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1.
Aerosol size distributions were measured with Micro Orifice Uniform Deposit Impactor (MOUDI) cascade impactors at the rural Angiola and urban Fresno Supersites in California's San Joaquin Valley during the California Regional PM10/PM2.5 Air Quality Study (CRPAQS) winter campaign from December 15, 2000 to February 3, 2001. PM2.5 filter samples were collected concurrently at both sites with Sequential Filter Samplers (SFS). MOUDI nitrate (NO3) concentrations reached 66 μg/m3 on January 6, 2001 during the 1000–1600 PST (GMT-8) period. Pair-wise comparisons between PM2.5 MOUDI and SFS concentrations revealed high correlations at the Angiola site (r > 0.93) but more variability (r < 0.85) at the Fresno site for NO3, sulfate (SO4=), and ammonium (NH4+). Correlations were higher at Fresno (r > 0.87) than at Angiola (r < 0.7) for organic carbon (OC), elemental carbon (EC), and total carbon (TC). NO3 and SO4= size distributions in Fresno were multi-modal and wider than the uni-modal distributions observed at Angiola. Geometric mean diameters (GMD) were smaller for OC and EC than for NO3 and SO4= at both sites. OC and EC were more concentrated on the lowest MOUDI stage (0.056 µm) at Angiola than at Fresno. The NO3 GMD increased from 0.97 to 1.02 µm as the NO3 concentration at Angiola increased from 43 to 66 µg m− 3 during a PM2.5 episode from January 4–7, 2001. There was a direct relationship between GMD and NO3 and SO4= concentrations at Angiola but no such relationships for OC or EC. This demonstrates that secondary aerosol formation increases both concentration and particle size for the rural California environment.  相似文献   

2.
《Atmospheric Research》2007,83(3-4):688-697
Intensive measurements of gas and aerosol for 2 weeks were carried out at Qingdao (gas and aerosol in 2000, 2001 and 2002), Fenghuangshan (gas and aerosol in 2000 and 2001), and Dalian (aerosol in 2002) in the winter–spring period. High SO2 episodes were observed on 18 January 2000 at both Qingdao and Fenghuangshan. According to back trajectory calculations and analysis of gaseous species, high SO2 episodes were caused by local pollution and transport.Nitrate, sulfate and ammonium were the major species in PM2.5. Mass fractions of NO3, nss-SO42− and NH4+ at Qingdao in 2002 were 10%, 12% and 5.5% for PM2.5, respectively, which were higher than that of nss-Ca2+ (1%). Chemical compositions observed at Dalian and Fenghuangshan were similar to those at Qingdao. The mass ratio of nss-SO42−/SO2 at Qingdao in winter was low (< 1.2), indicating that sulfate was probably produced by the slow oxidation of SO2 in the gas phase and/or was transported from outside of Qingdao in winter. The equivalent ratio of NH4+ to nss-SO42− was 1.39, suggesting that ammonium sulfate was one of the major chemical compositions in PM2.5. The NO3/SO42− ratio at Qingdao was higher than that at remote places in East Asia. Gas and aerosol data obtained at Fenghuangshan were similar to data at Qingdao, suggesting that emissions from small cities may have a great influence on pollution in northern China.  相似文献   

3.
The samples of water-soluble inorganic ions (WSIs), including anions (F?, Cl?, SO42?, NO3?) and cations (NH4+, K+, Na+, Ca2+, Mg2+) in 8 size-segregated particle matter (PM), were collected using a sampler (with 8 nominal cut-sizes ranged from 0.43 to 9.0 μm) from October 2008 to September 2009 at five sites in both polluted and background regions of a coastal city, Xiamen. The results showed that particulate matters in the fine mode (PM2.1, Dp < 2.1 μm) comprised large part of mass concentrations of aerosols, which accounted for 45.56–51.27%, 40.04–60.81%, 42.02–60.81%, and 40.46–57.07% of the total particulate mass in spring, summer, autumn, and winter, respectively. The water-soluble ionic species in the fine mode at five sampling sites varied from 15.33 to 33.82 (spring), 14.03 to 28.06 (summer), 33.47 to 72.52 (autumn), and 48.39 to 69.75 μg m? 3 (winter), respectively, which accounted for 57.30 ± 6.51% of the PM2.1 mass concentrations. Secondary pollutants of NH4+, SO42? and NO3? were the dominant contributors of WSIs, which suggested that pollutants from anthropogenic activities, such as SO2, NOx were formed in aerosols by photochemical reactions. The size distributions of Na+, Cl?, SO42? and NO3? were bimodal, peaking at 0.43–0.65 μm and 3.3–5.8 μm. Although some ions, such as NH4+ presented bimodal distributions, the coarse mode was insignificant compared to the fine mode. Ca2+ and Mg2+ exhibited unimodal distributions at all sampling sites, peaking at 2.1–3.3 μm, while K+ having a bimodal distributions with a major peak at 0.43–0.65 μm and a minor one at 3.3–4.7 μm, were used in most of samples. Seasonal and spatial variations in the size-distribution profiles suggested that meteorological conditions (seasonal patterns) and sampling locations (geographical patterns) were the main factors determining the formation of secondary aerosols and characteristics of size distributions for WSIs.  相似文献   

4.
Cloud/fog samples were collected during spring of 2007 in the highly polluted North China Plain in order to examine the impact of pollution and dust particles on cloud water chemistry. The volume weighted mean pH of cloud water was 3.68. The cloud acidity was shown to be associated with air mass origins. Cloud water with its air mass trajectories originating from the southern part of China was more acidic than those from northern China. Anthropogenic source and dust had obvious impact on cloud water composition as indicated by the very high mean concentrations of SO42? (1331.65 μeq L? 1), NO3? (772.44 μeq L? 1), NH4+ (1375.92 μeq L? 1) and Ca2+ (625.81 μeq L? 1) in the observation periods. During sandstorm days, cloud pH values were relatively high, and the concentrations of all the ions in cloud water reached unusual high levels. Significant decreases in the mass concentrations of PM2.5 and PM10 were observed during cloud events. The average scavenging ratio for PM2.5 and PM10 was 52.0% and 55.7%, respectively. Among the soluble ions in fine particles, NO3?, K+ and NH4+ tend to be more easily scavenged than Ca2+ and Na+.  相似文献   

5.
《Atmospheric Research》2009,91(2-4):253-263
A high-volume cascade impactor, equipped with a PM10 inlet, was used to collect size-segregated aerosol samples during the summer of 2004 at two Portuguese locations: a coastal-rural area (Moitinhos) and an urban area (Oporto). Concentrations of airborne particulate matter (PM), total carbon (TC), organic carbon (OC), elemental carbon (EC), and water-soluble organic carbon (WSOC) were determined for the following particle size ranges: < 0.49, 0.49–0.95, 0.95–3.0, and 3.0–10 µm. The total PM mass concentrations at the urban and coastal-rural sites ranged from 22.8 to 79.6 μg m 3 and 19.9 to 28.2 μg m 3, respectively, and more than 56% of the total aerosol mass was found in the fractions below 3.0 μm. At both locations the highest concentrations of OC and EC were found in the submicrometer size range. The regional variability for the OC and EC concentrations, with the highest concentrations being found in the urban area, was related to the contribution of local primary sources (mostly traffic emissions). It was also verified an enrichment of the small size particles in WSOC, representing on average 37.3(± 12.4)% and 59.7(± 18.0)% of OC in the very fine aerosol at the coastal-rural and urban areas, respectively. The amount of secondary OC calculated by the minimum OC/EC ratio method indicates that secondary organic aerosol formation was important throughout the study at both sites. The obtained results suggest that long-range transport and favourable summer conditions for photochemical oxidation are key factors determining secondary OC formation in the coastal-rural and urban areas. The ultraviolet absorption properties of the chromophoric constituents of the WSOC fractions were also different among the different particle size ranges and also between the two sampling locations, thus suggesting the strong impact of the diverse emission sources into the composition of the size-segregated organic aerosol.  相似文献   

6.
In this study, 24-h PM2.5 samples were collected using Harvard Honeycomb denuder/filter-pack system during different seasons in 2006 and 2007 at an urban site in Guangzhou, China. The particles collected in this study were generally acidic (average strong acidity ([H+]) ~ 70 nmol m? 3). Interestingly, aerosol sulfate was not fully neutralized in the ammonia-rich atmosphere (NH3 ~ 30 ppb) and even when NH4+]/[SO42?] was larger than 2. Consequently, strong acidity ([H+]) as high as 170 nmol m? 3 was observed in these samples. The kinetic rate of neutralization of acidity (acidic sulfate) by ambient ammonia was significantly higher than the rate of formation of ammonium nitrate involving HNO3 and NH3 for [NH4+]/[SO42?]  1.5 and much lower for NH4+]/[SO42?] > 1.5. Therefore, higher nitrate principally formed via homogeneous gas phase reactions involving ammonia and nitric acid were observed for [NH4+]/[SO42?] > 1.5. However, little nitrate, probably formed via heterogeneous processes e.g. reaction of HNO3 with sea salt or crustal species, was observed for [NH4+]/[SO42?]  1.5. These demonstrate a clear transition in the pathways of ambient ammonia to form aerosol ammonium at [NH4+]/[SO42?] = 1.5 and evidently explain the observed high acidity due to the unneutralized sulfate in the ammonium-rich aerosol (NH4+]/[SO42?] > 1.5). In fact, the measured acidity was almost similar to the excess acid defined as the acid that remains at [NH4+]/[SO42?] = 1.5 due to the un-neutralized fraction of sulfate ([H+] = 0.5[SO42?]). The presence of high excess acid and ammonium nitrate significantly lowered the deliquescence relative humidity of ammonium sulfate (from 80% to 40%) in the ammonium-rich samples.  相似文献   

7.
A comprehensive study on the chemical compositions of rainwater was carried out from Jan. to Dec. in 2008 in Chengdu, a city located on the acid rain control zone of southwest China. All samples were analyzed for pH and major ions (F, Cl?, NO3?, SO42?, K+, Na+, Ca2+, Mg2+, and NH4+). The pH increased due to the result of neutralization caused by the base ions. It was observed that Ca2+ was the most abundant cation with a VWM value of 196.6 μeq/L (17.3–1568.7 μeq/L), accounting for 49.7% (9.4%–79.2%) of the total cations. SO42? was the most abundant anion with VWM value of 212.8 μeq/L (41.8–1227.6 μeq/L). SO42? and NO3? were dominant among the anions, accounting for 90.4%–99.1% of the total measured anions.The concentrations of NO3? were higher than the most polluted cities abroad, which indicated Chengdu has been a severe polluted city over the world. The high fuel consumption from urbanization and the rapid increase of vehicles resulted in the high emission of SO2 and NOx, which were the precursor of the high concentration of acidic ions NO3? and SO42?. It was the main reason of the severe acid rain in Chengdu.The high concentrations of alkaline ions (mainly Ca2+, NH4+) in Chengdu city atmosphere have played an important role to neutralize the acidity of rainwater and the pH value has increased by 0.7 units since 1989. It is worth noting that the emission of NOx from the automobile exhaust is increased and is becoming the important precursor of acid rain now.  相似文献   

8.
Severe air pollution with visibility deterioration has long been a focus in the North China Plain (NCP). In this study, concentration and light extinction analysis of PM2.5 chemical components were carried out from 2014 to 2017 to study the pollution characteristics in Baoding, a case city of the NCP. The annual average concentration of total PM2.5 components showed a declining trend, decreasing by 11 µg m−3 (water-soluble inorganic ions), 23 µg m−3 (carbonaceous aerosols), and 1796 ng m−3 (inorganic elements). Contributing 82.9% to the concentration of total ions, the dominant components, NH4+, NO3, and SO42− became the main pollutants in PM2.5 pollution. Based on the IMPROVE algorithm, the average reconstructed PM2.5 mass concentration was 93 ± 69 µg m−3 during the observation period. Meanwhile, the light extinction coefficients were 373.8 ± 233.6 M m−1, 405.3 ± 300.1 M m−1, 554.3 ± 378.2 M m−1 and 1005.2 ± 750.3 M m−1, in spring, summer, autumn, and winter, respectively. Ammonium sulfate, ammonium nitrate, and organic matter were the largest contributors to light extinction, accounting for a total of 55%–77% in the four seasons. The bsca (light scattering by particles and gases) reconstructed from PM2.5 components (Rbsca) and the bsca converted from visibility (Vbsca) were compared to evaluate the performance of the IMPROVE algorithm, revealing a high correlation coefficient of 0.84. The high values of Vbsca were underestimated while the low values were overestimated, as determined through comparison with the one-to-ne line. Especially, when Rbsca > 1123 M m−1 (corresponding to < 2.0 km, approximately), Vbsca was underestimated by 17.6%. PM2.5 mass concentration and relative humidity also had an impact on the estimation.摘要华北平原大气污染与低能见度状况一直是人们关切的问题.本文通过分析2014 - 2017年PM2.5化学成分的浓度和消光效果, 研究了华北平原典型城市保定市的大气污染特征.结果表明, PM2.5组分的年均浓度显示下降趋势, 水溶性无机离子,碳质气溶胶和金属元素分别减少了11 µg m−3, 23 µg m−3和1796 ng m−3.NH4+,NO3和SO42−是PM2.5污染的主要污染物, 三者之和占总离子浓度的82.9%.基于IMPROVE方程对细颗粒物进行重构, 在观测期间PM2.5质量浓度平均为93 ± 69 µg m−3, 春季,夏季,秋季和冬季的消光系数分别为373.8 ± 233.6 M m−1,405.3 ± 300.1 M m−1,554.3 ± 378.2 M m−1和1005.2 ± 750.3 M m−1.硫酸铵,硝酸铵和有机物对消光的贡献最大, 不同季节下占比达55% ~77%.通过PM2.5组分进行重构, 利用IMPROVE算法计算得到Rbsca, 用能见度测量值转换得到Vbsca, 二者具有较高的相关性 (r2=0.84) ;但存在Vbsca的高值被低估, Vbsca的低值被高估的现象;特别是当Rbsca > 1123 M m−1 (对应能见度约小于2.0 km) 时, Vbsca的值被低估了17.6%.高浓度PM2.5和高湿度对IMPROVE算法结果有显著的影响.  相似文献   

9.
The relationships between meteorological conditions (temperature, wind-speed and direction, relative humidity, surface-inversion depth and strength, and stability) and PM2.5 concentrations in Fairbanks, Alaska were investigated using ten years of observational data. The results show that during wintertime (November through February) PM2.5 concentrations exceeding the 24 h National Air Quality Standard (35 μg/m3) occurred under calm wind, extremely low temperature (≤20 °C) and moisture (water-vapor pressure < 2 hPa) multiday surface-inversion conditions that trap the pollutants in the breathing level and inhibit transport of polluted air out of Fairbanks. PM2.5 concentrations tend to be higher under stable than other conditions, but are not sensitive to the degree of stability. The presence of a surface inversion and calm wind are necessary, but in combination with low temperatures and humidity, the conditions are sufficient for high PM2.5 concentrations. The low temperatures are required because they lead to increased emission rates from domestic heating and power production. During multiday inversions with temperatures above ? 20 °C, high relative humidity (> 75%) partly caused by water-vapor emission reduces PM2.5 concentrations.  相似文献   

10.
Zhang  Xiaoyu  Ji  Guixiang  Peng  Xiaowu  Kong  Lingya  Zhao  Xin  Ying  Rongrong  Yin  Wenjun  Xu  Tian  Cheng  Juan  Wang  Lin 《Journal of Atmospheric Chemistry》2022,79(2):101-115

In this study, 123 PM2.5 filter samples were collected in Wuhan, Hubei province from December 2014 to November 2015. Water- soluble inorganic ions (WSIIs), elemental carbon (EC), organic carbon (OC) and inorganic elements were measured. Source apportionment and back trajectory was investigated by the positive matrix factorization (PMF) model and the hybrid single particle lagrangian integrated trajectory (HYSPLIT) model, respectively. The annual PM2.5 concentration was 80.5?±?38.2 μg/m3, with higher PM2.5 in winter and lower in summer. WSIIs, OC, EC, as well as elements contributed 46.8%, 14.8%, 6.7% and 8% to PM2.5 mass concentration, respectively. SO42?, NO3? and NH4+ were the dominant components, accounting for 40.2% of PM2.5 concentrations. S, K, Cl, Ba, Fe, Ca and I were the main inorganic elements, and accounted for 65.2% of the elemental composition. The ratio of NO3?/SO42? was 0.86?±?0.72, indicating that stationary sources play dominant role on PM2.5 concentration. The ratio of OC/EC was 2.9?±?1.4, suggesting the existence of secondary organic carbon (SOC). Five sources were identified using PMF model, which included secondary inorganic aerosols (SIA), coal combustion, industry, vehicle emission, fugitive dust. SIA, coal combustion, as well as industry were the dominant contributors to PM2.5 pollution, accounting for 34.7%, 20.5%, 19.6%, respectively.

  相似文献   

11.
Chemical characteristics of haze during summer and winter in Guangzhou   总被引:33,自引:0,他引:33  
Airborne particles were collected with a 10-stage MOUDI and a PM10 sampler in Guangzhou, China, during both haze and normal days in the summer of 2002 and 2003, and winter 2002. The characteristics of PAHs, organic carbon, elemental carbon and water-soluble inorganic ions were studied under four periods (summer normal, summer haze, winter normal and winter haze). In this study, secondary pollutants (OC, SO42−, NO3 and NH4+) were the major chemical components and appeared to show a remarkably rapid increase from normal to haze days. The particle mass size distributions were bimodal and dominated by fine particles in haze days. A significantly higher OC/EC ratio was found in haze days (3.2–4.7) compared to normal days (1.8–2.8), indicating secondary organic aerosol formation might be significant during haze days. Correlation analysis between visibility and chemical species showed that the major scattering species were TC (total carbon) and sulfate in normal days and nitrate and TC in haze days, respectively. Simultaneously, correlation analysis between visibility and meteorological factors demonstrated that visibility increased with both temperature and wind speed, while it decreased with relative humidity. Furthermore, the relatively higher value of IcdP/(BghiP + IcdP) and the low value of Cmax, CPI, and BghiP/BeP in winter haze could be due to the growth of motor vehicle usage and energy consumption in winter.  相似文献   

12.
Gaseous pollutants and PM2.5 aerosol particles were investigated during a tropical storm and an air pollution episode in southern Taiwan. Field sampling and chemical analysis of particulate matter and gaseous pollutants were conducted in Daliao and Tzouying in the Kaohsiung area, using a denuder-filter pack system during the period of 22 October to 3 November 2004. Sulfate, nitrate and ammonium were the major ionic species in the PM2.5, accounting for 46 and 39% of the PM2.5 for Daliao and Tzouying, respectively. Higher PM2.5, Cl?, NO3? and NH4+, HNO2 and NH3 concentrations were found at night in both stations, whereas higher HNO3 was found during the day. In general, higher PM2.5, HCl, NH3, SO2, Cl?, NO3?, SO42? and NH4+ concentrations were found in Daliao. The synoptic weather during the experiment was first influenced by Typhoon NOCK-TEN, which resulted in the pollutant concentrations decreasing by about two-thirds. After the tropical thunderstorm system passed, the ambient air quality returned to the previous condition in 12 to 24 h. When there was a strong subsidence accompanied by a high-pressure system, a more stable environment with lower wind speed and mixing height resulted in higher PM2.5, as well as HNO2, NH3, SO42?, Cl?, NO3?, NH4+ and K+ concentrations during the episode days. The rainfall is mainly a scavenger of air pollutants in this study, and the stable atmospheric system and the high emission loading are the major reasons for high air pollutant concentrations.  相似文献   

13.
Climate output from the UK Hadley Centre's HadCM2 and HadCM3 experiments for the period 1860 to 2100, with IS92a greenhouse gas forcing, together with predicted patterns of N deposition and increasing CO2, were input (offline) to the dynamic vegetation model, Hybrid v4.1 (Friend et al., 1997; Friend and White, 1999). This model represents biogeochemical, biophysical and biogeographical processes, coupling the carbon, nitrogen and water cycles on a sub-daily timestep, simulating potential vegetation and transient changes in annual growth and competition between eight generalized plant types in response to climate.Global vegetation carbon was predicted to rise from about 600 to 800 PgC (or to 650 PgC for HadCM3) while the soil carbon pool of about 1100 PgC decreased by about 8%. By the 2080s, climate change caused a partial loss of Amazonian rainforest, C4 grasslands and temperate forest in areas of southern Europe and eastern USA, but an expansion in the boreal forest area. These changes were accompanied by a decrease in net primary productivity (NPP) of vegetation in many tropical areas, southern Europe and eastern USA (in response to warming and a decrease in rainfall), but an increase in NPP of boreal forests. Global NPP increased from 45 to 50 PgC y−1 in the 1990s to about 65 PgC y−1 in the 2080s (about 58 PgC y−1 for HadCM3). Global net ecosystem productivity (NEP) increased from about 1.3 PgC y−1 in the 1990s to about 3.6 PgC y−1 in the 2030s and then declined to zero by 2100 owing to a loss of carbon from declining forests in the tropics and at warm temperate latitudes — despite strengthening of the carbon sink at northern high latitudes. HadCM3 gave a more erratic temporal evolution of NEP than HadCM2, with a dramatic collapse in NEP in the 2050s.  相似文献   

14.
A mooring equipped with 200 high-resolution temperature sensors between 6 and 404 m above the bottom was moored in 1890 m water depth above a steep, about 10° slope of Mount Josephine, NE-Atlantic. The sensors have a precision of less than 0.5 mK. They are synchronized via induction every 4 h so that the 400 m range is measured to within 0.02 s, every 1 s. Thin cables and elliptical buoyancy assured vertical mooring motions to be smaller than 0.1 m under maximum 0.2 m s−1 current speeds. The local bottom slope is supercritical for semidiurnal internal tides by a factor of two. Exploring a one-month record in detail, the observations show: 1/semidiurnal tidal dominance in variations of dissipation rate ε, eddy diffusivity Kz and temperature, but no significant correlation between the records of ε and total kinetic energy, 2/a variation with time over four orders of magnitude of 100-m vertically averaged ε, 3/a local minimum in density stratification between 50 and 100 m above the bottom, 4/a gradual decrease in daily or longer averaged ε and Kz by one order of magnitude over a vertical distance of 250 m, upwards from 150 m above the bottom, 5/monthly mean values of <[ε]> = 2 ± 0.5 × 10−7 m2 s−3, <[Kz]> = 8 ± 3 × 10−3 m2 s−1 averaged over the lower 150 m above the bottom.  相似文献   

15.
Beijing is one of the largest and most densely populated cities in China. PM2.5 (fine particulates with aerodynamic diameters less than 2.5 μm) pollution has been a serious problem in Beijing in recent years. To study the temporal and spatial variations in the chemical components of PM2.5 and to discuss the formation mechanisms of secondary particles, SO2, NO2, PM2.5, and chemical components of PM2.5 were measured at four sites in Beijing, Dingling (DL), Chegongzhuang (CG), Fangshan (FS), and Yufa (YF), over four seasons from 2012 to 2013. Fifteen chemical components, including organic carbon (OC), elemental carbon (EC), K+, NH4 +, NO3 ?, SO4 2?, Cl?, Al, Ca, Fe, Mg, Na, Pb, Si, and Zn, were selected for analysis. Overall, OC, SO4 2?, NO3 ?, and NH4 + were dominant among 15 components, the annual average concentrations of which were 22.62 ± 21.86, 19.39 ± 21.06, 18.89 ± 19.82, and 13.20 ± 12.80 μg·m?3, respectively. Compared with previous studies, the concentrations of NH4 + were significantly higher in this study. In winter, the average concentrations of OC and EC were, respectively, 3 and 2.5 times higher than in summer, a result of coal combustion during winter. The average OC/EC ratios over the four sites were 4.9, 7.0, 8.1, and 8.4 in spring, summer, autumn, and winter, respectively. The annual average [NO3 ?]/[SO4 2?] ratios in DL, CG, FS, and YF were 1.01, 1.25, 1.08, and 1.12, respectively, which were significantly higher than previous studies in Beijing, indicating that the contribution ratio of mobile source increased in recent years in Beijing. Analysis of correlations between temperature and relative humidity and between SOR ([SO4 2?]/([SO4 2?] + [SO2])) and NOR ([NO3 ?]/([NO3 ?] + [NO2])) indicated that gas-phase oxidation reactions were the major formation mechanism of SO4 2? in spring and summer in urban Beijing, whereas slow gas-phase oxidation reactions and heterogeneous reactions both occurred in autumn and winter. NO3 ? was mainly formed through year-round heterogeneous reactions in urban Beijing.  相似文献   

16.
Concentrations and flux densities of methane were determined during a Lagrangian study of an advective filament in the permanent upwelling region off western Mauritania. Newly upwelled waters were dominated by the presence of North Atlantic Central Water and surface CH4 concentrations of 2.2 ± 0.3 nmol L−1 were largely in equilibrium with atmospheric values, with surface saturations of 101.7 ± 14%. As the upwelling filament aged and was advected offshore, CH4 enriched South Atlantic Central Water from intermediate depths of 100–350 m was entrained into the surface mixed layer of the filament following intense mixing associated with the shelf break. Surface saturations increased to 198.9 ± 15% and flux densities increased from a mean value over the shelf of 2.0 ± 1.1 μmol m−2 d−1 to a maximum of 22.6 μmol m−2 d−1. Annual CH4 emissions for this persistent filament were estimated at 0.77 ± 0.64 Gg which equates to a maximum of 0.35% of the global oceanic budget. This raises the known outgassing intensity of this area and highlights the importance of advecting filaments from upwelling waters as efficient vehicles for air-sea exchange.  相似文献   

17.
Shanghai is the largest industrial and commercial city in China, and its air quality has been deteriorating for several decades. However, there are scarce researches on the level and seasonal variation of fine particle (PM2.5) as well as the carbonaceous fractions when compared with other cities in China and around the world. In the present paper, abundance and seasonal characteristics of PM2.5, organic carbon (OC) and elemental carbon (EC) were studied at urban and suburban sites in Shanghai during four season-representative months in 2005–2006 year. PM2.5 samples were collected with high-vol samplers and analyzed for OC and EC using thermal-optical transmittance (TOT) protocol. Results showed that the annual average PM2.5 concentrations were 90.3–95.5 μg/m3 at both sites, while OC and EC were 14.7–17.4 μg/m3 and 2.8–3.0 μg/m3, respectively, with the OC/EC ratios of 5.0–5.6. The carbonaceous levels ranked by the order of Beijing > Guangzhou > Shanghai > Hong Kong. The carbonaceous aerosol accounted for  30% of the PM2.5 mass. On seasonal average, the highest OC and EC levels occurred during fall, and they were higher than the values in summer by a factor of 2. Strong correlations (r = 0.79–0.93) between OC and EC were found in the four seasons. Average level of secondary organic carbon (SOC) was 5.7–7.2 μg/m3, accounting for  30% of the total OC. Strong seasonal variation was observed for SOC with the highest value during fall, which was about two times the annual average.  相似文献   

18.
《Atmospheric Research》2009,91(2-4):195-202
We present results of direct aerosol radiative forcing over a French Mediterranean coastal zone based on one year of continuous observations of aerosol optical properties during 2005–2006. Monthly-mean aerosol optical depth at 440 nm ranged between 0.1 and 0.34, with high Angstrom coefficient (α > 1.2). The single scattering albedo (at 525 nm) estimated at the surface ranged between 0.7 and 0.8, indicating significant absorption. The presence of aerosols over the Mediterranean zone during summer decreases the shortwave radiation reaching the surface by as much as 26 ± 3.9 W m 2, and increases the top of the atmosphere reflected radiation by as much as 5.2 ± 1.0 W m 2. The shortwave atmospheric absorption translates to an atmospheric heating of 2.5 to 4.6 K day 1. Concerted efforts are needed for investigating the possible impact of the increase in heating rate on the maintenance of heat-waves frequently occurring over this coastal region during summer time.  相似文献   

19.
The variability of sea surface Total Alkalinity (TA) and sea surface Total Inorganic Carbon (CT) is examined using all available data in the western tropical Atlantic (WTA: 20°S-20°N, 60°W-20°W). Lowest TA and CT are observed for the region located between 0°N-15°N/60°W-50°W and are explained by the influence of the Amazon plume during boreal summer. In the southern part of the area, 20°S-10°S/40°W-60°W, the highest values of TA and CT are linked to the CO2–rich waters due to the equatorial upwelling, which are transported by the South Equatorial Current (SEC) flowing from the African coast to the Brazilian shore. An increase of CT of 0.9 ± 0.3 μmol kg−1yr−1 has been observed in the SEC region and is consistent with previous published estimates. A revised CT-Sea Surface Salinity (SSS) relationship is proposed for the WTA to take into account the variability of CT at low salinities. This new CT-SSS relationship together with a published TA-SSS relationship allow to calculate pCO2 values that compare well with observed pCO2 (R2 = 0.90).  相似文献   

20.
《Atmospheric Research》2008,87(3-4):297-314
This paper addresses the sensitivity of the relationships between radar reflectivity (Z) and liquid water content (M) for liquid water clouds to microphysical drizzle parameters by means of simulated radar observation at a frequency of 3 GHz of modeled cumulus clouds. A power law relationship for non drizzling clouds with water content as high as 3 gm 3: Zc = 0.026 Mc1.61 is numerically derived and agreed with previous empirical relationships relative to cumulus and stratocumulus. This relationship is then used to explore the influence of drizzle on the correlation between radar reflectively and water content. Due to their large diameters with respect to cloud droplets, drizzle sized drops dominate radar reflectivity but do not carry the cloud water content so that reflectivity and liquid water content are expected to be not correlated in clouds containing drizzle. It is shown that for congestus or extreme congestus cumuli, microphysical conditions for which the ZcMc relationship can be used with a tolerance of 5 and 10% are provided whereas for humilis or mediocris cumuli, the presence of drizzle breaks down the ZcMc relationship whatever the situations.  相似文献   

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