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.     

辽宁省大气湿沉降化学特征分析

通过分析降水酸度、化学特征和湿沉降量等酸沉降控制指标,得出2009年辽宁省大气湿沉降化学特征。研究发现,辽宁省总体上酸雨污染并不严重,但区域性污染突出;降水化学污染严重,呈地域分布不平衡特征,重污染城市位于辽宁省西部和中部;湿沉降量的空间分布与降水化学污染不同,沉降量大的城市位于东部和南部沿海,所有离子湿沉降量最大值均出现在夏季。     

2009-2018年太湖大气湿沉降氮磷特征对比研究

为了研究太湖2009-2018年大气湿沉降的时空变化特征,于2009年8月-2010年7月及2017年8月-2018年7月进行了两次环太湖大气湿沉降逐月调查,并从降水中ρ（TN）和ρ（TP）、湿沉降率及沉降通量三方面,对比分析了太湖大气湿沉降的时空变化特征.结果表明:①2009年8月-2010年7月降水中ρ（TN）、ρ（TP）平均值分别为3.170、0.077 mg/L;2017年8月-2018年7月降水中ρ（TN）、ρ（TP）平均值分别为3.160、0.056 mg/L;T检验结果表明,两次调查ρ（TN）、ρ（TP）污染水平差异显著,主要是由于2017年8月-2018年7月较高污染浓度降水事件的减少,全年降水中ρ（TN）、ρ（TP）变异较小.②与2017年8月-2018年7月相比,2009年8月-2010年7月太湖TN、TP湿沉降率平均值分别下降33%和53%,且TN、TP湿沉降空间分布更均匀.③与2009年8月-2010年7月相比,2017年8月-2018年7月太湖流域大气TN、TP沉降通量分别为7 641和131 t,分别下降30%、47%.研究显示,两次调查降水中ρ（TN）平均值均远高于水体富营养化阈值（0.2 mg/L）,因此大气湿沉降中的营养盐对太湖富营养化的贡献不可忽视.      

陕北黄土高原239+240Pu大气湿沉降历史重建

重建Pu同位素的大气沉降历史是开展Pu示踪应用以及核事故安全评价的重要基础。本研究根据东京年降水量和^239+240Pu年大气沉降数据,并结合经验模型对陕北黄土高原^239+240Pu年湿沉降通量进行初探。结果表明,1957~2005年间研究区^239+240Pu年湿沉降通量在0.000 2~4.116 7 Bq/m²之间,累计湿沉降通量为14.08 Bq/m²;通过与周边土壤剖面的Pu总量对比发现陕北黄土高原Pu同位素的干湿沉降比为1左右。在时间变化上,上世纪60年代初全球大规模核试验导致研究区1963年^239+240Pu湿沉降通量出现峰值,1964~2000年Pu湿沉降通量呈明显减小趋势,2001~2005年亚洲粉尘的地表再悬浮过程使得^239+240Pu年湿沉降通量有所增加。     

九龙江流域大气氮湿沉降研究

通过2004～2005年对位于我国东南沿海的九龙江流域及周边共17个站点的实地观测,运用GIS技术定量揭示了大气氮湿沉降强度和时空分布特征,并利用氮稳定同位素分析雨水硝态氮的主要来源.结果表明,①17个站点雨水总氮平均浓度为(2.20±1.69)～(3.26±1.37) mg·L-1(以N计,下同),铵态氮、硝态氮和有机氮分别占39%、25%和36%;②雨水氮浓度随降雨强度的增大呈降低趋势,旱季浓度明显大于雨季,降水对大气具有清洗作用;③低δ15N值表明雨水硝态氮主要来源于汽车尾气排放、化石燃料燃烧和化肥施用;④九龙江流域大气氮湿沉降量平均9.9 kg·hm-2,春夏2季约占全年的91%,大气氮湿沉降占沉降总量的66%,揭示了该地区1∶2的大气氮干湿沉降结构.大气氮湿沉降时空差异与降雨量和氮的排放直接相关.     

京蒙沙源区水库大气氮沉降变化特征及源解析

以京蒙沙源区大河口水库为研究对象,于2017年1月~12月对水库周围布设的12个大气沉降监测站点收集样品144个,测定大气干、湿沉降物中TN浓度,计算大气总氮干、湿沉降通量,分析大气TN干、湿沉降污染特征及季节性变化特征.另选取水库周边不同典型地块,布设14个采样点采集样品76个,测定土壤δ¹⁵N-TN含量水平,解析水库大气氮沉降主要来源,并借助HYSPLIT4气团后向轨迹模型分析各季节不同类型气团输移营养盐对大河口水库的影响.结果表明：水库全年大气TN干沉降通量变化范围为122.44~425.64kg/（km²·month）,平均值为200.83kg/（km²·month）;湿沉降通量变化范围1.23~188.89kg/（km²·month）,平均值为66.33kg/（km²·month）.大气总氮年沉降通量为3205.9kg/（km²·a）,约为全国氮沉降平均水平（790kg/（km²·a））的4.06倍.从沉降类型上来看,大气沉降主要以干沉降为主,占沉降总量的75.17%,湿沉降占总沉降通量的24.83%.大气氮干沉降通量表现为春、秋季节明显高于夏、冬季节,湿沉降通量春、夏季明显高于秋、冬季节的季节性变化规律.通过对典型地块δ¹⁵N-TN同位素数据分析,表明夏季有71.4%的大气沉降样品来源于不可分辨的混合源输入,春、秋、冬季大河口水库超过45%的样品来源于沙地,另一大污染源为研究区周围的耕地.运用HYSPLIT4后向轨迹模型证明,从蒙古国入境的气团对研究区污染物大气输移影响较大,冬季采暖期间的大气污染和春季频繁发生的沙尘暴是造成北方沙区水体春季水环境变差的因素之一.     

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.      

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%.     

Fluxes of CH4 and N2O from soil under a tropical seasonal rain forest in Xishuangbanna, Southwest China

CH4 and N2O fluxes from soil under a tropical seasonal rain forest in Xishuangbanna, Southwest China were measured for one year using closed static chamber technique and gas chromatography method. Three treatments were set in the studied field: (A) litter-free,(B) with litter, and (C) with litter and seedling. The results showed that the soil in our study was a sink of atmospheric CH4 and source of atmospheric N2O. The observed mean CH4 fluxes from treatments A, B, and C were -50.0±4.0, -35.9±2.8,-31.6±2.8 μgC/(m2·h),respectively,and calculated annual fluxes in2003 were -4.1,-3.1,and -2.9kgC/hm2,respectively.The observed mean N2O fluxes from treatments A,B,and C were 30.9±3.1,28.2±3.5,50.2±3.7μgN/(m2·h),respectively,and calculated annual fluxes in 2003 were 2.8, 2.6, and 3.7 kgN/hm2, respectively. Seasonal variations in CH4 and N2O fluxes were significant among all the three treatments. The presence of litter decreased CH4 uptake during wet season (P ＜ 0.05), but not during dry season. There was a similar increase in seedlings-mediated N2O emissions during wet and dry seasons, indicating that seedlings increased N2O emission in both seasons. A strong positive relationship existed between CH4 fluxes and soil moisture for all the three treatments, and weak relationship between CH4 fluxes and soil temperature for treatment B and treatment C. The N2O fluxes correlated with soil temperature for all the three treatments.     

Nitrogen sink in a small forested watershed of subtropical China

Global nitrogen (N) emission and deposition have been increased rapidly due to massive mobilization of N which may have longreaching impacts on ecosystems. Many agricultural and forest ecosystems have been identified as secondary N sources. In the present study, the input-output budget of inorganic N in a small forested watershed of subtropical China was investigated. Inorganic N wet deposition and discharge by stream water were monitored from March, 2007 to February, 2009. The concentrations and fluxes of inorganic N in wet precipitation and stream water and net retention of N were calculated. Global N input by dry deposition and biological fixation and N output by denitrification for forested watersheds elsewhere were reported as references to evaluate whether the studied forested watershed is a source or a sink for N. The results show that the inorganic N output by the stream water is mainly caused by NO3??-N even though the input is dominated by NH4 +-N. The mean flux of inorganic N input by wet precipitation and output by stream water is 1.672 and 0.537 g N/(m2 yr), respectively, which indicates that most of inorganic N input is retained in the forested watershed. Net retention of inorganic N reaches 1.135 g N/(m2 yr) considering wet precipitation as the main input and stream water as the main output. If N input by dry deposition and biological fixation and output by denitrification are taken into account, this subtropical forested watershed currently acts as a considerable sink for N, with a net sink ranging from 1.309 to 1.913 g N/(m2 yr) which may enhance carbon sequestration of the terrestrial ecosystem.     

常德市酸雨化学特征、趋势分析及控制对策

常德市是中南地区酸雨污染最为严重的城市之一。以常德市2004年至2006年的降雨连续监测数据为基础,应用统计学相关分析的方法,对常德市158次降雨的变化特征进行了分析和研究。结果表明,常德市降雨酸度呈波动性变化,近3年的降雨pH年均值都在5．4以下,对降雨中离子含量的分析可知,酸雨主要为硫酸型,有向硫酸和硝酸混合型转化的趋势。降雨中的主要离子浓度和通量在冬、春季节高于夏、秋季节,降雨中阴阳离子极不平衡,[SO4^2-]和[Ca^2＋]浓度对降雨离子的平衡有较大的影响。常德市的净酸度沉积量在2004年高达199．29meq m^-2yr^-1,而从2004年-2006年,净酸度沉积量和离子沉降总通量均在逐年降低,表明常德市降雨酸化现象有所缓和．     

Nitrogen depositions to the Baltic Sea: Experimental and model estimates

Air pollution in the Baltic region is being monitored and assessed within the framework of the Helsinki Commission for the Protection of the Marine Environment in the Baltic Sea. Measurements of inorganic nitrogen compounds in precipitation, and to a lesser extent in air, have been performed since the mid-1980s under the supervision of HELCOM's Expert Group on Air Pollution, EGAP. The purpose is to establish a basis for evaluating the airborne pollution load to the Baltic Sea. These data have been used to estimate deposition of nitrogen to the sea surface by using various methods of extrapolating coastal data on concentrations and precipitation amounts. These estimates are supplemented by model calculations with the EMEP models. Estimates for the period 1986–1990 show that the annual wet deposition fluxes vary from about 650 kg N km⁻² in the north to about 1100 kg N km ⁻² in the southern Baltic Sea, resulting in a total wet deposition of about 325 kT N yr⁻¹. Other authors have estimated dry depositions for 1980–1986 at about 60 kT N yr⁻¹. O the other hand, model calculations lead to a total dry and wet deposition of about 275 kT N yr⁻¹. The reasons for the deviations are discussed and used to infer methodological limitations.     

山东省主要城市酸沉降现状及影响因素分析

根据山东省多年降水观测资料,分析了其17个设区城市的酸雨现状,并研究了济南市和青岛市硫的干、湿沉降及其变化规律.结果表明,近5a(1997～2001年)青岛市降水酸度位列全省17城市之首,是唯一降水pH年均值低于酸雨临界值5.60的城市;山东省主要城市的降水酸度总体上呈下降趋势.济南市和青岛市近年来硫沉降总通量基本稳定或呈下降趋势,仍达10t/(km²·a)左右;在硫沉降总通量中,硫干沉降的贡献率达80%以上,而在硫干沉降通量中,SO₂干沉降的贡献率要远远高于SO₄^2-干沉降的贡献率.通过分析酸雨前体物排放强度、土壤酸碱性以及气象条件对酸沉降的影响,揭示了山东省内主要城市酸沉降的影响因子.     

广州市类二噁英-多氯联苯大气沉降通量和组成

研究了广州市4个采样点2005年11月到2006年3月期间的类二噁英-多氯联苯(DL-PCBs)的沉降通量和组成.研究表明,广州市DL-PCBs的平均沉降通量为223pg·m-·2d-1,对应的毒性当量为1.5pg·m-·2d-1.城区DL-PCBs的沉降通量是郊区的1.6倍.各采样点DL-PCBs同系物分布相同,主要的同系物为PCB118、PCB105、PCB77,其平均含量分别为30%、18%和17%.湿季的DL-PCBs的沉降通量高于干季,表明降水对沉降通量影响明显.通过初步的源分析,发现某些含PCBs产品和固体废物焚烧可能是大气中DL-PCBs主要的来源.     

密云水库周边小流域大气氮磷沉降特征研究

大气沉降是氮磷元素进入水体的重要途径之一,为了解密云水库水源地周边大气氮磷沉降特征,选取土门西沟小流域为研究区域,设置降水、降尘自动采样器进行为期一年(2019年9月—2020年8月)的大气沉降收集,分析大气干、湿沉降中不同形态氮磷通量逐月和季节变化及其影响因素,估算大气氮磷沉降对小流域及密云库区氮磷输入的贡献. 结果表明:①土门西沟小流域大气氮、磷年沉降通量分别为38.393和1.952 kg/(hm2·a),氮磷干湿沉降通量季节性变化显著. ②湿沉降受气象(降雨量、温度、降雨时间间隔)等因素影响,氮磷沉降通量表现为夏季>春季>秋季>冬季,温度升高、降雨时间间隔变长均会使氮磷湿沉降浓度增大,而降雨量大小与大气湿沉降通量直接相关. ③干沉降受物质来源及气象等因素影响,氮磷沉降通量呈夏冬季高、春秋季低的特点,其中风向、风速是影响大气氮磷干沉降的重要因子. ④经计算,土门西沟小流域大气氮、磷沉降贡献分别为1 339.90和1.50 kg/a,分别占其氮、磷输出贡献的28.57%和0.39%,若不考虑空间差异性,预计大气沉降直接落入密云水库总氮(TN)和总磷(TP)的沉降量分别为551.18和28.02 t. 研究显示,大气沉降是密云库区周边面源污染综合管理的重要一环,未来应引起足够关注.      

基于GOME-2卫星遥感数据估算近海海域氮沉降通量的方法研究

提出了一种利用NO2卫星遥感数据估算近海海域NO2干沉降与无机氮(除氨氮)湿沉降通量的新方法。利用该方法对中国黄海海域2009年N沉降通量进行了估算,并将估算结果与其他研究结果进行了对比。结果表明:该方法估算通量均值相对较高,但与其他研究在数量级上是一致的,并能够反映研究海域大气N沉降通量的空间分布状况,可为我国海洋环境监测与评价大面积数据获取提供技术支撑。     

洱海大气氮素湿沉降特征

通过对2020年位于洱海湖区周边4个站点大气降水的实地监测，定量揭示了大气湿沉降不同形态氮素（TN、DTN、AN、NN、NIT、PN）的浓度和时空分布规律，探讨了氮素沉降通量的变化特征及其主要影响因子，进而明确了大气氮湿沉降对湖区外源性氮素输入的贡献程度，评估了氮素湿沉降入湖负荷对湖区水环境的影响。结果表明：各监测点降水中氮素浓度年内总体呈先升后降再升的趋势，总氮浓度为0.18～8.73 mg/L，平均浓度为1.34±0.686 mg/L，氮素浓度呈现干季高湿季低的变化规律；氮素湿沉降通量月际变化大致呈M双峰型，沉降通量峰值出现在浓度最低但降雨量最大的8月，最小值出现在12月，沉降通量与降雨量呈极显著正相关，沉降通量AN/NN为1.97，农业生产活动的氮素排放是湿沉降的主要来源；2020年洱海湖面湿沉降总氮直接输入负荷量约为170.11 t，其中铵态氮86.86 t，硝态氮51.58 t，总氮直接入湖负荷约占流域农业面源排放量的6.18%。     

Interannual variability in acidic deposition on the Mt. Mitchell area forest

Recently the forest decline at high elevation mountains in the eastern U.S. has been suggested to be associated with the deposition of acidic substances on the forest canopy through dry, wet and cloud deposition pathways. To determine the relative importance of these deposition mechanisms, a field study was initiated in May 1986, at Mt. Mitchell, NC. Since Mt. Mitchell is frequently immersed in clouds (immersion time being in the range of 28–41%), our investigations were primarily focused on the collection of cloud water and the monitoring of meteorology and ambient air quality. The precipitation data and related chemistry were obtained from a nearby NADP (National Atmospheric Deposition Program) site (Clingman's Peak). To estimate the dry and cloud deposition, the deposition velocities for gases and the rates of cloud deposition for cloud droplets are calculated with the ATDD (Atmospheric Turbulence and Diffusion Division, National Oceanic and Atmospheric Administration) model and a cloud deposition model (CDM), respectively. The wet deposition is obtained from NADP annual reports. Computations show the deposition velocities for SO₂, NO₂ and O₃ to be in the range of tenths of cm s⁻¹. The mean rate of cloud deposition is about 0.13–0.21 mm h⁻¹. The rainfall ranged from 40 to 60 cm during the growing seasons (from mid-May to the end of September) of 1986–1988. Using these deposition parameters and the 3 year database, the deposition fluxes of sulfur (S) compounds are found primarily contributed through cloud capture mechanism (60%) followed by incident precipitation (25%) and dry deposition (15%). As to the deposition fluxes of nitrogen (N) compounds, cloud, wet and dry deposition contributedf about 50%, 25% and 25%, respectively. A comparison of deposition estimates at Mt. Mitchell with those at other sites shows that the sulfate deposition at sites exceeding 1200 m MSL in elevation in Bavaria, F.R.G., and the eastern U.S. is a almost identical within error limits. Reasons for large uncertainties in deposition estimates are also discussed as the mechanisms for redistribution of the deposited material on the forest canopy.     

福建省兴化湾大气重金属的干湿沉降

在兴化湾周围采集1年的大气颗粒物及降雨样品,测定分析了Cd,Pb,Zn和Cu 4种重金属的含量及其大气干湿沉降通量随季节的变化规律,并利用Pb同位素对大气颗粒物的来源进行了解析.结果表明:大气重金属的干沉降通量随季节变化不大,而湿沉降通量随季节变化明显.大气干沉降通量中,Cd,Cu随季节变化很小,而Pb,Zn有一定的季节变化,主要是因为降雨对大气颗粒物的去除作用.大气湿沉降通量中,所有重金属元素受降雨量影响显著,另外还与季节和风速有关.除Pb外,Cd,Zn和Cu的湿沉降通量均大于干沉降通量,说明湿沉降在大气对兴化湾重金属的输入过程中起主导作用.而Pb的输入则以颗粒态为主.根据Pb稳定同位素分析,兴化湾大气颗粒物中的重金属主要来源于工业活动.      

大连湾海域大气无机氮沉降通量研究

为了解大连湾无机氮沉降入海通量情况,2014年和2016年在大连湾区域开展了大气干湿沉降的采样和分析,并通过模型估算大连湾海域的无机氮沉降通量。结果表明,大连湾海域干沉降中无机氮入海通量约为46.4 t/a,采样期间,大气气溶胶中无机氮的最高浓度为15.5 μg/m3,最低浓度为0.589 μg/m3。季节变化上看,春季无机氮沉降均值为6.60 μg/m3,为全年最大,夏季无机氮沉降浓度为5.59 μg/m3,为全年无机氮沉降最小。大连湾海域湿沉降无机氮通量约为134.64 t/a,其中,9月无机氮湿沉降通量最高,为35.86 t,11月最低,为0.53 t。通过大气干湿沉降输入到大连湾的无机氮占大连湾海域无机氮输入总量的1.9%,且湿沉降通量占比更高,大约为干沉降通量的3倍。