Wet and dry depostion fluxes above the North Sea

A hyperbolic-dilution relationship exists between the dissolved metal concentrations in rain above sea and the precipitation volume. The real wet flux can then be expressed solely as a function of the hyperbolic regression coefficients, the precipitation volume and the number of rain events. Hyperbolic regression coefficients were determined during a restricted period of sampling during which all rain events were sampled and analyzed. In addition, measuring the annual precipitation volume above sea allowed us to estimate the annual wet deposition flux.Dry deposition fluxes at sea were (1) measured using vasilinated plexiplates and (2) calculated using a dry deposition model and cascade impactor results. Despite the large uncertainties on the calculated dry deposition fluxes, results obtained with both methods agree within a factor of 2.3. Resuspension fluxes of the trace metals are negligible compared to the deposition fluxes.     

Atmospheric sulphur deposition to forest stands: Throughfall estimates compared to estimates from inference

Wet and dry deposition of sulphur was estimated for 30 forest stands in the Netherlands using a throughfall method and an inferential method. Dry deposition estimates of the throughfall method were significantly higher compared to estimates from inference. The major sources of uncertainty of the throughfall dry deposition estimates were associated with non-representative throughfall sampling, wet deposition estimates, canopy exchange processes, deposition of neutral salts, dry deposition directly onto the throughfall collectors, and with the omission of stemflow fluxes and dry deposition directly to the undergrowth vegetation and forest floor. These uncertainties were found to act both ways to approximately the same extent and were not able to explain the observed gap between the two dry deposition estimates. For the inferential method, major sources of uncertainty in the dry deposition estimates arose in calculation of the dry deposition velocity of SO₂ and the omission of occult deposition of SO₄²⁻. In this study, uncertainties associated with the spatial averaging of air concentrations of SO₂ and SO₄ aerosol and the calculation of the deposition velocity of SO₄ aerosol were found to be relatively small. Modifying the R_c parametrization of SO₂, based on recent dry deposition measurements made over heather in the Netherlands, resulted in fairly good agreement between both dry deposition estimates. Occult deposition of SO₄²⁻ was found to contribute significantly to the total sulphur deposition to the forest stands. Both the modified R_c parametrization and the incorporation of occult deposition led to systematically higher sulphur deposition estimates by the inferential method compared to originally inferred deposition. This implies that in the Netherlands, sulphur deposition to forest ecosystems might have been underestimated heretofore.     

Monitoring the dry deposition of SO2 in the Netherlands: Results for grassland and heather vegetation

An automated system based on the micrometeorological gradient technique has been developed to measure the dry deposition of SO₂ on a routine basis. Measurements were made at two locations in the Netherlands. From these results dry deposition fluxes, dry deposition velocities and surface resistances for a heathland and for an agricultural grassland site were estimated using a selected set of data and a calculation procedure based on micrometeorological considerations. An extensive analysis was made to determine uncertainties in the resulting deposition parameters. From this analysis it has been concluded that the uncertainty in these parameters is almost completely determined by the random errors in measured concentrations. The meteorological surface exchange parameters can be estimated sufficiently accurately (<20% uncertainty). At the grassland site, average surface resistances to deposition of 6(±8) and 13(±12) s m⁻¹ were calculated for wet and dry conditions, respectively. At the heathland site, a similar distinct difference between R_c values for wet and dry conditions was found. These values are 20(±21) and 70(±90) s m⁻¹, respectively. The yearly average dry deposition flux for SO₂ at the grassland site amounts to 585(±330) mol ha⁻¹ yr⁻¹, while at the heathland site the yearly average flux was 300(±270) mol ha⁻¹ yr⁻¹. The yearly average dry deposition velocity at 4 m height was 1.2(±0.3) cm s⁻¹ at the grassland site and 0.8(±0.4) cm s⁻¹ at the heathland site.     

戴云山国家级自然保护区大气氮沉降特点

利用干湿沉降采集器,持续观测戴云山国家级自然保护区内大气氮素干、湿沉降,调查当地大气氮沉降的种类和沉降通量.结果表明,2015-03-27~2015-10-09观测期间,戴云山自然保护区大气氮干、湿沉降量分别为2.30 kg·hm~(-2)和14.79kg·hm~(-2),以湿沉降形式为主(87%).干沉降中可溶性有机氮的沉降量为1.21 kg·hm~(-2),占干沉降通量的53%;无机氮以硝态氮为主(0.71 kg·hm~(-2)),铵态氮相对较低(0.37 kg·hm~(-2)).湿沉降中无机氮和可溶性有机氮沉降量分别为9.41 kg·hm~(-2)和5.38 kg·hm~(-2),其中无机氮以铵态氮为主(6.07 kg·hm~(-2)).大气氮湿沉降量和当地降雨量显著正相关,降雨量越大,对应的湿沉降氮量也越大.戴云山国家级自然保护区大气氮素沉降量较高,可能会对当地生态环境产生较大的影响.     

Nitrogen budget for eastern Canada

A Lagrangian model incorporating S and N chemistry has been developed by the Atmospheric Environment Service. It was used to produce an annual nitrogen budget including annual nitrogen transboundary flux estimates for 1980 for eastern Canada.The model used trajectories computed from the analyzed winds produced at the Canadian Meteorological Centre (CMC) in addition to the temperature and precipitation analyses. The model parameterized the dry and wet deposition and chemical transformation of NO₂, nitrate (including HNO₃) and PAN using monthly, time-dependent dry deposition velocities, scavenging ratios and transformation rates. The model was integrated throughout eastern Canada on a 6-h basis for 1980. The boundary point concentrations were used to compute input and output fluxes which were summed over several boundary segments to give annual transboundary flux estimates.The total annual N deposition was about 0.6 TgN with high deposition in August and December and the lowest in February. Wet NO₃⁻ deposition (0.2 TgN) was higher than the dry deposition of any single N species (NO₂, nitrate or PAN) but lower than all dry N deposition combined. The annual N input (output) flux was about 1.0 (0.5) TgN. The highest input and output fluxes occurred in December and the lowest input and output fluxes occurred in May.     

Comparability and precision of MAP3S and NADP/NTN precipitation chemistry data at an acidic site in eastern North America

Precipitation chemistry data derived from more than six years of concurrent sampling under the MAP3S and NADP/NTN protocols at the Penn State site in rural Pennsylvania are compared. Preprocessing of the data (sample and gage depths, concentrations of H₃O⁺, SO₄²⁻, NO₃⁻, NH₄⁺) included aggregating the event and daily MAP3S data into weekly averages that coincide with the weekly data of the NADP/NTN program. A simple statistical model was applied to the differences of the paired data to look for systematic biases between the networks. The most notable bias occurred for ammonium concentration (NADP/NTN low), a finding consistent with other studies. A minor, but statistically significant, bias was also found for sulfate coccentration (NADP/NTN high). Both the ammonium and sulfate biases may be related to the relatively long time that the NADP/NTN samples remain in the field, thus strengthening arguments in favor of daily sampling protocols. The hydronium and nitrate concentrations exhibited remarkably high levels of comparability between the daily and weekly protocols. Overall, the data from the MAP3S and NADP/NTN networks are comparable, with the possible exception of ammonium, for some applications. The field results from about two years of duplicate sampling under the MAP3S protocol demonstrate that measurement precisions of only a few percent are possible when the protocol is consistently followed and the equipment is well maintained.     

三峡库区大气活性氮组成及干沉降通量

为了解三峡库区腹地大气中活性氮的组成及干沉降通量,于2015年每个季节选取代表性月份在万州城区采集了气体和颗粒物样品.利用离子色谱法测定氮素浓度,同时结合大叶阻力模型模拟计算的干沉降速率值,估算了不同形态氮素的干沉降通量.结果表明,HNO₃的干沉降速率值最大,年均值为0.39cm/s,约为其它氮素的3~8倍.NO₂和NH₃是大气活性氮的主要赋存形态,年均浓度值分别为（11.7±3.9）和（11.0±5.3）μg N/m³,两者之和约占总无机氮浓度的80%.万州城区总无机氮干沉降总量为8.5kg N/（hm²·a）,其中氧化态氮（NO₂、HNO₃、颗粒态NO₃^-）和还原态氮（NH₃、颗粒态NH₄⁺）干沉降通量分别为3.5,5.0kg N/（hm²·a）,占干沉降总量的41.4%和58.6%.因此,为有效控制三峡库区腹地的氮素污染,应重点关注NH₃的减排.     

Atmospheric dry deposition flux of metallic species to the North Sea

Air sampling on a series of 10 research cruises on the North Sea (south of 56°N) has yielded detailed spatial distributions of atmospheric metal concentrations, Al, Ca, Cd, Cu, Fe, Mg, Na, Pb and Zn which closely parallel the results of earlier published models. Air mass back trajectory analysis demonstrates the strong influence which source region may have upon the elemental composition of the North Sea atmosphere. A cascade impactor designed to collect efficiently large as well as small aerosol has produced detailed size distributions from which mass weighted deposition velocity estimates have been produced (Al, 0.33; Cd, 0.24; Cu, 0.44; Fe, 0.30; Pb, 0.13; Zn, 0.30 cm s⁻¹) enabling estimates for the dry deposition flux to the study area to be made. Extrapolation of these data to the whole of the North Sea yields dry deposition flux estimates (Cd, 33; Cu, 350; Pb, 370; Zn, 2640 tonnes yr⁻¹) which are in some instances substantially lower than those previously reported, but nevertheless represent a significant pathway for metallic species to enter this marine environment. The size distributions show the clear dominance that large aerosol has upon the overall dry deposition flux. Flux estimates are thus highly sensitive to the sampling of this large aerosol component, and to assumptions made regarding the sea surface as a source of giant trace metal-enriched particles which act only as a means of recycling marine metals.     

Measurements of wet and dry deposition at an urban location in India

Wet and dry depositions were collected in Pune city using 24-h and weekly sampling periods, respectively, from January 1984 to December 1988. All the wet and dry deposition samples were analysed for major cations and anions along with pH. Dry depositions were minimum in the monsoon season and maximum in the winter season though there was no significant difference in pH values. The wet deposition of all ionic components was found to be higher than the dry deposition. The depositions of the ionic components from natural sources (soil and sea) were higher than those from anthropogenic sources. The dry deposition velocities of the aerosols were found to be increasing with increase of their mass median diameters. The chemical composition of the dry deposition at Pune indicated maximum depositions of the alkaline substances, which are the main cause for the alkaline pH of rain water. Results of the present study have suggested that the atmospheric composition in the city is strongly influenced by natural sources rather than anthropogenic.     

Characterization of pollen deposition in a forest environment

Measurements of the dry deposition of pollen were made during the months of May and June 1987 in northern Wisconsin, using a smooth surrogate surface. Samples were taken on a raft located on Little Rock Lake and at a nearby field monitoring station. Rain samples were also collected at the field station. The wet SO₄²⁻ flux was 102.7 mg m⁻², compared with a dry SO₄²⁻ flux of 118 mg m⁻² at the field monitoring site and 45 mg m⁻² at the lake site.The SO₄²⁻ content of pollen ranged from 0.2 to 0.8% of the weight of the pollen, and NO₃⁻ concentrations were an order of magnitude lower. Between 9 and 22% of the pollen weight was available as total organic carbon (TOC) upon addition to water.The addition of pollen to distilled water produced an acid reaction, due to organic acids and not inorganic acidity.     

被动采样法表征降水离子浓度和通量的局限性

降水(湿沉降)是大气污染物进入地表环境的主要途径,由于传统的被动采样法易受到颗粒物和气体干沉降的干扰,而采集到的混合沉降样品不能科学表征降水化学组成,也不能准确量化湿沉降通量,因此目前正逐步被主动采样法所取代. 采用主动和被动2种采样法同步采集了降水样品,以考察被动采样法表征降水离子浓度和通量的适用性. 结果表明:被动采样法采集的降水样品中离子浓度明显偏高,其中ρ(NO₃-)、ρ(Mg2+)、ρ(Ca2+)、ρ(K+)、ρ(Cl-)、ρ(SO₄2-)、ρ(Na+)和ρ(NH₄+)分别比主动采样法高65%、58%、43%、41%、35%、26%、10%和9%. 受大气污染物干沉降影响,被动采样法获得的NO₃-、NH₄+和SO₄2-混合沉降通量分别比主动采样法获得的湿沉降通量高79%、18%和35%,差异最显著的是NO₃-. 被动采样法可以收集氮和硫的湿沉降,但不能有效捕获二者以颗粒物和气体形式发生的干沉降,对二者沉降总通量(干沉降通量+湿沉降通量)低估达39%〔23 kg/(hm2·a)〕和40%〔20 kg/(hm2·a)〕. 因此,鉴于大气污染形势日趋严重,污染物的干沉降作用凸显,被动采样法已难以准确测算污染物从大气向地表的沉降总通量,需要全面考虑细颗粒物(粒径≤2.5 μm)和气态物种(如HNO₃)的贡献.      

大气氮沉降向典型红壤区农田生态系统定量输入研究

在2005年,通过对中国科学院红壤生态实验站(江西鹰潭)内农田小气候要素和湍流的观测及大气和雨水中氮化物的分析,借助大叶阻力相似模型,研究了大气氮素(N)通过干、湿沉降输入研究地农田生态系统的N通量.结果表明,全年通过大气沉降向该农田生态系统输入N 132.6 kg.hm-2,其中干沉降输入N 82.63 kg.hm-2,占大气总输入N的67.94%.干沉降过程中,气体中以NH3-N沉降为主,占气态N沉降的43.02%~89.89%(均值为71.05%);颗粒中以NO3--N为主,占颗粒态N的33.67%~94.54%(均值为61.01%).每月通过湿沉降(雨水)输入N 0.50~8.45 kg.hm-2,以7月和11月较高.     

Deposition and forest canopy interactions of airborne sulfur: Results from the integrated forest study

The Integrated Forest Study (IFS) was a long-term research project designed to determine the effects of atmospheric deposition on forest nutrient cycles. Concentrations and fluxes of airborne sulfur compounds were determined for several years at the 13 IFS research forests in North America and Europe using a standard set of protocols. Annual mean air concentrations of sulfur ranged from ∼1.5 to 8 μgSm⁻³ and were generally dominated by SO₂ (∼60% of total sulfur on the average). Atmospheric deposition of sulfate at these forests was highest at the high elevation (∼ 1000–2000 eq ha⁻¹yr⁻¹) and at the southeastern U.S. sites (∼800–1000 eq ha⁻¹yr⁻¹), and lowest in the Pacific northwest (∼300 eq ha⁻¹yr⁻¹). Cloud water contributed significantly to the sulfur flux at the mountain sites (45–50%), and dry deposition was comparable to wet at the drier southeastern sites (>40% of total). Deposited sulfur appeared to behave more or less conservatively in these canopies, showing little net uptake (ofSO₂) and minor foliar leaching (of soil-derived, internal SO₄²⁻) relative to the total atmospheric flux. The estimated fluxes in total deposition were generally within 15% of the measured fluxes in throughfall plus stemflow, indicating that useful estimates of total atmospheric deposition of sulfur can be derived from measurements of throughfall.     

Tests of the use of net throughfall sulfate to estimate dry and occult sulfur deposition

Throughfall and stemflow measurements taken in a mature high elevation red spruce stand, and precipitation measurements made in a nearby clearing, were used to calculate weekly net throughfall (=throughfall + stemflow - precipitation) sulfate deposition and net throughfall volume in the stand over a 20-week period. The study fortuitously was divisible into a low cloudwater deposition period, during which precipitation volumes generally exceeded throughfall volumes, and a high cloud period, during which the reverse was true. Weekly cloudwater deposition volume was estimated independently from continuously recorded cloudwater collections by an artificial tree located on an elevated platform in the clearing. Weekly net throughfall volume correlated well with cloudwater deposition volume (r = +0.86). Precipitation accounted for only 25% of the throughfall sulfate collected throughout the study and only 15% of that collected during the high cloud period, as net throughfall sulfate was 2.4 times greater during the high cloud period than during the low cloud period. Weekly estimates of cloudwater sulfate deposition correlated well (r = +0.74) with measures of net throughfall sulfate during the high cloud period. Dry deposition models were used to estimate weekly dry S deposition; weekly estimates of the wash-off of this dry deposition also correlated well (r = +0.76) with net throughfall sulfate during the low cloud period. During the high cloud period, estimates of cloudwater S plus dry S deposition accounted for 67% of the sulfate collected in net throughfall; however, during the low cloud period only 55% of net throughfall sulfate was accounted for. The low percentage of sulfate accounted for during the low cloud period suggests that the dry models were underestimating S deposition. Possible reasons for underestimation include failure to consider fully topographic complexity and edge effects, underestimates of surface wetness, and the possibility of canopy sources of sulfate (foliar leaching). These results support the use of throughfall sulfate measurements as gross estimates of (1) total S deposition, (2) total dry S deposition (using net throughfall in environments where cloudwater deposition accounts for less than 5% of total sulfate deposition) and/or (3) total cloud S deposition (subtracting precipitation and dry inputs from total throughfall sulfate in high cloud environments).     

Atmospheric concentrations and deposition of nitrogen and major ions in conifer forests in the United States and Federal Republic of Germany

Emission densities of air pollutants are higher in Europe than in the U.S. as a whole, suggesting similar differences in atmospheric deposition. We determined air concentrations and deposition during the warm season at conifer forests in Tennessee and northern Germany. Our results confirmed major differences in both chemistry and fluxes. Atmospheric and precipitation concentrations of all ions except H⁺ were higher at the German site, most significantly for the nitrogen species. The much higher levels of NH₄⁺ at this site reflect higher emissions of NH₃, which was the species largely responsible for the lower levels of H⁺. Total airborne nitrate was dominated by HNO₃ in Tennessee. In Germany we found comparable amounts of HNO₃ and aerosol NO₃⁻, the concentration of which varied seasonally, apparently in response to agricultural emissions of NH₃ that reacted to form NH₄NO₃. Total deposition of all major ions was much higher at the German site, particularly for the nitrogen species, which exhibited a marked edge effect in throughfall. Dry deposition was determined from air concentrations by using a canopy resistance model and from a statistical model of throughfall fluxes, each of which yielded comparable fluxes for several ions. Dry deposition contributed 10–70% of the ion input and was most important at the German site. Both forest canopies absorbed 40–50% of total deposited nitrogen, primarily from dry deposition.     

珠江三角洲秋季臭氧干沉降特征的数值模拟

利用区域化学传输模式WRF-Chem对2014年10月珠江三角洲臭氧干沉降特征进行模拟,结果表明：臭氧干沉降通量呈现明显的时空分布差异,日间平均沉降通量[0.68μg/（m²·s）]明显大于夜间[0.21μg/（m²·s）];同时,珠江三角洲城区的臭氧沉降通量及日较差均比周边植被覆盖区小.受NO_x和VOCs等前体物以及各气象要素场的综合影响,臭氧浓度日变化具有明显的单峰型分布特征,在14：00~15：00达到峰值,秋季臭氧浓度高值区位于珠江三角洲主要排放源下风向区域的广佛交界、江门及中山东部等地区;臭氧的干沉降速率也具有明显的时空变化特征：从07：00~08：00的0.27cm/s开始迅速增大,10：00~16：00基本保持在0.60cm/s左右,17：00开始平缓减小至午夜的0.21cm/s左右;干沉降速率的变化主要受空气动力学阻抗R_a、粘性副层阻抗R_b以及表面阻抗R_c影响,研究表明夜间的干沉降速率主要受R_a影响,而日间R_c起主要作用.这3种阻抗分别受大气稳定度、摩擦速度和下垫面土地利用类型影响,在珠江三角洲区域亦表现出明显的时空变化特征.     

上海市大气沉降物中多环芳烃赋存特征及其来源

以上海市大气沉降为研究对象,采集了上海市8月、9月、10月3个月的大气沉降物,分析了上海市大气沉降物中16种PAHs的质量浓度、空间分布特征和组成结构,计算了上海市8个采样点∑15PAHs大气沉降物通量.同时,采用正定矩阵因子分解(PMF)模型对大气沉降中的PAHs进行源解析,模型对PAHs的来源有较为细致的判读,结果表明:大气沉降物中∑16PAHs的浓度范围0.458~21.013μg/L,其中,溶解相中∑16PAHs的浓度范围为0.174~0.625μg/L,颗粒相中∑16PAHs的浓度范围为0.275 20.455μg/L.上海市∑15PAHs大气沉降通量在0.24~14.74μg/(m2×d)之间,沉降通量均值为2.77μg/(m2×d).根据PMF模型解析,机动车尾气排放为大气沉降物中PAHs的主要污染物,源贡献率为40.23%,其次,居民烹调、煤炭燃烧、石油挥发泄露和炼焦排放依次占23.73%、14.75%、14.35%和6.92%.     

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.     

沙尘和灰霾期间中国近海大气氮沉降通量估算

利用WRF-CMAQ模型估算了2011年4月26日~5月3日沙尘事件和2016年1月1日~7日灰霾事件在中国近海引起的总无机氮（TIN）沉降通量,分析了两类事件对中国近海海洋初级生产力的贡献,探究了灰霾事件时中国近海无机氮沉降的可能来源.结果表明：典型沙尘和灰霾过程中,中国近海TIN干沉降通量均值分别为6.77,3.01mg N/（m²·d）,是晴朗天的6.84,3.04倍,可提供38.5,17.1mg C/（m²·d）的海洋初级生产力;沙尘期间无机氮沉降以还原态氮（NH₃和铵态氮,占TIN的62.2%）为主,灰霾期间则以氧化态氮（HNO₃和硝态氮,占TIN的84.3%）为主.典型沙尘事件TIN沉降对黄海影响最大,对渤海影响最小;典型灰霾事件对黄海和东海TIN沉降影响相当,高于对渤海的贡献.典型灰霾期间,京津冀和山东西北部（区域一）对渤、黄、东海TIN干沉降的贡献均大于长江三角洲及周边地区（区域二）,区域一对3个海域TIN干沉降的贡献约为38.7%~74.6%,区域二的贡献约为1.14%~12.1%.     

Dry deposition inferential measurement techniques—I. Design and tests of a prototype meteorological and chemical system for determining dry deposition

A simple filterpack system and a supporting meteorological and surface-condition monitoring system have been deployed in a trial network to test methods by which dry deposition rates can be estimated on a routine basis, using average air concentration data and site-specific deposition velocities. The filterpack used in this dry deposition inferential measurement (DDIM) sampler differs from standard filterpacks by the use of a heated horizontal settling tube at the inlet. This modification is intended to protect the SO₂ sampling system from adverse effects associated with filter liquefaction at high humidities, while at the same time providing a simple means for eliminating large particles from the sampled air. Tests indicate that the sampler works well for SO₂ and for particulate species, and that HNO₃ concentrations are underestimated by about 25%. The DDIM approach differs from previous network measurement programs in that the data sets are designed to permit extension from observations at a subset of research sites to less intensive routine measurement sites. Hence a major goal is the definition of a suitable set of supporting data from which dry deposition rates can be inferred using air concentration data. Local vegetation characteristics are noted. At present, the additional variables that are monitored are solar radiation, wind speed, wind direction standard deviation, temperature, humidity, surface wetness, and precipitation. Observers report changes in the surrounding surface, such as the presence of snow or unusual drought.