Origin of soluble chemical species in bulk precipitation collected in Tokyo,Japan: Statistical evaluation of source materials

An iterative least-squares method with a receptor model was applied to the analytical data of the precipitation samples collected at 23 points in the suburban area of Tokyo, and the number and composition of the source materials were determined. Thirty-nine monthly bulk precipitation samples were collected in the spring and summer of 1987 from the hilly and mountainous area of Tokyo and analyzed for Na⁺, K⁺, NH₄⁺, Mg²⁺, Ca²⁺, F⁻, Cl⁻, Br⁻, NO₃⁻ and SO₄²⁻ by atomic absorption spectrometry and ion chromatography. The pH of the samples was also measured. A multivariate ion balance approach (Tsurumi, 1982, Anal. Chim. Acta138, 177–182) showed that the solutes in the precipitation were derived from just three major sources; sea salt, acid substance (a mixture of 53% HNO₃, 39% H₂SO₄ and 8% HCl in equivalent) and CaSO₄. The contributions of each source to the precipitation were calculated for every sampling site. Variations of the contributions with the distance from the coast were also discussed.     

Factor analysis of trends in Texas acidic deposition

Precipitation chemistry data collected between 1980 and 1987 for 11 NADP/NTN sites in Texas have been analyzed using factor analysis and a trend analysis of monthly averages. Factor analysis identified four major factors which differed significantly from site to site: (1) a Gulf factor of Na⁺, Cl^-, and Mg²⁺; (a) a soil factor of Ca²⁺, K⁺, Na⁺, and Mg²⁺; (3) an acid factor of H⁺, NO₋³, and SO₄⁴⁻; and (4) an aged aerosol factor of NO₃⁻, SO₄²⁻, and NH₄⁺. At Longview, the acid and Gulf factors accounted for 18 and 46%, respectively, of the variation of the data. A trend analysis was performed on the logarithm of the monthly averages at the Longview and Victoria sites, the two sites with the largest and most complete data. Results suggest that hydrogen ions have been increasing at both sites, while calcium ions have been decreasing.     

Influence of sea salt aerosols and long range transport on precipitation chemistry at El Verde,Puerto Rico

The chemistry of bulk precipitation was measured from November 1983 to September 1987 at El Verde in the Luquillo Experimental Forest, Puerto Rico. Wet-only precipitation was also analyzed as part of the National Atmospheric Deposition Program from 1984 to 1987. Volume-weighted mean pH was 5.14 in bulk precipitation and 5.12 in wet precipitation. Concentrations of most species were correlated negatively with weekly rainfall. Sea salt aerosols contributed most of the Na⁺, Cl⁻, Mg²⁺ and K⁺ found in wet and bulk precipitation; sulfate and calcium, however, were derived primarily from non-sea salt sources. Due to the high rainfall (3.4 m annually during the study period) and close proximity of the study site to the ocean, deposition rates of the major cations and anions were high relative to many other tropical sites. Precipitation chemistry at El Verde appears to be affected by several factors. During summer, Saharan dusts contribute a significant portion of the excess Ca²⁺, K⁺ and Mg²⁺. During winter months, cold fronts may transport SO₄²⁻ and NO₃⁻ from North America and the western part of Puerto Rico to the sampling site.     

Urban precipitation chemistry: A review and synthesis

Urban sampling sites have been specifically excluded from recent large networks for measuring chemical composition of precipitation. Because information on precipitation composition in urban areas is needed for a variety of current applications, it is useful to summarize present knowledge. Most of the available information is based on samples of bulk precipitation, collected by continuously open collectors. This method is now widely acknowledged to be of limited value because of its poor sampling characteristics for dry deposition. For many ions, particularly those residing on large airborne particles, urban bulk sampling yielded considerably higher concentrations than found in samples collected in ‘wet-only’ samplers. Spatial variability of ionic concentrations in urban areas is expressed in terms of the sample standard deviation of site precipitation-weighted means, as a percentage of the overall urban mean. Median values of the most major ions were near 30%; half of the available measurements were between 20 and 47%. Differences between urban and nearby rural concentrations of ions in precipitation were often reported. Those ions with some tendency to occur in higher concentrations in cities included Na⁺, Mg²⁺, Ca²⁺, NO₃⁻, SO₄²⁻ and Cl⁻. These differences should be viewed with caution, however, because they were usually based on one or two, possibly unrepresentative, rural sampling sites. Seasonal variations of urban [H⁺] were different in Europe and the U.S. Highest concentrations occurred in winter in Europe, but in summer in the U.S. There is a pressing need for additional urban precipitation chemistry monitoring and research.     

Use of simple daily atmospheric circulation types for the interpretation of precipitation composition at a site (Eskdalemuir) in Scotland, 1978–1984

A simple daily weather type of classification for the British Isles (Lamb, 1972, Geophys. Mem.16) may be used as a convenient method to categorize precipitation composition (excess SO²⁻₄, NO⁻₃, NH⁻₃, NH⁺₄, H⁺) at a site in southern Scotland. Precipitation associated with four weather types in particular (Westerly: W, Cyclonic: C, Southerly: S, Southwesterly: SW), has a strong influence on the annual mean precipitation-weighted composition. The single most important influence is the ‘dilution’ effect of precipitation associated with W-types. Trends in composition over the period 1978–1984 appear to be strongly related to the annual amounts of C-type and, especially, W-type precipitation. These links may confound the relationships between emissions and deposition over a restricted region. The pronounced annual cycle in precipitation composition at the station may also be explained, in large part, by the annual meteorological cycle which can, in turn, be characterized by the weather types. The significance of these findings is that there are known, and large, change in the relative annual frequencies of the major weather types on time-scales of decades. This indicates a possible contribution to non-linearity between emissions and depositions on the longer time-scale.     

Chemical composition of rain in Thessaloniki,Greece, in relation to meteorological conditions

Wet precipitation was collected in Thessaloniki, Greece, during the period March 1989–December 1990 by using an automatic wet-only precipitation sampler.Rainwater samples were analysed for major cations (H⁺, NH₄⁺, Na⁺, K⁺, Ca²⁺, Mg²⁺) and anions (Cl⁻, NO₃⁻, SO₄²⁻), in addition to acidity and conductivity measurements. The majority of rain had a neutral or alkaline character as a result of neutralization, primarily caused by calcareous soil dust and secondarily by atmospheric ammonia. In all rain, SO₄²⁻ concentration exceeded NO₃⁻ concentration. The contribution of maritime sources to the total SO₄²⁻ concentration was very low (<2%).The chemical composition of precipitation was analysed in conjunction with meteorological variables (season of the year, precipitation type, airflow patterns) to evaluate temporal variations and chemical source influence. Rain caused by weak, localized flows showed the highest acidity and the minimum influence of neutralization processes.     

Elements in the precipitation of S. Paulo City (Brazil)

Rainwater samples in S. Paulo city were collected on an event basis from October 1983 to October 1985 covering two dry and two rainy periods. Bulk samples only were obtained. At the same site and period, fine, coarse and inhalable particles were also collected. Na⁺, Ca²⁺, K⁺, Mg²⁺, NO₃⁻, SO₄²⁻ and NH₄⁺ contents were determined in rainwater samples, while Na, Ca, K, Cl and S concentrations were measured in aerosol samples. Rainwater is slightly acid (mean pH = 5.0), and contains high concentrations of Ca²⁺, NO₃⁻, SO₄²⁻ and NH₄⁺. Dry and wet fluxes and washout ratios were determined for some elements. Results obtained suggest that the atmospheric composition in this city is strongly influenced by anthropogenic sources.     

An analysis of precipitation chemistry measurements in Shimane,Japan

In order to understand the concentration and deposition levels of the major ions in Shimane, on the Japan Sea coast where precipitation chemistry data are scarce, the precipitation was collected at three sites (Matsue, Gotsu and Masuda) from April 1985 to March 1988.The mean precipitation chemistry was very close to each other except for the seasalt concentration. Masuda showed a halved seasalt contribution compared with the other sites. The volume-weighted annual pH mean at each site ranged from 4.6 to 4.9. Nitrate to SO₄⁻² equivalent ratios were in the range of 0.2 and 0.4 throughout the year. Ammonia and calcium species are interpreted to have neutralized approximately 70% of the original sulfuric and nitric acids.The annual depositions of the major ions in g m⁻²y⁻¹ were as follows: H⁺; 0.023–0.037, NH₄⁺; 0.57–0.68, Ca²⁺; 0.51–0.92, SO₄²⁻; 3.29–5.04, NO₃⁻; 1.20–1.70. These levels are of the same intensity as corresponding values of JEA network results.     

Chemical characterization of acid precipitation in Albany,New York

Chemical composition of precipitation in Albany, NY from July 1986 to December 1988 has been studied. Mean volume-weighted concentrations (μeq^ℓ−1) were: acidity, 104.0; alkalinity, −63.7; SO₄²⁻, 52.8; NO₃⁻, 29.8; Cl⁻, 5.6; F⁻, 0.50; NH₄⁺, 19.3; Ca²⁺, 6.5; Mg²⁺, 2.8; Na⁺, 3.5; and K⁺, 1.4. Mean pH was 4.2 . Seasonal patterns were pronounced for most species. Concentrations of H⁺, SO₄²⁻, NO₃⁻, NH₄⁺ and Ca²⁺ peaked in the summer and spring. Deposition was related to rainfall amount by a power law relationship in which the exponent of the equation was ∮.6. Wet SO₄²⁻ deposition was 2.35 keq ha⁻¹ over a 30-month period. The SO₄²⁻ and NO₃⁻ deposition rates observed at Albany indicate that transport from midwestern sources have a major influence at this site. On the average, free H⁺ ion concentrations determined from pH measurements accounted for 51% of the measured total acidity. There were unknown species, most likely organic acids, that could contribute to the acidity. Correlation and regression analyses indicated that major anions, SO₄²⁻ and NO₃⁻, were closely associated with H⁺ and NH₄⁺ ions. Factor analysis revealed four common factors which are related to fossil-fuel combustion, sea spray, cement factory and biomass burning.     

Cloud chemistry at Mt Rigi,Switzerland: Dependence on drop size and relationship to precipitation chemistry

The chemical composition of winter and spring cloud water sampled at 1620 masl elevation on Mt Rigi in central Switzerland was dominated by NO₃⁻, SO₄²⁻, NH₄⁺ and H⁺. A wide range of concentration levels was observed, with maxima of 3700, 1800 and 4600 micronormal for NO₃⁻, SO₄²⁻ and NH₄⁺, respectively. Concentrations at a lower elevation (1030 masl) site on the mountain were higher due to lower cloud liquid water contents and higher pollutant levels at that site. The lowest pH observed was 2.95; large concentrations of NH₃ in the region prevented pH values from falling even lower. A comparison of simultaneously sampled cloud water and precipitation revealed much higher concentrations for most species in the cloud water, except in one case of extreme precipitation riming when the concentrations in the two phases converged. An exception to the pattern was H⁺; at times the precipitation was more acidic than the cloud water. The chemical composition of the cloud drops varied with drop size. Drops smaller than 10 μm diameter were enriched in NO₃⁻, SO₄²⁻ and NH₄⁺ relative to larger drops. Since the larger drops are the ones most effeciently captured by snow crystals, knowledge of their composition is essential to understanding the chemical implications of accretional growth of precipitation.     

A paired comparison of two precipitation chemistry sites in East-Central Mississipi

A paired comparison was performed on 2 years of precipitation chemistry data from Meridian and Newton, MS. The Meridian site is in violation of several National Atmospheric Deposition Program siting criteria, whereas the Newton site, 35 km west, is mostly in compliance. The two sites are compared through the use of volume-weighted means, deposition, logarithmic distributions, boxplots, paired t-tests, the nonparametric Wilcoxon test, and a form of linear regression analysis that accounts for cases in which both populations are subject to error. Results indicate Meridian has higher concentrations of all measured ions except NH₄⁺. Elevated NH₄⁺ concentrations at Newton are most likely due to the location of the site in a cattle pasture. Significant differences (95% confidence level) were found for Cl⁻, Na⁺, K⁺, Ca²⁺ and Mg²⁺. SO₄²⁻ was found to be borderline significant.     

Aerosol characteristics of Arctic haze sampled during AGASP-II

As part of the second Arctic Gas and Aerosol Sampling Program (AGASP-II), Arctic aerosol samples were collected by the NOAA WP-3D aircraft in spring 1986. The samples were analyzed in bulk and individual-particle form, using ion chromatography (IC) and electron microscopy (EM), respectively. Information on the chemical composition of the aerosol as determined by various techniques is presented, as well as morphology, concentration, and size distribution data obtained from individual particle analyses. For most flights, a stratospheric sample and a haze profile samople were collected. Haze samples exhibited greater particle concentrations than stratospheric samples, the highest concentrations in haze reaching ∼10³ cm⁻³ (non-volatile particles > 0.05 μm diam). Sulfur was consistently observed to be a major element in both large and small particles in haze samples. Crustal elements such as Si, Al, K, Ca and Fe were often present in significant concentrations together with S. Particles that did not emit X-rays, possibly organic or sooty C, were observed in significant concentrations in both tropospheric and stratospheric samples. Chemical spot tests confirmed that SO₄²⁻ was the major S-containing species and that NO₃⁻ was not nearly as prevalent as SO₄²⁻ in the Arctic aerosol particles. The mass concentrations of major anions (Cl⁻, SO₄²⁻ and NO₃⁻) and cations (Na⁺, K⁺, NH₄⁺, Ca²⁺ and Mg²⁺) in the bulk aerosols were determined using IC. The ratios between ion concentrations, e.g. Ca²⁺/Na⁺, SO₄²⁻/Na⁺ and Cl⁻/Na⁺, may serve as indicators of aerosol origins and mixing status of various air masses. Aerosols collected on six flights demonstrated variability of particle characteristics in relation to sources and transport of Arctic haze.     

Ionic composition of submicron particles (PM1.0) during the long-lasting haze period in January 2013 in Wuhan, central China

In January 2013, a long-lasting severe haze episode occurred in Northern and Central China; at its maximum, it covered a land area of approximately 1.4 million km². In Wuhan, the largest city in Central China, this event was the most severe haze episode in the 21st century. Aerosol samples of submicron particles (PM_1.0) were collected during the long-lasting haze episode at an urban site and a suburban site in Wuhan to investigate the ion characteristics of PM_1.0 in this area. The mass concentrations of PM_1.0 and its water-soluble inorganic ions (WSIIs) were almost at the same levels at two sites, which indicates that PM_1.0 pollution occurs on a regional scale in Wuhan. WSIIs (Na⁺, NH₄⁺, K⁺, Mg²⁺, Ca²⁺, Cl^-, NO₃^- and SO₄^2-) were the dominant chemical species and constituted up to 48.4% and 47.4% of PM_1.0 at WD and TH, respectively. The concentrations of PM_1.0 and WSIIs on haze days were approximately two times higher than on normal days. The ion balance calculations indicate that the particles were more acidic on haze days than on normal days. The results of the back trajectory analysis imply that the high concentrations of PM_1.0 and its water-soluble inorganic ions may be caused by stagnant weather conditions in Wuhan.     

Rainwater composition in Athens,Greece

Wet precipitation-only samplers were used to collect wet deposition at two sites in the Athens basin, Greece for the period March 1986–February 1987.Concentrations of major cations (H⁺, NH⁺₄, Na⁺, K⁺, Ca²⁺ and Mg²⁺) and major anions (Cl⁻, NO⁻₃ and SO²⁻₄) were determined for the first time in rainwater samples in Greece. Bicarbonate concentrations were calculated. The relative importance of natural and anthropogenic sources were estimated by a chemical balance. The majority of rain collected has a neutral or alkaline character. Acidity was due to the presence of H₂SO₄ and HNO₃. The statistical analysis of the correlation between the concentration of chemical species confirm the influence of natural and anthropogenic sources. In all samples, SO²⁻₄ concentrations exceed NO⁻₃ concentrations despite the dominance of low S oil burning in the region. The wet flux of S was calculatd to be 0.34 gm⁻²a⁻¹.     

Chemistry of atmospheric precipitation at the Western Arabian Gulf Coast

Rainwater and atmospheric bulk deposition samples were collected at a station on the rooftop of the Research Institute of King Fahd University of Petroleum and Minerals in Dhahran. Continuous sampling was carried out manually throughout the rainy season between December 1987 and February 1988, and for one rainfall event in March 1987. A total number of 13 samples were collected and investigated for pH and dissolved ionic composition using inductivity coupled plasma emission spectrometry (ICP) and ion chromatography (IC). The range and volume-weighted average pH were 5.1–7.2 and 5.48, respectively. Significant negative linear correlations were observed between the precipitation pH and rain depth, and between pH and the summation of dissolved {(Ca²⁺ + Mg²⁺)−(SO₄²⁻ + NO₃⁻ + NO₂⁻)} (in μeqℓ⁻¹). The ionic summation also correlated negatively with rain depth. The ionic abundance in rainwater (in μeqℓ⁻¹) expressed in concentration order showed the general trend SO₄²⁻ > HCO₃⁻¹ = Cl⁻ = NO₃⁻ > NO₂⁻ for anions and Ca²⁺ > Na⁺ > Mg²⁺ > NH₄⁺ > K⁺ > H⁺ > Sr²⁺ for cations. Good mass balance between cations and anions was observed. Total NO₃⁻ contribute equally to precipitation acidity as SO₄²⁻ and Ca²⁺ plus Mg²⁺ in alkaline suspended particulates from natural sources are the major ions which buffer the acidity of precipitation. The NH₄⁺ ion which is also present plays an insignificant role in the acid/base equilibrium of rainwater.     

西安市大气降水的主要化学组分及其来源

为认识西安市大气降水主要化学组分的现状,对2019年西安市市区和郊区大气降水样品的pH值、电导率、水溶性离子和重金属的质量浓度、湿沉降通量和来源进行了研究.结果表明,西安市冬季大气降水pH、电导率、水溶性离子和重金属浓度均高于其它季节.降水中主要的水溶性离子为Ca²⁺、 NH⁺₄、 SO■和NO^-₃,其之和占总离子浓度的(88.5±2.8)%;市区和郊区主要重金属是Zn和Fe、 Zn和Mn,其之和分别占总金属浓度的(54.0%±3)%和(47.0%±8)%.市区和郊区降水中水溶性离子的湿沉降通量分别为(253.2±58.4)mg·(m²·month)^-1和(241.9±61.1)mg·(m²·month)^-1,呈现出冬季高于其他季节的特点;重金属的湿沉降通量分别为(86.2±37.5)mg·(m²·month)^-1和(88.1±37.4)mg·(m...     

A comparison of two cloudwater/fogwater collectors: The rotating arm collector and the caltech active strand cloudwater collector

A side-by-side comparison of the Rotating Arm Collector (RAC) and the Caltech Active Strand Cloudwater Collector (CASCC) was conducted at an elevated coastal site near the eastern end of the Santa Barbara Channel in southern California. The CASCC was observed to collect cloudwater at rates of up to 8.5 ml min⁻¹. The ratio of cloudwater collection rates was found to be close to the theoretical prediction of 4.2:1 (CASCC:RAC) over a wide range of liquid water contents (LWC). At low LWC, however, this ratio climbed rapidly, possibly reflecting a predominance of small droplets under these conditions, coupled with a greater collection efficiency of small droplets by the CASCC. Cloudwater samples collected by the RAC had significantly higher concentrations of Na⁺, Ca²⁺, Mg²⁺ and Cl⁻ than those collected by the CASCC. These higher concentrations may be due to differences in the chemical composition of large vs small droplets. No significant differences were observed in concentrations of NO₃⁻, SO₄²⁻ or NH₄⁺ in samples collected by the two instruments.     

The research of below-cloud scavengingof rainwater in Guilin City

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不同类型建筑垃圾堆场大气降尘中水溶性离子污染特征

为了解建筑垃圾长期堆放产生的扬尘对大气的影响,选择北京市两个拆迁建筑垃圾堆放场,于2019年夏季、秋季进行降尘连续采样.共收集拆迁原地堆放有效降尘样品11个,异地集中堆放有效降尘样品11个,利用离子色谱法对大气降尘中水溶性离子组分及质量浓度进行分析.结果表明：阳离子中质量浓度最高的是Ca²⁺,其次是K⁺,NH₄⁺浓度最低;阴离子中质量浓度最高的是SO₄^2-,其次是Cl^-,NO₃^-最低,降尘样品呈碱性.建筑垃圾拆迁原地堆放场地Ca²⁺、Mg²⁺、SO₄^2-、Cl^-、Na⁺、NH₄⁺平均浓度高于异地集中堆放场地对应各离子浓度.拆迁原地堆放场地中Ca²⁺、SO₄^2-、Na⁺、Cl^-受局地风向影响较大,空间分布情况与风向扩散趋势大致相同;异地集中堆放场地各离子浓度高值区域分布较原地堆放远,Ca²⁺、K⁺、SO₄^2-、Cl^-、Mg²⁺这5种离子空间分布与次主导风向较为相符.同时,两个场地水溶性离子平均浓度与距建筑垃圾堆放地的距离有一定的关系,采样点在距堆放中心200 m范围之内离子平均浓度最大,总体来说,距离堆放中心近的采样点位离子浓度高于距离较远的采样点位离子浓度.     

北京市内到郊区氮沉降时空变化特征

对北京市区到远郊梯度带上的4个采样点(北京师范大学(BNU)、奥林匹克森林公园(AS)、减河公园(JH)、延庆上辛庄(YQ))降雨和针叶树穿透雨雨量及其化学成分进行了监测,分析了从市中心到远郊的氮沉降时空变化规律.结果表明:梯度带上各点铵态氮(NH+4-N)与硝态氮(NO-3-N)均为5、6月最大,7月开始迅速减小,雨季降雨的稀释作用是主要原因.在空间上,NH+4-N与NO-3-N沉降量大小为BNUJHASYQ,4个样点对应的可溶性无机氮(铵态氮与硝态氮)总沉降量分别为22.6、13.7、12.1、5.42 kg·hm~(-2)a-1(以N计).无机氮沉降以湿沉降为主,4个样点上湿沉降所占比例分别为BNU 72.44%、AS 65.97%、JH 62.78%、YQ 93.86%;沉降成分以铵态氮为主,所占比例分别为BNU56.41%、AS 59.47%、JH 61.21%、YQ 63.33%,从城区到远郊逐次增大.国内外同类研究综合表明,湿沉降中无机氮浓度均是工业区市区郊区远郊区,北京降雨中无机氮浓度相对较高.大多数研究区的城区与郊外大气氮沉降均是以铵态氮为主,与市区交通及生活源氮氧化物排放较高的实际并不一致,其成因与机制尚不明确.