太湖及其周围河流中N2O的空间分布与释放通量

本次研究选择中国东部一个生态和环境空间分异极大的浅水湖泊(太湖)以及周围河流,分别于2003年7月和9月两次采集湖水和河水样品,分析其中的N2O浓度,并利用扩散模型公式估算水-气界面N20交换通量.结果显示N2O饱和度的空间变化从70%不饱和到2708%过饱和变化范围很大.N2O饱和度的空间分布,N20与CH4、无机氮、TDS(总溶解固体物质)之间的相关性都表明:太湖重度富营养区N2O的产生极大地受到人为N输入的影响.然而,初步的通量分析显示湖泊N2O的释放因子不超过0.63%,小于河流中的默认值,N2O产率也略低于水环境中的平均值,太湖以面积为权重的释放通量平均值并不高,在7月和9月分别为14.0μmol/m2·d和9.7μmol/m2·d.这些结果表明流域人为N输入对整个湖泊N2O的促进作用是有限的,预计未来湖泊N2O释放不会因为人为活动增加而出现人幅度增加的状况.流域内各生态景观N2O释放量的比较,也表明富营养湖泊总体上仍然是一个十分有限的大气N2O释放源.相反,太湖周围河流存在较大的N2O释放速率,在7月和9月估算的N2O释放通量分别为142.1μmol/m2·d和28.8μmol/m2·d.将这一释放速率推广到整个流域后,预计河网的N2O释放量将占到耕作土壤的10%～50%,显示了河流对区域N2O质量平衡具有较重要的影响.     

贵州百花湖分层晚期有机质降解过程与溶解N2O循环

百花湖是一个具有季节性分层的富营养小型湖泊,在秋季湖水倒转期经常发生水质恶化事件,碳氮循环出现异常。文章研究特选择在秋初,湖泊分层开始消失时,测定了湖水中不同深度的N₂O,CH₄,CO₂,有机和无机碳同位素以及其他化学参数变化。结果发现:采样时百花湖在约6m和16m深度附近出现了两个温度不连续层(SDL和PDL),并影响到有机颗粒的沉降和分解。相对而言,有较多的有机质在这两个层内发生降解,但降解的途径有所不同,上部主要是有氧降解,下部则主要是无氧降解过程。N₂O的产生和消耗与有机质的降解过程完全对应:PDL层以上,ΔN₂O与AOU的线性关系反映了N₂O主要形成于硝化作用;PDL层以下反硝化作用导致N₂O严重不饱和;PDL内位于硝化作用和反硝化作用过渡带的N₂O峰,显然是硝化与反硝化联合作用的结果。PDL层内较大的CH₄浓度变化梯度,说明嗜甲烷细菌可能通过氧化NH+4贡献了部分N₂O。百花湖秋、冬季表层湖水N₂O都是过饱和的,都是大气N₂O的源,依据分子扩散模型计算湖泊N₂O的释放通量在12～14μmol/m·day之间,秋、冬季没有明显的差别。秋季底层湖水的反硝化作用是湖泊N₂O的汇,其消耗通量与表层的释放通量基本相当。     

贵州百花湖分层晚期有机质降解过程与溶解N2O循环

百花湖是一个具有季节性分层的富营养小型湖泊,在秋季湖水倒转期经常发生水质恶化事件,碳氮循环出现异常。文章研究特选择在秋初,湖泊分层开始消失时,测定了湖水中不同深度的N₂O,CH₄,CO₂,有机和无机碳同位素以及其他化学参数变化。结果发现:采样时百花湖在约6m和16m深度附近出现了两个温度不连续层(SDL和PDL),并影响到有机颗粒的沉降和分解。相对而言,有较多的有机质在这两个层内发生降解,但降解的途径有所不同,上部主要是有氧降解,下部则主要是无氧降解过程。N₂O的产生和消耗与有机质的降解过程完全对应:PDL层以上,ΔN₂O与AOU的线性关系反映了N₂O主要形成于硝化作用;PDL层以下反硝化作用导致N₂O严重不饱和;PDL内位于硝化作用和反硝化作用过渡带的N₂O峰,显然是硝化与反硝化联合作用的结果。PDL层内较大的CH₄浓度变化梯度,说明嗜甲烷细菌可能通过氧化NH+4贡献了部分N₂O。百花湖秋、冬季表层湖水N₂O都是过饱和的,都是大气N₂O的源,依据分子扩散模型计算湖泊N₂O的释放通量在12～14μmol/m·day之间,秋、冬季没有明显的差别。秋季底层湖水的反硝化作用是湖泊N₂O的汇,其消耗通量与表层的释放通量基本相当。     

河流碳通量与陆地侵蚀研究

河流碳通量系陆地侵蚀产物,它构成全球碳循环的一个重要环节。河流碳通量在数量上远小于全球碳循环的其他环节,但由于与陆地生态系统联系密切,故对它的研究尤为重要。全球每年河流碳通量约为1GtC（10⁹t碳）,其中约60％为无机碳、40％为有机碳。溶解态有机碳和颗粒状有机碳主要来源于土壤侵蚀,另有一部分有机碳来源于河湖中的浮游植物;溶解态无机碳主要源于大气中CO₂和碳酸盐;颗粒无机碳主要指未溶解的碳酸盐。亚洲季风区河流对全球河流碳通量具有较大贡献,而对其研究程度较低。河流碳通量研究既可为流域治理提供基础资料,也是进一步了解人为CO₂“未知汇”的途径之一。     

若尔盖高原沼泽湿地CH4排放研究

若尔盖高原沼泽湿地海拔 3400 m，面积 4038km²，是我国面积最大的高原沼泽湿地分布区。2001年 5～9月的非冰冻期，其主要沼泽类型木里苔草沼泽的CH₄排放通量范围是 0.51～ 8.20 m g/（m ²· h），平均值为 2.87 m g/（m ²· h）；乌拉苔草沼泽CH₄排放通量范围是 0.36～10.04 m g/（m ²· h），平均值为 4.51 m g/（m ²· h）。在空间分布上，不同沼泽类型之间CH₄排放通量具有一定的差异。在季节变化上，没有明显的排放高峰。根据代表性观测点的CH₄平均排放量、日数和沼泽总面积推算，非冰冻期若尔盖高原沼泽湿地CH₄的排放量为 0.052Tg/a。     

腾冲新生代火山区温泉CO2气体排放通量研究

近期研究表明,不仅火山喷发期会向当时的大气圈输送大量的温室气体,火山间歇期同样会释放大量的温室气体。在火山活动间歇期,火山区主要以喷气孔、温(热)泉以及土壤微渗漏等形式向大气圈释放温室气体。腾冲是我国重要的新生代火山区,同时也是重要的水热活动区,那里出露大量的温泉,然而目前未见腾冲火山区温泉气体排放通量的研究报道。本文利用数字皂膜通量仪测量了腾冲新生代火山区温泉中CO₂的排放通量。研究结果表明,腾冲新生代火山区温泉向当今大气圈输送的CO₂通量达3.58×10³ t·a^-1,相当于意大利锡耶纳Bassoleto地热区温泉中CO₂的排放规模。腾冲火山区温泉的CO₂释放通量主要受深部岩浆囊、断裂分布、地下水循环、围岩成分等多方面因素的影响。本文根据温泉中CO₂的排放特征,将腾冲温泉分为南北两区,南区温泉CO₂通量远高于北区的温泉,热海地热区的通量为腾冲CO₂通量的最大值。在北温泉区,CO₂通量主要受控于断裂的分布;而在南温泉区,除受到断裂控制外,热海地热区底部的岩浆囊及其与围岩的相互作用成为CO₂气体的重要物质来源,同时高温的岩浆囊为温泉及CO₂的形成提供了重要热源。     

植物——大气N2O的一个潜在排放源

N₂₂和CH₄的重要温室气体。目前,全球N₂₂₂O不仅是一个普遍存在的自然现象,而且其排放量可达到与土壤排放相比较的水平,因而植物可能是未知的大气N₂O的一个重要排放源;植物排放N₂O受植物的种类、生长发育阶段、养分供给、光照强度及CO₂浓度等因素的影响。     

祁连山大雪山地区大气PM2.5细粒子中可溶性离子特征

为了研究祁连山大雪山地区大气PM_2.5细粒子中可溶性无机离子组分的变化特征, 于2010年7月至2011年7月在祁连山冰川与生态环境综合观测站附近采集46个大气PM_2.5的Telfon滤膜样品, 并应用离子色谱对可溶性离子进行了分析.结果显示: 所测样品的阴、 阳离子中, SO₄^2-、 NO^-₃、 Ca²⁺和NH⁺₄的质量浓度分别为1.54μg·m^-3、 0.38μg·m^-3、 0.73μg·m^-3和0.22μg·m^-3, 累计约占到水溶性离子总量的88%.可溶性离子浓度呈现出春夏季节明显高于秋冬季节的特征, 夏季的浓度最高, 其次是春季、 冬季和秋季. Cl^-、 Ca²⁺、 Na⁺和Mg²⁺之间的相关性极高, SO₄^2-和NO^-₃与大部分阳离子的相关性都很高, 说明大部分硫酸盐是来自于中亚沙尘源区的自然源, 而并非是通过人类活动造成的一次污染物通过二次反应过程得到的. NH⁺₄仅与SO₄^2-通过相关性检验说明, 该地区NH₃主要中和了大气中硫酸并生成(NH₄)₂SO₄.该地区的大气环境主要来源于自然源的影响, 但夏季风期间人为污染排放已经不可忽视, 这也得到HYSPLIT后向轨迹模式的计算验证.     

土壤温室气体昼夜变化及其环境影响因素研究

通过对北京东灵山草地和桦树林土壤气体CO₂,N₂O和CH₄浓度及其排放通量的昼夜连续观测,探讨了生长季节草地和森林土壤温室气体昼夜变化及其环境影响因素。研究表明:1)土壤CO₂排放通量昼高夜低,N₂O排放通量有明显小时尺度波动,但昼夜变化不突出;土壤CO₂和N₂O浓度昼夜变化不明显,且与排放通量波动不一致;土壤是大气CH₄的一个汇,相对厌氧的环境可能有利于土壤吸收CH₄。2)无雨时气温昼夜变化通过影响土壤表层的气体扩散和CO₂产生过程,来影响土壤CO₂和N₂O的地表排放通量,而对土壤10cm以下CO₂和N₂O的产生影响不大。小时尺度的土壤CO₂和N₂O浓度波动则可能还有其他影响因素或机制。3)降雨时土壤渗水引起的土壤空气对流取代气体浓度扩散成为土壤与大气空气交换的主要方式,导致土壤CO₂和N₂O排放通量的同步波动。降雨渗水较多时,较多的溶解氧随着雨水进入土壤内,会促进土壤CO₂的生成和抑制N₂O的产生。4)土壤CO₂与N₂O浓度存在显著的正相关关系,反映出土壤CO₂和N₂O有相对稳定的产率比。土壤有效碳可能是造成土壤CO₂与N₂O浓度正相关的主要原因,土壤空气的氧分压则可能是造成土壤CO₂和N₂O浓度波动不一致的重要因素。     

流体包裹体盐度低温拉曼光谱测定方法研究

氯盐溶液作为流体包裹体中最普遍和最重要的盐水化合物,是测定包裹体盐水溶液含盐度的主要溶质,但由于其强离子键化合物的分子特性在常温、常压下没有拉曼效应,拉曼光谱测试无法获取氯盐的有效特征信息,使得利用拉曼光谱研究流体包裹体分子组分及含盐度的方法存在严重缺陷。本文联合利用激光拉曼光谱探针和冷热台,原位采集了不同盐度的NaCl-H₂O和CaCl₂-H₂O标准盐水溶液在低温下(-185℃)形成的冰、NaCl水合物和CaCl₂水合物的拉曼光谱,分析了不同盐度标准盐水溶液形成的水合物拉曼特征峰的变化规律,尝试建立流体包裹体盐度低温拉曼光谱测定方法。分析表明,NaCl水合物约3425 cm^-1拉曼特征峰与冰约3120 cm^-1拉曼特征峰峰面积比值和配制的NaCl-H₂O标准溶液盐度呈良好的正相关(r²=0.9995),CaCl₂水合物约3431 cm^-1拉曼特征峰与冰约3120 cm^-1拉曼特征峰峰面积比值也和配制的CaCl₂-H₂O标准溶液盐度呈较好的正相关(r²=0.9458)。利用愈合人工水晶法合成的NaCl-H₂O和CaCl₂-H₂O包裹体标样检验了用上述方法低温测定流体包裹体盐度的可靠性,结果表明该技术用于盐度大于0.5 mol/L的NaCl-H₂O体系流体包裹体时,数据精度好于20%;用于盐度大于0.5 mol/L的CaCl₂-H₂O体系流体包裹体时,数据精度最高可达5%,完全可达到半定量-定量测定的要求。研究还发现,包裹体内压可能对低温拉曼光谱测定流体包裹体盐度影响不大,分析中获得的冰拉曼特征峰的拉曼位移(约3120 cm^-1)与前人略有差异,可能与实验条件下获得的冰的多型不同有关。与国内外同行的研究结果比较,本研究更加注重该项实验技术的实际应用,通过对不同体系盐水溶液系列进行拉曼光谱实验分析,对实验条件和方法进行不断优化,在确定流体体系的同时实现了包裹体盐水溶液盐度半定量-定量测定,准确度优于传统方法,并且该方法具有很强的实用性。     

Effects of nitrogen on the ecosystem respiration,CH<Subscript>4</Subscript> and N<Subscript>2</Subscript>O emissions to the atmosphere from the freshwater marshes in northeast China

Freshwater marshes could be a source of greenhouse gases emission because they contain large amounts of soil carbon and nitrogen. These emissions are strongly influenced by exogenous nitrogen. We investigate the effects of exogenous nitrogen on ecosystem respiration (CO₂), CH₄ and N₂O emissions from freshwater marshes in situ in the Sanjiang Plain Northeast of China during the growing seasons of 2004 and 2005, using a field fertilizer experiment and the static opaque chamber/GC techniques. The results show that there were no significant differences in patterns of seasonal variations of CO₂ and CH₄ among the fertilizer and non-fertilizer treatments, but the seasonal patterns of N₂O emission were significantly influenced by the exogenous nitrogen. Seasonal averages of the CO₂ flux from non-fertilizer and fertilizer were 987.74 and 1,344.35 mg m ⁻² h ⁻¹, respectively, in 2004, and 898.59 and 2,154.17 mg m ⁻² h ⁻¹, respectively, in 2005. And the CH₄ from the control and fertilizer treatments were 6.05 and 13.56 mg m ⁻² h ⁻¹ and 0.72 and 1.88 mg m ⁻² h ⁻¹, respectively, in 2004 and 2005. The difference of N₂O flux between the fertilizer and non-fertilizer treatments is also significant either in 2004 and 2005. On the time scale of 20-, 100-, and 500-year periods, the integrated global warming potential (GWP) of CO₂ + CH₄ + N₂O released during the two growing seasons for the treatment of fertilizer was 97, 94 and 89%, respectively, higher than that for the control, which suggested that the nitrogen fertilizer can enhance the GWP of the CH₄ and N₂O either in long time or short time scale.     

WMO区域本底站气溶胶特征分析*

文章通过2002年8月12~27日和2003年7月20日~8月1日在浙江临安县的WMO区域空气污染本底站临安站所采集的气溶胶样品的质量浓度,水溶性离子,有机碳/元素碳(OC/EC)及部分化学元素的特征分析,并与1991年夏季(8月22~28日)气溶胶的某些特征比较,初步研究结果为:1991年至2003年夏季的气溶胶TSP,PM11和PM2.1浓度均呈现出减少的趋势,但是PM11/TSP和PM2.1/PM11则有增加的趋势。1991年、2002年和2003年PM11/TSP的值为90 % 左右,PM2.1/PM11 分别为46.52 % , 69.33 % 和72.29 % ,说明气溶胶以小粒子为主,小粒子又以细粒子为主。1991年、2002年和2003年浓度最高的离子为SO^2-₄,其次为NH^＋₄。其中SO^2-₄占所测离子浓度的百分数分别为65.39 % ,57.75 % 和57.27 % ,并且主要以(NH₄)₂SO₄,(K)₂SO₄和(Na)₂SO₄的形式存在。各离子浓度占所测离子浓度的百分数基本上不随年代变化,具有一定稳定性。2002年和2003年气溶胶中的OC浓度分别为29.91μg/m³和14.14μg/m³,均为各自的组分之首。2002年和2003年OC的比值PM2.1/PM11分别为64.63 % 和77.71 % ,EC的比值PM2.1/PM11分别为69.89 % 和87.17 % ,可见气溶胶中OC和EC主要存在于PM2.1的粒子中。元素富集因子分析表明,自然源与人为源对气溶胶中的元素都有重要的贡献。主因子分析结果显示PM2.1和PM11元素源基本相同,自然源主要是地壳、土壤尘和海盐, 人为源主要是煤飞灰(煤和焦碳)、冶炼工业和道路机动车辆的排放、废物处理、垃圾焚烧及建筑工业粉尘等。     

Nitrous oxide (N<Subscript>2</Subscript>O) emissions from a mesotrophic reservoir on the Wujiang River,southwest China

Aquatic ecosystems have been identified as a globally significant source of nitrous oxide (N₂O) due to continuous active nitrogen involvement, but the processes and influencing factors that control N₂O production are still poorly understood, especially in reservoirs. For that, monthly N₂O variations were monitored in Dongfeng reservoir (DFR) with a mesotrophic condition. The dissolved N₂O concentration in DFR displayed a distinct spatial–temporal pattern but lower than that in the eutrophic reservoirs. During the whole sampling year, N₂O saturation ranging from 144% to 640%, indicating that reservoir acted as source of atmospheric N₂O. N₂O production is induced by the introduction of nitrogen (NO₃ ^?, NH₄ ⁺) in mesotrophic reservoirs, and is also affected by oxygen level and water temperature. Nitrification was the predominate process for N₂O production in DFR due to well-oxygenated longitudinal water layers. Mean values of estimated N₂O flux from the air–water interface averaged 0.19 µmol m^?2 h^?1 with a range of 0.01–0.61 µmol m^?2 h^?1. DFR exhibited less N₂O emission flux than that reported in a nearby eutrophic reservoir, but still acted as a moderate N₂O source compared with other reservoirs and lakes worldwide. Annual emissions from the water–air interface of DFR were estimated to be 0.32 × 10⁵ mol N–N₂O, while N₂O degassing from releasing water behind the dam during power generation was nearly five times greater. Hence, N₂O degassing behind the dam should be taken into account for estimation of N₂O emissions from artificial reservoirs, an omission that historically has probably resulted in underestimates. IPCC methodology should consider more specifically N₂O emission estimation in aquatic ecosystems, especially in reservoirs, the default EF5 model will lead to an overestimation.     

Nitrogen and oxygen isotopic compositions of water-soluble nitrate in Taihu Lake water system, China: implication for nitrate sources and biogeochemical process

The stable isotope nitrogen-15 (¹⁵N) is a robust indicator of nitrogen (N) source, and the joint use of δ¹⁵N and δ¹⁸O–NO₃ ^? values can provide more useful information about nitrate source discrimination and N cycle process. The δ¹⁵N and δ¹⁸O–NO₃ ^? values, as well as major ion tracers, from Taihu Lake in east China were investigated to identify the primary nitrate sources and assess nitrate biogeochemical process in the present study. The results show that the nitrate concentration in West Taihu Lake (WTL) was generally higher than those in East Taihu Lake (ETL) and its upstream inflow rivers. The NO₃ ^?/Cl^? value combined with mapping of δ¹⁵N–NO₃ ^? and NO₃ ^? concentration suggest that the mixing process should play a major effect in WTL, and denitrification was the dominant N transformation process in WTL. A linear relationship of close to ~1: 2 was observed between δ¹⁵N–NO₃ ^? and δ¹⁸O–NO₃ ^? values in WTL, confirming the occurrence of denitrification in WTL. The δ¹⁵N–NO₃ ^? data imply that sewage and manure were the principal nitrate sources in WTL and its feeder rivers, while the nitrate in ETL might derive from soil organic nitrogen and atmospheric deposition. The δ¹⁸O–NO₃ ^? data indicate most of nitrate from microbial nitrification of organic nitrogen matter possibly make a significant contribution to the lake.     

A review on the mechanism and affecting factors of nitrous oxide emission in constructed wetlands

Constructed wetlands (CWs) are considered important sources of nitrous oxide (N₂O). Various reports in the literature indicate that CWs have high N₂O emission rates. The release of N₂O from CWs treating wastewater emissions range from ?16.7 to 188 mg N₂O m^?2day^?1. N₂O in CWs is produced mainly by nitrification, denitrification, nitrifier denitrification, and nitrate-ammonification. Denitrification is considered the major source of N₂O under most conditions. In recent years, two main methods of sampling N₂O gas in CWs have been employed, including the headspace equilibration technique and the closed static chambers technique. N₂O emission may be affected by various operating parameters and environmental conditions. One of the main environmental factors affecting the removal of nitrogen in CWs is dissolved oxygen, which affects nitrification and denitrification processes, thus greatly influencing N₂O emission. CW gas dynamics is affected mainly by season and weather conditions, especially temperature and moisture. Aquatic plants, flow regime, oxidation–reduction potential, nitrate concentration, C/N ratio and other factors can affect N₂O emission in CWs.     

Nitrous oxide emission from Gulf Coast wetlands

Nitrous oxide evolution may contribute to partial destruction of the ozone layer in the stratosphere. A two year study of the release of N₂O from adjoining salt, brackish, and fresh marsh sediment indicates that the annual emission was 31, 48, and 55 mg N m^?2 respectively. Emission from open water area was less than the corresponding emission from the marsh sediment. In vitro experiments indicate that the N₂O emission was increased when the sediment was drained for extended periods of time. The addition of NO₃^? significantly increased the rate of N₂O evolution, indicating that a large potential for denitrification exists in the anoxic sediment. Appreciable losses of N₂O would only be expected when the marshes receive an extraneous source of nitrate such as sewage and/or wastewater.The contribution of the Gulf Coast wetlands to the atmospheric N₂O balance is estimated to be 3.3 × 10⁹ g N₂O. The maximum average daily emission was equivalent to 1.5 g N₂O-N ha^?1, which is less than the measured emission from uncultivated soils (Mosieret al., 1981) but greater than the estimates from noncropped land (CAST, 1976).     

Denitrification and N2O production in near-shore marine sediments

Methods were developed for determining rates of denitrification in coastal marine sediments by measuring the production of N₂ from undisturbed cores incubated in gas-tight chambers. Denitrification rates at summer temperatures (23°C) in sediment cores from Narragansett Bay, Rhode Island, were about 50μmol N₂m^?2 hr^?1. This nitrogen flux is equal to approximately one-half of the NH⁺₄flux from the sediments at this temperature and is of the magnitude necessary to account for the anomalously low N/P and anomalously high O/N ratios often reported for benthic nutrient fluxes. The loss of fixed nitrogen as N₂ during the benthic remineralization of organic matter, coupled with the importance of benthic remineralization processes in shallow coastal waters may help to explain why the availability of fixed nitrogen is a major factor limiting primary production in these areas. Narragansett Bay sediments are also a source of N₂O, but the amount of nitrogen involved was only about 0.2 μmol m^?2 hr^?1 at 23°C.