我国氮沉降观测方法进展及其在珠三角的应用

在对我国大气氮沉降观测方法进行系统整理的基础上,以珠三角为例对长期氮沉降观测的结果进行了详细的时空分析.结果显示,大气氮沉降通量从东南沿海到西北内陆递减,且遭受人类活动影响较大的生态系统具有高沉降负荷的倾向.森林生态系统湿沉降通量的观测值变化范围为18~38kgN/(hm~2·a);农田生态系统中湿沉降通量的变化范围为6~78kgN/(hm~2·a),混合沉降通量为15~133kgN/(hm~2·a),干沉降通量为54~83kgN/(hm~2·a);而在城市生态系统中混合沉降通量可达101kgN/(hm~2·a).在人口密集的珠三角地区,氮沉降通量与NH_4~+-N/NO_3~--N值近年来均呈下降趋势,这主要与珠三角产业结构调整以及城市发展带来的巨大能耗有关.整体而言,我国氮沉降观测方法日渐趋于多样化,且观测的准确度不断提高,但偏远地区观测站点仍较为匮乏.对氮沉降的研究多集中于湿沉降和混合沉降,而针对干沉降的研究仍较为不足.     

氮沉降对林带土壤N2O和CH4通量的影响

于2008年4月~2009年10月在龙王山对林带土壤进行模拟氮沉降试验,采用静态箱-气相色谱法测定土壤N2O和CH4通量,研究氮沉降增加对土壤N2O和CH4排放(吸收)的影响.结果表明,短期内,氮沉降没改变土壤N2O和CH4通量的季节性变化规律和日变化规律.与对照(CK)相比,短期的低氮[50 kg N/(hm2·a), TL]、中氮[100kgN/(hm2·a), TM]和高氮[150kgN/(hm2·a), TH]处理对土壤的N2O和CH4年平均通量和日平均通量都没有显著影响.     

华西雨屏区典型人工林对降雨过程中NH_4~+-N和NO_3~--N的过滤作用

氮沉降已成为河流、湖泊及城市等生态系统的主要污染威胁因素之一,森林生态系统能从林冠、地被和土壤自上而下截留过滤大气降雨中的NH+4-N和NO-3-N,是区域大气环境污染生态防治的重要途径.选取华西雨屏区几种典型人工林森林生态系统为研究对象,采用定位监测与室内分析相结合的研究方法,于2011年4—12月对大气降水、穿透雨、树干茎流、地表径流和地下渗滤NH+4-N和NO-3-N的含量与分配进行了研究.结果表明:观测期内40次降雨总雨量为492.72 mm,NH+4-N和NO-3-N的总沉降量分别为13.248 kg·hm-2和16.320 kg·hm-2;3种人工林林冠层对NH+4-N和NO-3-N的过滤能力表现为香樟林混交林柳杉林,而地表和土壤层均表现为混交林香樟林柳杉林;无林地、香樟林、柳杉林和混交林生态系统无机氮截留过滤净输入量分别为19.557、44.079、42.331、64.896 kg·hm-2,对无机氮的综合过滤作用表现为混交林香樟林柳杉林无林地.这些结果说明华西雨屏区合理配置混交林能更加有效地降低大气氮沉降对生态系统的影响.     

内蒙古温带草原氮沉降的观测研究

在内蒙古太仆寺旗对温带草原地区的氮沉降进行了为期1 a(2011年11月～2012年10月)的观测.在线分析大气NH3和NO2浓度,用CMAQ模型计算的干沉降速率计算了气体干沉降量;采集降水、降尘和穿透雨样品并测定NH4+和NO3-浓度,分别得到湿沉降、颗粒物干沉降和穿透雨沉降量.观测结果表明该地区的氮沉降量已经高达3.43 g.(m2.a)-1,有可能对草原生态系统产生危害.其中,湿沉降占44%,气体干沉降占38%,颗粒物干沉降占18%.干沉降对氮沉降的贡献大于湿沉降,必需重视干沉降的测定,而穿透雨沉降明显小于总沉降,说明穿透雨法不适合于草原地区.从组分上看,还原态氮(包括NH4+和NH3)对氮沉降的贡献为71%,而氧化态氮(NO3-和NO2)的贡献仅29%,因此在控制氮沉降时,不应只针对NOx排放进行削减,NH3减排同样重要.     

大气沉降向林地(小叶栎)输入硫素通量的观测

利用中国科学院红壤生态试验站森林小气候观测站(江西鹰潭)逐时气象梯度参数连续自动观测数据,采用阻力模式计算SO₂、硫酸盐(SO₄^2-)粒子的干沉降速率(Vd),结合大气SO₂、SO₄^2-粒子浓度现场测定,研究了该地2年大气硫沉降量.结果表明,2000年大气SO₂和SO₄^2-粒子时年Vd值分别为0.748cm/s、0.665cm/s;2002年分别为0.180cm/s、0.221cm/s.2000和2002年大气干沉降硫(SO₂+SO₄^2-粒子)通量分别为104.6kgS/(hm2a)和140.6kgS/(hm2a),SO2干沉降是大气干沉降主要贡献者,占98.38%和97.2%;大气沉降硫总量分别为150kgS/(hm2a)和185kgS/(hm2a);可见大气干沉降是大气硫沉降主要贡献者,分别占70%和76.2%.     

林地大气氮沉降的观测研究

2004年11月～2005年10月,以小叶栎林地为研究对象,研究了大气沉降氮通量及其3种物理形态(气态、颗粒态、雨水)4种氮化物(NH₃,NH₄⁺-N,NO₃^--N,NO₂)的相对贡献.结果表明,大气氮沉降总量为82.8kg/(hm²·a),其中干沉降占67%;NH3-N是氮沉降的主要贡献者,占干沉降的82%,占总氮沉降量的56%;还原态的氮化物(NH₃,NH₄⁺-N)占总氮沉降量65%.     

氮沉降增加对青藏高原林地氮淋溶通量的影响

森林生态系统对大气氮沉降升高的响应机制是国内外学者研究的热点问题之一,近年来中国学者相继在温带森林和热带森林建立了氮沉降增加影响的野外实验平台,但关于氮沉降增加对青藏高原地区森林土壤氮素淋溶通量影响的野外原位研究匮乏。基于此,该研究于2012-2013年生长季,在青藏高原林芝地区云冷杉林通过野外模拟试验,研究了3种水平(0、15和30 kg/(hm~2·a)(以N为计,下同))及3种形态((NH_4)_2SO_4、NH4Cl和KNO_3)氮沉降增加对土壤可溶性氮素淋溶通量的影响。结果表明:林芝地区不同形态氮素的淋溶通量均存在显著的季节和年际变化特征,铵态氮(NH4+-N)、硝态氮(NO_3~--N)的生长季月淋溶通量为0.02～0.6 kg/hm~2,可溶性总氮(TDN)、可溶性总有机氮(DON)月淋溶通量为0.07～2.0 kg/hm2,不同形态氮淋溶通量峰值均出现在7-9月;森林穿透雨中硝态氮沉降通量的增加,对氮素淋溶通量具有明显的促进作用,造成NO_3~--N显著淋失(p0.05),且这种促进作用在施加低剂量硝态氮肥的处理上更为明显(p0.01);大气氮沉降增加对DON和TDN淋溶通量有显著的抑制作用,且随着氮沉降量的增加其抑制作用也随之增加。     

黑龙江凉水国家级自然保护区大气氮沉降特征

为了监测黑龙江凉水国家级自然保护区的大气氮沉降水平,在2015年生长季用干湿沉降采集器连续观测了大气氮湿沉降和颗粒物干沉降量,并在非生长季用自制观测桶观测了大气混合氮沉降量.结果表明:(1)该区2015~2016年度大气氮沉降总通量(生长季湿沉降+颗粒物干沉降以及非生长季混合沉降)为12.93 kg·(hm~2·a)~(-1),其中无机氮沉降总通量为8.27kg·(hm~2·a)~(-1),NH_4~+/NO_3~-为1.3;有机氮沉降总通量为4.66 kg·(hm~2·a)~(-1),占全氮比例为36.0%.(2)生长季(湿沉降+颗粒物干沉降)和非生长季(混合沉降)氮沉降总量分别为11.42 kg·hm~(-2)和1.51 kg·hm~(-2),分别占全年氮沉降总通量的88.3%和11.7%.(3)生长季氮湿沉降总量为9.28 kg·hm~(-2),占生长季氮干湿沉降总量的81.3%,且与降水量显著正相关(R2=0.87,P0.001);生长季颗粒物干沉降总量为2.14 kg·hm~(-2),占生长季干湿沉降总量的18.7%.该区氮湿沉降量受降水量影响明显,且在全国属于中等水平,存在一定的环境风险,当地在生活生产过程中应注意环境保护与水质监测.     

南海东部大气湿沉降中无机氮的研究

通过分析2000至2014年菲律宾马尼拉(Manila)和洛斯巴诺斯(Los Banos)大气湿沉降资料,初步探讨近15年湿沉降中无机氮含量特征以及对南海东部海域水生生态系统的影响。结果显示,湿沉降中NO-3-N和NH+4-N的浓度均为旱季高雨季低;NO-3-N浓度在近15年虽有波动,但并无明显变化趋势;而洛斯巴诺斯区域的NH+4-N浓度自2009后稍有波动上升。NO-3-N和NH+4-N的沉降通量与浓度相反,表现为雨季高而旱季低,年际上总体表现为NH+4-N的沉降通量大于NO-3-N,马尼拉无机氮的沉降通量大于洛斯巴诺斯,并且在2003年之后,马尼拉和洛斯巴诺斯NH+4-N的沉降通量均呈明显上升趋势,菲律宾经济的快速增长及人类活动是主导其上升的主要因素。马尼拉和洛斯巴诺斯湿沉降中NO-3-N/NH+4-N值分别为0.33和0.41,该比值和无机氮浓度与南海东部各海区表层海水的值有明显的差别,因此降水可能改变该海域表层水体无机氮的组成结构,进而影响水体中浮游植物的生长及其群落结构。     

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.      

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.     

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.     

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).     

阔叶林地大气氮化物干沉降速率动态变化研究

以2004年中国科学院红壤生态试验站森林小气候分站气象资料,计算近地面湍流特征参数(U*、θ*和L),采用大叶阻力相似模型计算各种氮化物干沉降速率(Vd),研究了该阔叶林地大气氮化物Vd动态变化.结果表明,1年中大气NO3-粒子/NH4+粒子、HNO3(g)、NO2和NH3的Vd年均值分别为0.216,0.985,0.115,0.274 cm/s;1天中,Vd白天大于晚上,最大值出现在中午11:00~12:00.大气氮化物Vd冬、春季高,夏、秋季低.     

太湖氮磷营养盐大气湿沉降特征及入湖贡献率

2009年8月—2010年7月在太湖流域不同区域10个采样点收集降水样品230多个,测定其中不同形态N,P营养盐的质量浓度,分析太湖大气湿沉降中N,P营养盐沉降特征,计算N,P营养盐湿沉降率及其占太湖河流入湖负荷的贡献率. 结果表明:湿沉降中ρ(TN)年均值为3.16 mg/L,DTN(溶解性总氮)占TN的70%以上,其中以NH₄+-N为主;湿沉降中ρ(TN)年均值最高值出现在南部湖区,最低值出现在北部湖区. 湿沉降中ρ(TP)年均值为0.08 mg/L,相对较低. 5个区域湿沉降中不同形态N的质量浓度均表现为冬季高、夏季低,而不同形态N,P的湿沉降量均为夏季最大. 南部、东部湖区TN的湿沉降率相对较大. 各采样点湿沉降中NH₄+-N沉降率约占DTN沉降率的30.4%～52.0%,NO₃--N沉降率约占DTN的31.6%;各区域间湿沉降中DTP(溶解性总磷)占TP的比例差异较大. 大气湿沉降中TN和TP的年沉降总量分别为10 868 和247 t,为同期河流入湖负荷的18.6%和11.9%,湿沉降对太湖富营养化的贡献及可能带来的水生态系统的影响不容忽视.      

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.      

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.     

A new method for estimation of dry deposition of particles based on throughfall measurements in a forest edge

Throughfall measurements are very often used to calculate the atmospheric input to ecosystems. Such attempts are normally complicated by canopy interaction processes which are difficult to assess. This study presents an approach to calculate dry deposition and canopy leaching of Ca²⁺, Mg²⁺ and K⁺ to forests. The calculations are based on throughfall measurements in a forest edge of a spruce stand and by use of Na⁺ as a model substance for dry deposition of particles. This ‘forest edge approach’ is compared with an approach based on equal Na⁺ to base cation ratios in wet and dry deposition (‘wet/dry ratio approach’), which has been widely used in the literature. Our calculations show that the wet/dry ratio approach may overestimate the dry deposition of Ca²⁺, Mg²⁺ and K⁺ by up to 100% and leaching will correspondingly be underestimated. The assumptions underlying the different approaches and the use of throughfall measurements to estimate dry deposition are discussed and it is suggested that throughfall measurements in forest edges may be a valuable improvement to studies of atmospheric deposition in forests.     

Ammonia volatilization losses and 15N balance from urea applied to rice on a paddy soil

Ammonia volatilization loss and ^15N balance were studied in a rice field at three different stages after urea application in Taihu Lake area with a micrometeorological technique. Factors such as climate and the NH4^＋-N concentration in the field floodwater affecting ammonia loss were also investigated. Results show that the ammonia loss by volatilization accounted for 18.6%-38.7% of urea applied at different stages, the greatest loss took place when urea was applied at the tillering stage, the smallest at the ear bearing stage, and the intermediate loss at the basal stage. The greatest loss took place within 7 d following the fertilizer application. Ammonia volatilization losses at three fertilization stages were significantly correlated with the ammonium concentration in the field floodwater after the fertilizer was applied. ^15N balance experiment indicated that the use efficiency of urea by rice plants ranged between 24.4% and 28.1%. At the early stage of rice growth, the fertilizer nitrogen use efficiency was rather low, only about 12%. The total amount of nitrogen lost from different fertilization stages in the rice field was 44.1%-54.4%, and the ammonia volatilization loss was 25.4%-33.3%. Reducing ammonia loss is an important treatment for improving N use efficiency.