate–rich slope deposits in the Polish Carpathians were studied in order to:i)determine the micromorphological features of heterogeneous soils formed in a carbonate depositional environment,and ii)track primary and secondary calcium carbonate forms and their distribution in such stratified soils.Three cases of soils with different arrangements of calcium carbonate were distinguished,controlled mostly by slope processes.For instance,the increasing content and random distribution of angular and subangular rock fragments found in the overall soil matrix and the irregular coarse:fine size limit suggested different intensities of accumulation and mixing of soil material transported along the slope.Slope processes,together with the calcium carbonate content,mineralogical characteristics and texture influenced the type and arrangement of the bfabric pattern.The calcium carbonate distribution within the soils,besides the obvious inheritance from parent material,was governed by the translocation and mixing of deposits on slopes.The climatic conditions prevailing in the area favour the development of secondary forms of calcium carbonate.However,only three of the seven studied profiles contained pedogenic forms of calcium carbonate,yet they were distributed randomly.The occurrence,distribution and preservation of secondary carbonates depended on the content of primary calcium carbonate and soil features such as texture.The transported material down the slope may indicate a very low content of primary calcium or lack thereof,hence its pedogenic forms could not be created.展开更多
In order to tackle the shortcomings of high brittleness,hard graphitization,and poor oxidation resistance resulted from carbonization of phenolic resin of Mg O- C refractories, effects of 2 mass% spherical Ni, and2 ma...In order to tackle the shortcomings of high brittleness,hard graphitization,and poor oxidation resistance resulted from carbonization of phenolic resin of Mg O- C refractories, effects of 2 mass% spherical Ni, and2 mass% spherical Ni plus 7. 5 mass% Al composite powder on microstructure of the secondary carbon in Mg O- C refractories matrix were investigated. The results show that a large number of carbon whiskers form after the carbonization of phenolic resin with Ni powder;in the Mg O- C refractories matrix with only Ni powder,the carbon microspheres form at all treatment temperatures and change slightly with the temperature rising;the carbon whiskers begin to generate in the specimens with composite powder at 1 000 ℃,the diameter of the carbon whiskers is about 0. 4- 0. 5 μm,and the length is about 3- 4 μm,and the formed carbon whiskers increase gradually with the temperature rising.展开更多
Campaigns were conducted to measure Organic Carbon (OC) and Elemental Carbon (EC) in PM2.5 during winter and summer 2003 in Beijing. Modest differences of PM2.5 and PM10 mean concentrations were observed between t...Campaigns were conducted to measure Organic Carbon (OC) and Elemental Carbon (EC) in PM2.5 during winter and summer 2003 in Beijing. Modest differences of PM2.5 and PM10 mean concentrations were observed between the winter and summer campaigns. The mean PM2.5/PM10 ratio in both seasons was around 60%, indicating PM2.5 contributed significantly to PM10. The mean concentrations of OC and EC in PM2.5 were 11.2±7.5 and 6.0±5.0 μg m^-3 for the winter campaign, and 9.4±2.1 and 4.3±3.0 μg m^-3 for the summer campaign, respectively. Diurnal concentrations of OC and EC in PM2.5 were found high at night and low during the daytime in winter, and characterized by an obvious minimum in the summer afternoon. The mean OC/EC ratio was 1.87±0.09 for winter and 2.39±0.49 for summer. The higher OC/EC ratio in summer indicates some formation of Secondary Organic Carbon (SOC). The estimated SOC was 2.8 μg m^-3 for winter and 4.2 μg m^-3 for summer.展开更多
The demand on low-carbon emission fabrication technologies for energy storage materials is increasing dramatically with the global interest on carbon neutrality.As a promising active material for metal-sulfur batterie...The demand on low-carbon emission fabrication technologies for energy storage materials is increasing dramatically with the global interest on carbon neutrality.As a promising active material for metal-sulfur batteries,sulfur is of great interest due to its high-energy-density and abundance.However,there is a lack of industry-friendly and low-carbon fabrication strategies for high-performance sulfur-based active particles,which,however,is in critical need by their practical success.Herein,based on a hail-inspired sulfur nano-storm(HSN)technology developed in our lab,we report an energy-saving,solvent-free strategy for producing core-shell sulfur/carbon electrode particles(CNT@AC-S)in minutes.The fabrication of the CNT@AC-S electrode particles only involves low-cost sulfur blocks,commercial carbon nanotubes(CNT)and activated carbon(AC)micro-particles with high specific surface area.Based on the above core-shell CNT@AC-S particles,sulfur cathode with a high sulfur-loading of 9.2 mg cm^(-2) delivers a stable area capacity of 6.6 mAh cm^(-2) over 100 cycles.Furthermore,even for sulfur cathode with a super-high sulfur content(72 wt%over the whole electrode),it still delivers a high area capacity of 9 mAh cm^(-2) over50 cycles in a quasi-lean electrolyte condition.In a nutshell,this study brings a green and industryfriendly fabrication strategy for cost-effective production of rationally designed S-rich electrode particles.展开更多
To investigate formation mechanisms of secondary organic carbon(SOC) in Eastern China,measurements were conducted in an urban site in Shanghai in the summer of 2015. A period of high O3 concentrations(daily peak 〉...To investigate formation mechanisms of secondary organic carbon(SOC) in Eastern China,measurements were conducted in an urban site in Shanghai in the summer of 2015. A period of high O3 concentrations(daily peak 〉 120 ppb) was observed, during which daily maximum SOC concentrations exceeding 9.0 μg/(C·m^3). Diurnal variations of SOC concentration and SOC/organic carbon(OC) ratio exhibited both daytime and nighttime peaks. The SOC concentrations correlated well with Ox(= O3+ NO2) and relative humidity in the daytime and nighttime, respectively, suggesting that secondary organic aerosol formation in Shanghai is driven by both photochemical production and aqueous phase reactions. Single particle mass spectrometry was used to examine the formation pathways of SOC. Along with the daytime increase of SOC, the number fraction of elemental carbon(EC) particles coated with OC quickly increased from 38.1% to 61.9% in the size range of 250–2000 nm, which was likely due to gas-to-particle partitioning of photochemically generated semi-volatile organic compounds onto EC particles. In the nighttime, particles rich in OC components were highly hygroscopic, and number fraction of these particles correlated well with relative humidity and SOC/OC nocturnal peaks. Meanwhile, as an aqueous-phase SOC tracer, particles that contained oxalate-Fe(III) complex also peaked at night. These observations suggested that aqueous-phase processes had an important contribution to the SOC nighttime formation. The influence of aerosol acidity on SOC formation was studied by both bulk and single particle level measurements, suggesting that the aqueous-phase formation of SOC was enhanced by particle acidity.展开更多
PM10 (particulate matter with aerodynamic diameter less than 10 μm) samples were collected simultaneously at nine urban sites and one urban background site during two intensive observation campaigns in 2006. Concen...PM10 (particulate matter with aerodynamic diameter less than 10 μm) samples were collected simultaneously at nine urban sites and one urban background site during two intensive observation campaigns in 2006. Concentrations of elemental carbon (EC) and organic carbon (OC) in PM10 were analyzed using an element analyzer. The characteristics regarding spatial and seasonal distribution patterns of OC and EC concentrations and their contributions to PM10 mass, as well as correlation between OC and EC, were investigated in detail. The average OC and EC concentrations for urban sites were 57.5 ± 20.8 and 8.3 ± 3.9 μg/m^3, respectively, both being around three times higher than those for urban background site. As a whole, EC concentrations did not show distinct seasonal variations, though OC concentrations were generally higher in autumn than in spring. For urban sites, total carbonaceous aerosol (TCA) accounted for 33.2% in spring and 35.0% in autumn of PM10 mass. The OC and EC concentrations were found significantly correlated to each other both in spring and in autumn, implying the existence of similar emission sources such as coal combustion. The OC/EC ratios generally exceeded 2.0, indicating the presence of secondary organic carbon (SOC), whose estimated concentration for urban Chongqing was 26.7 and 39.4μg/m^3, accounting for 48.9 and 61.9% of the total OC observed in the samples, in spring and in autumn, respectively.展开更多
PM2.5 samples were collected at urban, industrial and coastal sites in Tianjin during winter, spring and summer in 2007. Concentrations of elemental carbon (EC) and organic carbon (OC) were analyzed using the IMPR...PM2.5 samples were collected at urban, industrial and coastal sites in Tianjin during winter, spring and summer in 2007. Concentrations of elemental carbon (EC) and organic carbon (OC) were analyzed using the IMPROVE thermal-optical reflectance (TOR) method. Both OC and EC exhibited a clear seasonal pattern with higher concentrations observed in the winter than in the spring and summer, due to cooperative effect of changes in emission rates and seasonal meteorology. The concentrations of carbonaceous species were also influenced by the local factors at different sampling sites, ranking in the order of industrial〉 urban 〉 coastal during winter and spring. In the summer, the port emissions, enriched with EC, had a significant impact on carbonaceous aerosols at the coastal site. Total carbonaceous aerosol accounted for 40.0% in winter, 33.8% in spring and 31.4% in summer of PM2.5 mass. Good correlation (R = 0.84-0.93) between OC and EC indicated that they had common dominant sources of combustion such as coal burning and traffic emissions. The daily average OC/EC ratios ranged from 2.1 to 9.1, the elevated OC/EC ratios being found in the winter. The estimated secondary organic carbon (SOC) accounted for 46.9%, 35.3% and 40.2% of the total OC in the winter, spring and summer, respectively, indicating that SOC may be an important contributor to fine organic aerosol in Tianjin.展开更多
PM(2.5) samples were collected in Zhengzhou during 3 years of observation, and chemical characteristics and source contribution were analyzed. Approximately 96% of the daily PM(2.5) concentrations and annual avera...PM(2.5) samples were collected in Zhengzhou during 3 years of observation, and chemical characteristics and source contribution were analyzed. Approximately 96% of the daily PM(2.5) concentrations and annual average values exceeded the Chinese National Ambient Air Quality Daily and Annual Standards, indicating serious PM(2.5) pollution. The average concentration of water-soluble inorganic ions was 2.4 times higher in heavily polluted days(daily PM32.5 concentrations > 250 μg/mand visibility < 3 km) than that in other days, with sulfate, nitrate, and ammonium as major ions. According to the ratio of NO-3/SO2-4,stationary sources are still the dominant source of PM(2.5) and vehicle emission could not be ignored. The ratio of secondary organic carbon to organic carbon indicated that photochemical reactivity in heavily polluted days was more intense than in other days.Crustal elements were the most abundant elements, accounting for more than 60% of 23 elements. Chemical Mass Balance results indicated that the contributions of major sources(i.e., nitrate, sulfate, biomass, carbon and refractory material, coal combustion, soil dust,vehicle, and industry) of PM(2.5) were 13%, 16%, 12%, 2%, 14%, 8%, 7%, and 8% in heavily polluted days and 20%, 18%, 9%, 2%, 27%, 14%, 15%, and 9% in other days, respectively.Extensive combustion activities were the main sources of polycyclic aromatic hydrocarbons during the episode(Jan 1-9, 2015) and the total benzo[a]pyrene equivalency concentrations in heavily polluted days present significant health threat. Because of the effect of regional transport, the pollution level of PM(2.5) in the study area was aggravated.展开更多
基金supported by the National Technology Supporting, Kaifeng Environmental Protec-tion Bureau, Henan Province, China
文摘During 2005, the filter samples of ambient PM10 from five sites and the source samples of particulate matter were collected in Kaifeng, Henan Province of China. Nineteen elements, water-soluble ions, total carbon (TC) and organic carbon (OC) contained in samples were analyzed. Seven contributive source types were identified and their contributions to ambient PM10 were estimated by chemical mass balance (CMB) receptor model. Weak associations between the concentrations of organic carbon and element carbon (EC) were observed during the sampling periods, indicating that there was secondary organic aerosol pollution in the urban atmosphere. An indirect method of "OC/EC minimum ratio" was applied to estimate the concentration of secondary organic carbon (SOC). The results showed that SOC contributed 26.2%, 32.4% and 18.0% of TC in spring, summer-fall and winter, respectively, and the annual average SOC concentration was 7.07 μg/m^3, accounting for 5.73% of the total mass in ambient PM10. The carbon species concentrations in ambient PM10 were recalculated by subtracting SOC concentrations from measured concentrations of TC and OC to increase the compatibility of source and receptor measurements for CMB model.
基金financed by the National Science Centre(Poland)(PRELUDIUM 14 project no.2017/27/N/ST10/00342)the Ministry of Science and Higher Education of the Republic of Poland,No.BM–4112/17 and BM–2120/18。
文摘Seven soil profiles developed on calcium carbonate–rich slope deposits in the Polish Carpathians were studied in order to:i)determine the micromorphological features of heterogeneous soils formed in a carbonate depositional environment,and ii)track primary and secondary calcium carbonate forms and their distribution in such stratified soils.Three cases of soils with different arrangements of calcium carbonate were distinguished,controlled mostly by slope processes.For instance,the increasing content and random distribution of angular and subangular rock fragments found in the overall soil matrix and the irregular coarse:fine size limit suggested different intensities of accumulation and mixing of soil material transported along the slope.Slope processes,together with the calcium carbonate content,mineralogical characteristics and texture influenced the type and arrangement of the bfabric pattern.The calcium carbonate distribution within the soils,besides the obvious inheritance from parent material,was governed by the translocation and mixing of deposits on slopes.The climatic conditions prevailing in the area favour the development of secondary forms of calcium carbonate.However,only three of the seven studied profiles contained pedogenic forms of calcium carbonate,yet they were distributed randomly.The occurrence,distribution and preservation of secondary carbonates depended on the content of primary calcium carbonate and soil features such as texture.The transported material down the slope may indicate a very low content of primary calcium or lack thereof,hence its pedogenic forms could not be created.
文摘In order to tackle the shortcomings of high brittleness,hard graphitization,and poor oxidation resistance resulted from carbonization of phenolic resin of Mg O- C refractories, effects of 2 mass% spherical Ni, and2 mass% spherical Ni plus 7. 5 mass% Al composite powder on microstructure of the secondary carbon in Mg O- C refractories matrix were investigated. The results show that a large number of carbon whiskers form after the carbonization of phenolic resin with Ni powder;in the Mg O- C refractories matrix with only Ni powder,the carbon microspheres form at all treatment temperatures and change slightly with the temperature rising;the carbon whiskers begin to generate in the specimens with composite powder at 1 000 ℃,the diameter of the carbon whiskers is about 0. 4- 0. 5 μm,and the length is about 3- 4 μm,and the formed carbon whiskers increase gradually with the temperature rising.
文摘Campaigns were conducted to measure Organic Carbon (OC) and Elemental Carbon (EC) in PM2.5 during winter and summer 2003 in Beijing. Modest differences of PM2.5 and PM10 mean concentrations were observed between the winter and summer campaigns. The mean PM2.5/PM10 ratio in both seasons was around 60%, indicating PM2.5 contributed significantly to PM10. The mean concentrations of OC and EC in PM2.5 were 11.2±7.5 and 6.0±5.0 μg m^-3 for the winter campaign, and 9.4±2.1 and 4.3±3.0 μg m^-3 for the summer campaign, respectively. Diurnal concentrations of OC and EC in PM2.5 were found high at night and low during the daytime in winter, and characterized by an obvious minimum in the summer afternoon. The mean OC/EC ratio was 1.87±0.09 for winter and 2.39±0.49 for summer. The higher OC/EC ratio in summer indicates some formation of Secondary Organic Carbon (SOC). The estimated SOC was 2.8 μg m^-3 for winter and 4.2 μg m^-3 for summer.
基金supported by the Double First-Class Construction Funds of Sichuan University and National Natural Science Foundation of China(NNSFC)financial support from the National Science Foundation of China(51873126,51422305,51721091)。
文摘The demand on low-carbon emission fabrication technologies for energy storage materials is increasing dramatically with the global interest on carbon neutrality.As a promising active material for metal-sulfur batteries,sulfur is of great interest due to its high-energy-density and abundance.However,there is a lack of industry-friendly and low-carbon fabrication strategies for high-performance sulfur-based active particles,which,however,is in critical need by their practical success.Herein,based on a hail-inspired sulfur nano-storm(HSN)technology developed in our lab,we report an energy-saving,solvent-free strategy for producing core-shell sulfur/carbon electrode particles(CNT@AC-S)in minutes.The fabrication of the CNT@AC-S electrode particles only involves low-cost sulfur blocks,commercial carbon nanotubes(CNT)and activated carbon(AC)micro-particles with high specific surface area.Based on the above core-shell CNT@AC-S particles,sulfur cathode with a high sulfur-loading of 9.2 mg cm^(-2) delivers a stable area capacity of 6.6 mAh cm^(-2) over 100 cycles.Furthermore,even for sulfur cathode with a super-high sulfur content(72 wt%over the whole electrode),it still delivers a high area capacity of 9 mAh cm^(-2) over50 cycles in a quasi-lean electrolyte condition.In a nutshell,this study brings a green and industryfriendly fabrication strategy for cost-effective production of rationally designed S-rich electrode particles.
基金supported by the National Natural Science Foundation of China(Nos.91544224,21507010,41775150)the Ministry of Science&Technology of China(No.2012YQ220113-4)the Changjiang Scholars program of the Chinese Ministry of Education
文摘To investigate formation mechanisms of secondary organic carbon(SOC) in Eastern China,measurements were conducted in an urban site in Shanghai in the summer of 2015. A period of high O3 concentrations(daily peak 〉 120 ppb) was observed, during which daily maximum SOC concentrations exceeding 9.0 μg/(C·m^3). Diurnal variations of SOC concentration and SOC/organic carbon(OC) ratio exhibited both daytime and nighttime peaks. The SOC concentrations correlated well with Ox(= O3+ NO2) and relative humidity in the daytime and nighttime, respectively, suggesting that secondary organic aerosol formation in Shanghai is driven by both photochemical production and aqueous phase reactions. Single particle mass spectrometry was used to examine the formation pathways of SOC. Along with the daytime increase of SOC, the number fraction of elemental carbon(EC) particles coated with OC quickly increased from 38.1% to 61.9% in the size range of 250–2000 nm, which was likely due to gas-to-particle partitioning of photochemically generated semi-volatile organic compounds onto EC particles. In the nighttime, particles rich in OC components were highly hygroscopic, and number fraction of these particles correlated well with relative humidity and SOC/OC nocturnal peaks. Meanwhile, as an aqueous-phase SOC tracer, particles that contained oxalate-Fe(III) complex also peaked at night. These observations suggested that aqueous-phase processes had an important contribution to the SOC nighttime formation. The influence of aerosol acidity on SOC formation was studied by both bulk and single particle level measurements, suggesting that the aqueous-phase formation of SOC was enhanced by particle acidity.
文摘PM10 (particulate matter with aerodynamic diameter less than 10 μm) samples were collected simultaneously at nine urban sites and one urban background site during two intensive observation campaigns in 2006. Concentrations of elemental carbon (EC) and organic carbon (OC) in PM10 were analyzed using an element analyzer. The characteristics regarding spatial and seasonal distribution patterns of OC and EC concentrations and their contributions to PM10 mass, as well as correlation between OC and EC, were investigated in detail. The average OC and EC concentrations for urban sites were 57.5 ± 20.8 and 8.3 ± 3.9 μg/m^3, respectively, both being around three times higher than those for urban background site. As a whole, EC concentrations did not show distinct seasonal variations, though OC concentrations were generally higher in autumn than in spring. For urban sites, total carbonaceous aerosol (TCA) accounted for 33.2% in spring and 35.0% in autumn of PM10 mass. The OC and EC concentrations were found significantly correlated to each other both in spring and in autumn, implying the existence of similar emission sources such as coal combustion. The OC/EC ratios generally exceeded 2.0, indicating the presence of secondary organic carbon (SOC), whose estimated concentration for urban Chongqing was 26.7 and 39.4μg/m^3, accounting for 48.9 and 61.9% of the total OC observed in the samples, in spring and in autumn, respectively.
基金supported by The National Natural Science Foundation of China (Grant no.20677030)The Commonweal Project of National Environment Protection (Grant no.200709013)
文摘PM2.5 samples were collected at urban, industrial and coastal sites in Tianjin during winter, spring and summer in 2007. Concentrations of elemental carbon (EC) and organic carbon (OC) were analyzed using the IMPROVE thermal-optical reflectance (TOR) method. Both OC and EC exhibited a clear seasonal pattern with higher concentrations observed in the winter than in the spring and summer, due to cooperative effect of changes in emission rates and seasonal meteorology. The concentrations of carbonaceous species were also influenced by the local factors at different sampling sites, ranking in the order of industrial〉 urban 〉 coastal during winter and spring. In the summer, the port emissions, enriched with EC, had a significant impact on carbonaceous aerosols at the coastal site. Total carbonaceous aerosol accounted for 40.0% in winter, 33.8% in spring and 31.4% in summer of PM2.5 mass. Good correlation (R = 0.84-0.93) between OC and EC indicated that they had common dominant sources of combustion such as coal burning and traffic emissions. The daily average OC/EC ratios ranged from 2.1 to 9.1, the elevated OC/EC ratios being found in the winter. The estimated secondary organic carbon (SOC) accounted for 46.9%, 35.3% and 40.2% of the total OC in the winter, spring and summer, respectively, indicating that SOC may be an important contributor to fine organic aerosol in Tianjin.
基金supported by the public welfare projects from MEPPRC (No. 201409010)
文摘PM(2.5) samples were collected in Zhengzhou during 3 years of observation, and chemical characteristics and source contribution were analyzed. Approximately 96% of the daily PM(2.5) concentrations and annual average values exceeded the Chinese National Ambient Air Quality Daily and Annual Standards, indicating serious PM(2.5) pollution. The average concentration of water-soluble inorganic ions was 2.4 times higher in heavily polluted days(daily PM32.5 concentrations > 250 μg/mand visibility < 3 km) than that in other days, with sulfate, nitrate, and ammonium as major ions. According to the ratio of NO-3/SO2-4,stationary sources are still the dominant source of PM(2.5) and vehicle emission could not be ignored. The ratio of secondary organic carbon to organic carbon indicated that photochemical reactivity in heavily polluted days was more intense than in other days.Crustal elements were the most abundant elements, accounting for more than 60% of 23 elements. Chemical Mass Balance results indicated that the contributions of major sources(i.e., nitrate, sulfate, biomass, carbon and refractory material, coal combustion, soil dust,vehicle, and industry) of PM(2.5) were 13%, 16%, 12%, 2%, 14%, 8%, 7%, and 8% in heavily polluted days and 20%, 18%, 9%, 2%, 27%, 14%, 15%, and 9% in other days, respectively.Extensive combustion activities were the main sources of polycyclic aromatic hydrocarbons during the episode(Jan 1-9, 2015) and the total benzo[a]pyrene equivalency concentrations in heavily polluted days present significant health threat. Because of the effect of regional transport, the pollution level of PM(2.5) in the study area was aggravated.