大气氮沉降及其对水体氮负荷估算的研究进展

大气氮沉降已经并将继续对全球生态系统产生重大影响。大气氮沉降是陆源氮进入水体的重要途径,会使水体氮含量增加,富营养化加重,严重影响生态系统的稳定性。因此,大气氮沉降通量及其对水生生态系统的影响等问题值得深入探讨。介绍了国内外大气氮沉降监测网络、空间分异等方面的研究进展,总结了大气氮干湿沉降的研究方法及大气氮沉降对水体氮负荷的影响,并探讨了该领域目前存在的问题及发展趋势。     

邯郸市大气氮干湿沉降通量及其特征

为研究大气降尘对土壤、水体等环境介质中氮的贡献,在邯郸市区设置3个大气干湿沉降采样点,并进行了为期1年的监测。根据监测数据分析了氮干湿沉降通量、氮形态及随季节的变化。结果显示,监测期内3个采样点的全年平均氮干沉降通量为385.2kg/km~2,湿沉降通量为2 292.5kg/km~2,总沉降通量为2 677.7kg/km~2。氮沉降以湿沉降为主,占总沉降通量的85.6%。氮湿沉降通量与降雨量线性相关(R~2=0.87),各采样点的降雨量和氮湿沉降主要集中在4—8月。氮干沉降与降尘量均随季节变化,总的来说冬春季开始增长,夏季降低,到了初秋又开始增长,并在10月达到峰值。不论是干沉降还是湿沉降,各监测点氮形态都是以有机氮为主,硝酸盐氮次之,氨氮所占比例最低。     

珠江口大气氮磷干湿沉降通量及其污染特征

为准确核定入海污染负荷和系统实施入海污染物总量控制,观测了珠江口地区大气氮磷的干湿沉降通量,并分析了其时空变异规律、化学组成特征以及主要的影响因素。结果显示,珠江口地区大气总氮和总磷的平均月沉降通量分别约为299.00、4.12kg/km2,其中湿沉降通量占总沉降通量的60%以上。干沉降和湿沉降通量均表现出明显的时空变异规律,前者的季节性变化主要受农业活动氮磷挥发的影响,而后者与年内降雨量分布以及季风作用下降雨云团来源的关系更为密切;沉降负荷的空间分布规律基本与不同区域受人类活动影响的特点相一致。由于不同污染来源和季风气候的影响,氮沉降化学组成的季节差异特征也较为明显,氨氮在秋冬季沉降中所占的比例明显高于春夏季,而有机氮则与之相反。     

上海大气氮湿沉降的污染特征

为探讨上海大气氮湿沉降的污染特征,采集了2007年11月至2008年10月上海雨水样品,分析了大气氮湿沉降浓度,探讨了上海大气湿沉降氮通量及上海市区,市郊和远郊大气氮湿沉降的时空污染特征.结果表明:(1)上海市区、市郊和远郊大气氮湿沉降质量浓度平均值分别为2.96、2.31、2.21 mg/L.从上海大气湿沉降总体来看,大气氮湿沉降劣V类、V类的超标率分别达到51.09%和13.87%.推断大气氮湿沉降的主要来源是机动车辆所排放的大量氮氧化物.(2)除冬季外,其余季节上海市区大气氮湿沉降浓度均大于市郊和远郊;市区和远郊大气氮湿沉降浓度均在秋季最大,市郊大气氮湿沉降浓度在春季最大.(3)上海大气年氮湿沉降通量为78.42 kg/hm~2,同其他区域相比较,属于世界上高氮沉降区域.(4)上海大气月氮沉降通量与月平均降雨量呈显著的线性正相关(p<0.05),说明上海大气氮湿沉降通量主要受降雨量的影响.     

滇池流域大气氮、磷干湿沉降通量及入湖贡献

为了探究滇池流域氮、磷干湿沉降对滇池水体外源输入营养盐的贡献率,于2021年收集了滇池流域六大功能区的雨水及降尘,测定大气沉降中不同形态氮、磷质量浓度,分析滇池流域氮、磷大气沉降分布特征,并估算氮、磷干湿沉降全年沉降通量及对滇池入湖负荷的贡献。结果表明：流域内全年大气总氮（TN）、总磷（TP）湿沉降通量分别为20.244～220.938、1.155～65.826 kg/km²,干沉降通量分别为44.275～481.120、4.255～111.840 kg/km²;工业生产和矿产开发功能区分别为流域氮、磷干湿沉降通量最高的区域。溶解性无机氮（DIN）和溶解性无机磷（DIP）是大气沉降中氮、磷的主要形态;流域内氮、磷大气沉降入湖负荷分别为1 018.92、88.88 t,其中滇池湖面大气直接沉降负荷占流域入湖污染负荷总量的3.70%和2.35%,流域其他区域入湖系数换算下大气沉降入湖负荷在流域河流入湖负荷中的占比分别为8.69%和6.26%。流域氮、磷大气沉降已逐渐成为滇池外源污染物的重要来源之一,深入掌握其时空分布特征及入湖贡献率是进一步加强流域管理和减轻湖体外源污染物输入的重要前提。     

太湖上游流域地表水及污水处理厂尾水氮、磷污染特征分析

抽样分析了太湖上游流域地表水、以生活污水为主的污水处理厂尾水以及工业园区(印染、化工)集中污水处理厂尾水水样,重点表征了地表水和污水处理厂尾水氮、磷污染物的组成及污染特征。结果表明,污水处理厂尾水及地表水中的氮污染类别主要为亚硝态氮、硝态氮,高浓度有机氮主要存在于化工园区集中污水处理厂尾水中,而磷污染的主要类别为有机磷,其浓度平均占总磷浓度的50%以上。建议污水处理厂进一步强化生物脱氮效率,提高混凝沉淀效果,并针对有机氮实施有针对性的预处理手段以提高总氮去除率。     

南宁市郊空气和大气干湿沉降物中多环芳烃的污染特征

采用空气被动采样器和大气干湿采样器分夏、冬季采集大气及其干湿沉降物样品,利用气相色谱-质谱联用仪测定16种多环芳烃(PAHs)优先控制污染物。结果表明:冬、夏季大气干湿沉降物中PAHs的平均值分别为581.06、174.59ng/(m2·d),冬季PAHs的组成以2～3环PAHs为主,夏季以4～6环PAHs为主;冬、夏季空气中PAHs的平均值分别为149.16、168.70ng/d,均以2～3环PAHs为主。大气干湿沉降物PAHs的沉降通量时空变化为:冬季,商住文教混合区农业区工业区;夏季,工业区农业区商住文教混合区;冬季大于夏季3.3倍。空气PAHs沉降通量的时空变化为:冬季,工业区商住文教混合区农业区;夏季,农业区工业区商住文教混合区;冬季略低于夏季。     

太湖湖泊缓冲带不同类型草林复合系统中氮、磷的溶出与沉降特征

以太湖竺山湾缓冲带中湿地岸带、支浜岸带、人工防护林3种主要类型的草林复合系统为研究对象,分别对其自身氮、磷溶出及沉降特征进行了研究,从而揭示缓冲带本身对地表径流和地下渗流的影响。结果表明,3种样地中总氮的溶出率在0.3%~2.5%,平均溶出率表现为人工防护林支浜岸带湿地岸带;总磷的溶出率在0.8%~4.0%,平均溶出率表现为支浜岸带湿地岸带人工防护林。氮、磷在向下沉降的过程中表现出不同的规律。各样地不同深度土壤渗透液中总氮浓度的变化趋势不一,基本表现为随深度增加而增加,总氮浓度为湿地岸带人工防护林支浜岸带;总磷浓度的变化趋势也不尽相同,与总氮相比,总磷的沉降效果不显著。综合来看,3种草林复合系统对污染物的沉降效果为湿地岸带人工防护林支浜岸带。     

太湖苕溪流域农业面源污染评价及对策

苕溪水系是太湖的重要支流,其总流量的70％入太湖.近年来沿水系农业发展带来的面源污染问题日益突出,在一定程度上影响了太湖的水源环境.通过对苕溪流域农业面源污染的调查和评价发现:流域种植业化肥TN污染负荷率高达98.03％,TP为1.97％;畜禽养殖粪便COD污染负荷率达74.91％,TN为20.59％,TP为4.50％;淡水养殖中精养鱼塘污染物TN污染负荷率达54.15％,COD为39.95％,TP为5.90％.针对这一现状,提出了太湖苕溪流域环境友好型农业发展的对策建议.     

浙东沿海城市大气颗粒物污染特征及来源解析研究

对2009年夏季浙东沿海地区环境空气质量进行监测,监测大气颗粒物(TSP、PM10、PM2.5、PM1.0)浓度,分析颗粒物污染特征、水溶性离子及无机元素组成,运用化学质量平衡受体模型(CMB模型)对浙东沿海地区大气TSP来源进行解析.结果表明,浙东沿海地区的大气颗粒物主要以细颗粒物为主,颗粒物中主要的水溶性离子为SO2-4、NH+4、Ca2+,土壤尘是该地区大气TSP的主要来源,北仑、乐清和奉化TSP中土壤尘的分担率分别达到55.49%、42.52%、40.70%,各监测点TSP来源具有一定的地域特征.     

Distribution and bioaccumulation of organochlorine pesticides in surface sediments and benthic organisms from Taihu Lake, China

The spatial distribution and bioaccumulation of organochlorine pesticides (OCPs) in surface sediments and benthic organisms from Taihu Lake were studied. OCPs were detected in all sediment samples with total concentrations ranging from 4.22 to 461 ng g⁻¹ dry weight (dw). The ratios of certain metabolites to their parent compounds indicated there are still new inputs of parent DDT (dichlorodiphenyltrichloroethane) to Taihu Lake, while the highest residues of HCHs (hexachlorocyclohexanes) mainly came from earlier usage and fresh γ-HCH (lindane). No positive correlation was found between the distribution of OCPs and organic matter contents in sediments. Concentrations of OCPs and lipids in typical large benthic organisms, Bellamya aeruginosa (B. aeruginosa) and Corbicula fluminea (C. fluminea), increased with body weight. HCHs, DDTs, chlordanes and heptachlors were the dominant compounds detected in organisms and C. fluminea accumulated much more OCP than B. aeruginosa. Higher values of biota-sediment accumulation factor (BSAF) were detected in C. fluminea, which was both affected by biological characteristics of the organisms and physicochemical properties of the compounds.     

Atmospheric deposition and canopy exchange processes in alpine forest ecosystems (northern Italy)

Throughfall and bulk precipitation chemistry were studied for five years (June 1994–May 1999) at two high elevation forest sites (Val Gerola and Val Masino) which were known to differ in terms of tree health, as assessed by live crown condition. The ion concentration of bulk precipitation samples did not differ significantly between sites, except for Mg²⁺, while the throughfall concentrations differed in the measured values of H⁺, N-NO₃⁻, Cl⁻, Na⁺, K⁺, DOC and weak organic acids. The results of the application of the canopy exchange model indicated a higher contribution from the dry deposition of N-NO₃⁻, N-NH₄⁺ and H⁺ at Val Gerola, where the damage symptoms were more evident. In addition, the canopy leaching of Ca²⁺, K⁺ and weak organic acids were 47%, 21% and 27% higher at Val Gerola than at Val Masino. Annual SO₄²⁻ deposition fluxes (21.3 kg ha⁻¹ yr⁻¹ at Val Masino and 23.6 kg ha⁻¹ yr⁻¹ at Val Gerola) were similar to those reported for moderately polluted European and U.S. sites. Annual N loads were 13.6 and 13.1 kg ha⁻¹ yr⁻¹ in the bulk input, and 15.0 and 18.0 kg ha⁻¹ yr⁻¹ in throughfall inputs, at Val Masino and Val Gerola, respectively. The contribution of the organic fraction to the total N atmospheric deposition load is significant, constituting 17% of the bulk flux and 40% of the throughfall flux. Measured nitrogen loads exceed the critical nutrient loads by several kg N ha⁻¹ at both stations. In particular the nitrogen throughfall load at Val Gerola was about 3 times higher than the critical values.     

Resolving the variability of CDOM fluorescence to differentiate the sources and fate of DOM in Lake Taihu and its tributaries

Taihu Basin is the most developed area in China, which economic development has resulted in pollutants being produced and discharged into rivers and the lake. Lake Taihu is located in the center of the basin, which is characterized by a complex network of rivers and channels. To assess the sources and fate of dissolved organic matter (DOM) in surface waters, we determined the components and abundance of chromophoric dissolved organic matter (CDOM) within Lake Taihu and 66 of its tributaries, and 22 sites along transects from two main rivers. In Lake Taihu, there was a relative less spatial variation in CDOM absorption a_CDOM(355) with a mean of 2.46 ± 0.69 m⁻¹compared to the mean of 3.36 ± 1.77 m⁻¹ in the rivers. Two autochthonous tryptophan-like components (C1 and C5), two humic-like components (C2 and C3), and one autochthonous tyrosine-like component (C4) were identified using the parallel factor analysis (PARAFAC) model. The C2 and C3 had a direct relationship with a_CDOM(355), dissolved organic carbon (DOC), and chemical oxygen demand (COD). The separation of lake samples from river samples, on both axes of the Principal Component Analysis (PCA), showed the difference in DOM fluorophores between these various environments. Components C1 and C5 concurrently showed positive factor 1 loadings, while C4 was close to the negative factor 1 axis. Components C2 and C3 showed positive second factor loadings. The major contribution of autochthonous tryptophan-like components to lake samples is due to the autochthonous production of CDOM in the lake ecosystems. The results also showed that the differences in geology and associated land use control CDOM dynamics, such as the high levels of CDOM with terrestrial characteristics in the northwestern upstream rivers and low levels of CDOM with increased microbial characteristics in the southwestern upstream rivers. Most of river samples from the downstream regions in the eastern and southeastern plains had a similar relative abundance of humic-like fluorescence, with less of the tryptophan-like and more of the tyrosine-like contributions than did samples from upstream regions.     

Atmospheric deposition, retention, and stream export of dioxins and PCBs in a pristine boreal catchment

The mass-balance between diffuse atmospheric deposition of organic pollutants, amount of pollutants retained by the terrestrial environment, and levels of pollutants released to surface stream waters was studied in a pristine northern boreal catchment. This was done by comparing the input of atmospheric deposition of polychlorinated dibenzo-p-dioxins and furans (PCDD/Fs) and PCBs with the amounts exported to surface waters. Two types of deposition samplers were used, equipped with a glass fibre thimble and an Amberlite sampler respectively. The measured fluxes showed clear seasonality, with most of the input and export occurring during winter and spring flood, respectively. The mass balance calculations indicates that the boreal landscape is an effective sink for PCDD/Fs and PCBs, as 96.0-99.9 % of received bulk deposition was retained, suggesting that organic pollutants will continue to impact stream water in the region for an extended period of time.     

Lichen-based critical loads for atmospheric nitrogen deposition in Western Oregon and Washington Forests, USA

Critical loads (CLs) define maximum atmospheric deposition levels apparently preventative of ecosystem harm. We present first nitrogen CLs for northwestern North America’s maritime forests. Using multiple linear regression, we related epiphytic-macrolichen community composition to: 1) wet deposition from the National Atmospheric Deposition Program, 2) wet, dry, and total N deposition from the Communities Multi-Scale Air Quality model, and 3) ambient particulate N from Interagency Monitoring of Protected Visual Environments (IMPROVE). Sensitive species declines of 20-40% were associated with CLs of 1-4 and 3-9 kg N ha⁻¹ y⁻¹ in wet and total deposition. CLs increased with precipitation across the landscape, presumably from dilution or leaching of depositional N. Tight linear correlation between lichen and IMPROVE data suggests a simple screening tool for CL exceedance in US Class I areas. The total N model replicated several US and European lichen CLs and may therefore be helpful in estimating other temperate-forest lichen CLs.     

High concentrations and dry deposition of reactive nitrogen species at two sites in the North China Plain

Atmospheric concentrations of major reactive nitrogen (N_r) species were quantified using passive samplers, denuders, and particulate samplers at Dongbeiwang and Quzhou, North China Plain (NCP) in a two-year study. Average concentrations of NH₃, NO₂, HNO₃, pNH₄⁺ and pNO₃⁻ were 12.0, 12.9, 0.6, 10.3, and 4.7 μg N m⁻³ across the two sites, showing different seasonal patterns of these N_r species. For example, the highest NH₃ concentration occurred in summer while NO₂ concentrations were greater in winter, both of which reflected impacts of N fertilization (summer) and coal-fueled home heating (winter). Based on measured N_r concentrations and their deposition velocities taken from the literature, annual N dry deposition was up to 55 kg N ha⁻¹. Such high concentrations and deposition rates of N_r species in the NCP indicate very serious air pollution from anthropogenic sources and significant atmospheric N input to crops.     

Nitrogen deposition and its ecological impact in China: An overview

Nitrogen (N) deposition is an important component in the global N cycle that has induced large impacts on the health and services of terrestrial and aquatic ecosystems worldwide. Anthropogenic reactive N (N_r) emissions to the atmosphere have increased dramatically in China due to rapid agricultural, industrial and urban development. Therefore increasing N deposition in China and its ecological impacts are of great concern since the 1980s. This paper synthesizes the data from various published papers to assess the status of the anthropogenic N_r emissions and N deposition as well as their impacts on different ecosystems, including empirical critical loads for different ecosystems. Research challenges and policy implications on atmospheric N pollution and deposition are also discussed. China urgently needs to establish national networks for N deposition monitoring and cross-site N addition experiments in grasslands, forests and aquatic ecosystems. Critical loads and modeling tools will be further used in N_r regulation.     

太湖流域小型水源性湖泊氮、磷时空分布及营养状态评价

2009年11月至2010年10月,对太湖流域小型水源性湖泊20个采样点水体的TN、TP、NO3--N、NH4+-N、NO2--N以及PO43-等水质因子进行测定分析,讨论了氮、磷时空分布特征,并评价其富营养化程度。结果表明,TN、TP年均值分别为1.50、0.05mg/L;TN、TP的季节性变化规律具有一定差异,TN浓度为冬、春季高于夏、秋季,而TP浓度为2009年11月至2010年3月高于其他月份。由于受入湖河流的影响,TN、TP的空间分布格局较为相似,均表现为西南部高于东北部、入湖口分别高于湖中心和出湖口。NO3--N年均值为0.68mg/L,浓度变化趋势呈双峰型(2010年3、9月为峰值),基本同TN的变化趋势一致,空间分布表现为入湖口分别低于湖中心和出湖口(除冬季外),显示水体硝化过程对硝酸盐的贡献。NH4+-N年均值为0.23mg/L,从2010年4月开始浓度逐渐升高,到2010年7月达到全年最高值,其浓度空间分布特征表现为入、出湖口均高于湖中心(除秋季外)。NO2--N和PO43-的年均值都较低,均为0.01mg/L(以P计),时空差异不明显。根据CARLSON提出的营养状态指数法计算分析可知,该湖泊冬、春季处于中营养状态,夏、秋季营养状态略高,且磷是全年初级生产力的限制因子。