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1.
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2.
采用漂浮通量箱法和扩散模型法同步地观测了模拟内陆水体在不同条件下的CH4和N2O的水-气交换通量,旨在比较两类方法取得结果的异同。结果显示:这两类方法所测得的绝大多数CH4排放通量都与水中溶解氧呈显著线性负相关(显著性系数P0.001)。同时N2O排放通量与表层水温及水中铵态氮、硝态氮、溶解碳和溶解氧的关系可用包含所有上述水环境因素的Arrhenius动力学方程来表达,这些因素可以共同解释86%~90%的N2O通量变化(P0.0001),且不同方法测定的N2O通量的表观活化能和对表层水温的敏感系数分别介于47~59 kJ mol-1和1.92~2.27之间;扩散模型法所获得的CH4和N2O通量分别是箱法测定值的13%~175%和15%~240%,差异程度因模型而异;不同模型取得通量间相差20%~1200%,平均相差2.3倍。上述结果表明:仅用一种模型方法来取得CH4或N2O排放通量易形成较大偏差;不同扩散模型法和箱法测定的通量在反映CH4和N2O排放的内在规律方面具有一致性,但它们对真实气体通量的测量是否都存在不同程度的系统误差,尚需进一步研究。  相似文献   

3.
Gas exchange experiments were conducted in the tropical Atlantic Ocean during a ship expedition with FS Meteor using a small rubber raft. The temporal change of the mixing ratios of CO, H2, CH4 and N2O in the headspace of a floating glass box and the concentrations of these gases in the water phase were measured to determine their transfer velocities across the ocean-atmosphere interface. The ocean acted as a sink for these gases when the water was undersaturated with respect to the mixing ratio in the headspace. The transfer velocities were different for the individual gases and showed still large differences even when normalized for diffusivity. Applying the laminar film model, film thicknesses of 20 to 70 m were calculated for the observed flux rates of the different gas species. When the water was supersaturated with respect to atmospheric CO, H2, CH4 and N2O, the transfer velocities of the emission process were smaller than those determined for the deposition process. In case of H2 and CH4, emission was even not calculable although, based on the observed gradient, the laminar film model predicted significant fluxes at the air-sea interface. The results are interpreted by destruction processes active within the surface microlayer.  相似文献   

4.
CH4和N2O作为主要温室气体,自工业革命以来排放量急剧增加,已经被列入《京都议定书》要求控制它们的排放。本文利用高光谱分辨率的辐射传输模式,计算了CH4、N2O在晴空大气和有云大气条件下的瞬时辐射效率和平流层调整的辐射效率,以及它们的全球增温潜能(GWP)和全球温变潜能(GTP),并根据模式结果拟合了CH4和N2O的辐射强迫的简单计算公式。本文的研究表明:CH4和N2O在有云大气下的平流层调整的辐射效率分别为4.142×10-4 W m-2 ppb-1和3.125×10-3 W m-2 ppb-1 (1ppb=10-9),经大气寿命调整后的辐射效率分别为3.732×10-4 W m-2 ppb-1和2.987×10-3 W m-2 ppb-1,与IPCC(2007)的相应结果高度一致。CH4和N2O 100年的全球增温潜能GWP分别为16和266;100年的脉冲排放的全球温变潜能GTPP分别为0.24和233;持续排放的全球温变潜能GTPS分别为18和268。它们在未来全球变暖和气候变化中,影响仅次于CO2,仍然起着非常关键的作用。  相似文献   

5.
Carbonyl sulfide emissions from biomass burning have been studied during field experiments conducted both in an African savanna area (Ivory Coast) and rice fields, central highland pine forest and savanna areas in Viet-Nam. During these experiments CO2, CO and C2H2 or CH4 have also been also monitored. COS values range from 0.6 ppbv outside the fires to 73 ppbv in the plumes. Significant correlations have been observed between concentrations of COS and CO (R 2=0.92,n=25) and COS and C2H2 (R 2=0.79,n=26) indicating a COS production during the smoldering combustion. COS/CO2 emission factors (COS/CO2) during field experiments ranged from 1.2 to 61×10–6 (11.4×10–6 mean value). COS emission by biomass burning was estimated to be up to 0.05 Tg S/yr in tropics and up to 0.07 Tg S/yr on a global basis, contributing thus about 10% to the global COS flux. Based on the S/C ratio measured in the dry plant biomass and the COS/CO2 emission factor, COS can account for only about 7% of the sulfur emitted in the atmosphere by biomass burning.  相似文献   

6.
A method for the estimation of the reaction probability of the heterogeneous N2O5+H2O 2HNO3 reaction using the deposition profile in a laminar flow tube, in which the walls are coated with the condensed aqueous phase of interest, is presented. The production of gas phase nitric acid on the surface followed by its absorption complicates the deposition profiles and hence the calculation of the reaction probability. An estimation of the branching ratio for this process enables a more appropriate calculation to be carried out. Reaction probabilities of N2O5 on substances including some normally constituting atmospheric aerosols, NaCl, NH4HSO4, as well as Na2CO3 are estimated and found to depend on relative humidity and characteristics of the coating used. These fell within the range (0.04–2.0)×10–2.  相似文献   

7.
We measured CO2, CO, CH4, H2, and NO2 in air masses polluted by savanna fires over Côte d'Ivoire, western Africa. Elevated concentrations of these trace gases were found in fire plumes and also in extensive haze layers. Trace gas mixing ratios ranged as high as 605 ppmv for CO2, 14.8 ppmv for CO, 2.7 ppmv for CH4, 4.2 ppmv for H2, and 25 ppbv for NO2. We compare our emission ratios to those obtained in previous field and laboratory studies. The emission ratios, expressed as an average and as a range or as an average only, were: dCO/dCO2 5.3×10–2 (3–18×10–2); dCH4/dCO 5.3×10–2; dH2/dCO 2.4×10–1 and dNO2/dCO2 1.8×10–4 (1.5–2.2×10–4). The values found match those found during similar measurements, though our results point to rather vigorous burning in the savanna of western Africa.  相似文献   

8.
Generally, it is assumed that UV-light, high temperature or reactive molecules like O3 and OH are needed to activate gas reactions in air. In consequence, the catalytic activity on natural materials such as sand and soil on the earth's surface is assumed to be insignificant. We have measured O2-dissociation rates on natural quartz sand at 40˚C and compared these with O2-dissociation rates near 500˚C on materials with well-known catalytic activity. In terms of probabilities for dissociation of impinging O2-molecules the measured rates are in the 10−12–10−4 range. We have also measured dissociation rates of H2 and N2, water-formation from H2 and O2 mixtures, exchange of N between N2, NO x and a breakdown of HNO3, NO2 and CH4 on natural quartz sand at 40˚C. The measured rates together with an effective global land area have been used to estimate the impact of thermodynamically driven reactions on the earth's surface on the global atmospheric budgets of H2, NO2 and CH4. The experimental data on natural quartz sand together with data from equilibrium calculations of air suggest that an expected increase in anthropogenic supply of air pollutants, such as NO x or other “reactive” nitrogen compounds, hydrogen and methane, will be counter-acted by catalysis on the earth's surface. On the other hand, at Polar Regions and boreal forests where the “reactive” nitrogen concentration is below equilibrium, the same catalytic effect activates formation of bio-available nitrogen compounds from N2, O2 and H2O.  相似文献   

9.
Emission of nitrous oxide from temperate forest soils into the atmosphere   总被引：5，自引：0，他引：5  
N2O emission rates were measured during a 13-month period from July 1981 till August 1982 with a frequency of once every two weeks at six different forest sites in the vicinity of Mainz, Germany. The sites were selected on the basis of soil types typical for many of the Central European forest ecosystems. The individual N2O emission rates showed a high degree of temporal and spatial variabilities which, however, were not significantly correlated to variabilities in soil moisture content or soil temperatures. However, the N2O emission rates followed a general seasonal trend with relatively high values during spring and fall. These maxima coincided with relatively high soil moisture contents, but may also have been influenced by the leaf fall in autumn. In addition, there was a brief episode of relatively high N2O emission rates immediately after thawing of the winter snow. The individual N2O emission rates measured during the whole season ranged between 1 and 92 g N2O-N m–2 h–1. The average values were in the range of 3–11 g N2O-N m–2 h–1 and those with a 50% probability were in the range of 2–8 g N2O-N m–2 h–1. The total source strength of temperate forest soils for atmospheric N2O may be in the range of 0.7–1.5 Tg N yr–1.  相似文献   

10.
We present an approach for assessing the impact of systematic biases in measured energy fluxes on CO2 flux estimates obtained from open-path eddy-covariance systems. In our analysis, we present equations to analyse the propagation of errors through the Webb, Pearman, and Leuning (WPL) algorithm [Quart. J. Roy. Meteorol. Soc. 106, 85–100, 1980] that is widely used to account for density fluctuations on CO2 flux measurements. Our results suggest that incomplete energy balance closure does not necessarily lead to an underestimation of CO2 fluxes despite the existence of surface energy imbalance; either an overestimation or underestimation of CO2 fluxes is possible depending on local atmospheric conditions and measurement errors in the sensible heat, latent heat, and CO2 fluxes. We use open-path eddy-covariance fluxes measured over a black spruce forest in interior Alaska to explore several energy imbalance scenarios and their consequences for CO2 fluxes.  相似文献   

11.
The CO2 concentrations and fluxes over an urban forest site (Namsan) and an urban residential region (Boramae) in Seoul, Korea, during the non-growing season (2–4 March 2011), the growing season (10–12 June 2011), and the late-growing season (22–24 September 2011) were analyzed. The CO2 concentrations of two sites showed nearly the same diurnal variation, with a maximum value occurring during the night and a minimum value occurring during daytime, as well as the same seasonal variation, with a maximum value during the non-growing season (early spring) and a minimum value during the growing season (summer). The CO2 flux over the urban forest did not show any typical diurnal variation during the non-growing season, but did show diurnal variation with a small positive value during the night and a large negative value during daytime in the growing and late-growing seasons due to photosynthesis in the urban forest. The CO2 flux over the urban residential region showed a positive daily mean value for all periods, with large values during the non-growing season and small values during the growing season, and it also showed diurnal variation with two maxima at 0600–1000 LST and 1800–2400 LST, and two minima at 0300-0600 LST and 1100-1500 LST, and was strongly correlated with the use of liquefied natural gas for cooking and heating by surrounding houses.  相似文献   

12.
反硝化过程是维系闭合氮循环所必需的氮素形态转化环节。土壤反硝化过程速率及产物比的直接测定是研究氮循环过程机理的基础,但却是一个难题。为解决此难题,德国卡尔斯鲁厄技术研究所与中国科学院大气物理研究所最近合作新建了一套通过氦环境培养-气体同步直接测定土壤反硝化气体--氮气（N2）、氧化亚氮（N2O）、一氧化氮（NO）和二氧化碳（CO2）排放的系统和与之配套的三阶段培养方法。为检验该新建系统和配套方法测定土壤反硝化过程的准确性和可靠性,以华北地区广泛分布的盐碱地农田土壤（采自山西运城）为研究对象开展实验室培养试验,在初始可溶性有机碳（DOC）供应比较充足约300 mgC kg–1干土（d.s.）的条件下,测试了不同初始土壤硝态氮含量水平（10、100 mgN kg–1d.s.左右,分别表示为10N和100N）的反硝化气体和CO2排放过程。结果显示：100N的反硝化速率（定义为N2、N2O 和NO 排放速率之和）显著高于10N 处理（统计检验显著水平p＜0.01）;两个处理的反硝化产物均以N2为主（质量比分别占77%和75%）,产物的NO/N2O摩尔比分别为1.2和1.5,N2O/N2摩尔比均为0.19;土壤反硝化气体动态排放速率及相关指标的测定结果表明,培养土壤中消失的硝态氮被回收81%～87%,培养前后的氮平衡率达92%～95%。因此,该新建方法测定土壤反硝化速率和产物比的结果具有很好的可靠性,为定量研究土壤反硝化过程提供了有效的直接测定手段。研究中检测到的土壤反硝化产物NO/N2O摩尔比大于1,不同于以往用液体培养基纯培养反硝化细菌得出的NO/N2O摩尔比远小于1的结论。这意味着,不能用NO/N2O摩尔比小于1与否来推断土壤排放的N2O和NO是主要来源于反硝化作用还是硝化作用。  相似文献   

13.
Increased precipitation during the vegetation periods was observed in and further predicted for Inner Mongolia. The changes in the associated soil moisture may affect the biosphere-atmosphere exchange of greenhouse gases. Therefore, we set up an irrigation experiment with one watered （W） and one unwatered plot （UW） at a winter-grazed Leymus chinensis-steppe site in the Xilin River catchment, Inner Mongolia. UW only received the natural precipitation of 2005 （129 mm）, whereas W was additionally watered after the precipitation data of 1998 （in total 427 mm）. In the 3-hour resolution, we determined nitrous oxide （N20）, methane （CH4） and carbon dioxide （CO2） fluxes at both plots between May and September 2005, using a fully automated, chamber-based measuring system. N20 fluxes in the steppe were very low, with mean emissions （±s.e.） of 0.9-4-0.5 and 0.7-4-0.5 μg N m^-2 h^-1 at W and UW, respectively. The steppe soil always served as a CH4 sink, with mean fluxes of -24.1-4-3.9 and -31.1-4- 5.3 μg C m^-2 h^-1 at W and UW. Nighttime mean CO2 emissions were 82.6±8.7 and 26.3±1.7 mg C m^-2 h^-1 at W and UW, respectively, coinciding with an almost doubled aboveground plant biomass at W. Our results indicate that the ecosystem CO2 respiration responded sensitively to increased water input during the vegetation period, whereas the effects on CH4 and N2O fluxes were weak, most likely due to the high evapotranspiration and the lack of substrate for N2O producing processes. Based on our results, we hypothesize that with the gradual increase of summertime precipitation in Inner Mongolia, ecosystem CO2 respiration will be enhanced and CH4 uptake by the steppe soils will be lightly inhibited.  相似文献   

14.
Field measurements of N2O emission rates were carried out from August until October 1982 in a subtropical region in Europe, i.e. in Andalusia, Spain. The measurements were performed by using an automatic sampling and analysis technique allowing the semi-continuous determination of N2O emission rates. The N2O emission rates were positively correlated to the soil surface temperature and exhibited a diurnal rhythm with maximum rates in the afternoon and minimum rates in the early morning with average values of 1 g N2O–N/m2/h for the grass lawn and 15 g N2O–N/m2/h for cultivated land. Application of urea and ammonium nitrate resulted in elevated N2O emission rates when compared to the unfertilized control. The loss of fertilizer-nitrogen as N2O was 0.18% for urea and 0.04% for NH4NO3 which compares very well with data obtained in a temperate climate (Germany). The total source strength of fertilizer-derived N2O is estimated to be 0.01–2.2 Tg N2O–N per year. The N2O flux from unfertilized natural soils may be as high as 4.5 Tg N2O–N, indicating that the N2O emission from soils contributes significantly to the global N2O budget.  相似文献   

15.
Anthropogenic emissions of methane (CH4) and nitrous oxide (N2O) from livestock agriculture (enteric fermentation, animal waste management systems, and pasture manure) and plant growing of the Russia (CH4 emissions from rice fields, direct and indirect N2O emissions from agricultural lands) are considered. In 2004, the total emissions of these greenhouse gases in the agricultural sector amounted to 1.4 × 105 thousand t CO2-equivalent, which corresponds to 45% of the 1990 level (3.1 × 105 thousand t CO2-equivalent). In 2004, the contribution of N2O to the total agricultural emissions was approximately twice (67.0%) that of CH4 (33.0%). Direct N2O emissions from agricultural soils (0.5 × 105 thousand t CO2-equivalent) and CH4 emissions from the internal fermentation of domestic animals (0.4 × 105 thousand t CO2-equivalent) are the most significant sources in the agricultural sector of the Russian Federation. In 2004, all these agricultural sources emitting methane and nitrous oxide contributed about 7% CO2-equivalent to the total emission of the anthropogenic greenhouse gases in Russia.  相似文献   

16.
In a nighttime system and under relatively dry conditions (about 15 ppm H2O), the reaction mixture of NO2, O3, and NH3 in purified air turns out to result in the formation of nitrous oxide (N2O). The experiments were performed in a continuous stirred flow reactor, in the concentration region of 0.02–2 ppm.N2O is thought to arise through the heterogeneous reaction of gaseous N2O5 and absorbed NH3 at the wall of the reaction vessel % MathType!MTEF!2!1!+-% feaafeart1ev1aaatCvAUfeBSjuyZL2yd9gzLbvyNv2CaerbuLwBLn% hiov2DGi1BTfMBaeXatLxBI9gBaerbd9wDYLwzYbItLDharqqtubsr% 4rNCHbGeaGqiVu0Je9sqqrpepC0xbbL8F4rqaqpepeea0xe9qqVa0l% b9peea0lb9sq-JfrVkFHe9peea0dXdarVe0Fb9pgea0xa9pue9Fve9% Ffc8meGabaqaciGacaGaaeqabaWaaeaaeaaakeaatCvAUfKttLeary% qr1ngBPrgaiuaacqWFOaakcqWFobGtcqWFibasdaWgaaWcbaGae83m% amdabeaakiab-LcaPmaaBaaaleaacqWFHbqyaeqaaOGaey4kaSIaai% ikaiab-5eaonaaBaaaleaacqWFYaGmaeqaaOGae83ta80aaSbaaSqa% aiab-vda1aqabaGccaGGPaWaaSbaaSqaaiaadEgaaeqaaOGaeyOKH4% Qae8Nta40aaSbaaSqaaiab-jdaYaqabaGccqWFpbWtcqGHRaWkcqWF% ibascqWFobGtcqWFpbWtdaWgaaWcbaGae83mamdabeaakiabgUcaRi% ab-HeainaaBaaaleaacqWFYaGmaeqaaOGae83ta8eaaa!59AC!\[(NH_3 )_a + (N_2 O_5 )_g \to N_2 O + HNO_3 + H_2 O\]In principle, there is competition between this reaction and that of adsorbed H2O with N2O5, resulting in the formation of HNO3. At high water concentrations (RH>75%), no formation of N2O was found. Although the rate constant of adsorbed NH3 with gaseous N2O5 is much larger than that of the reaction of adsorbed H2O with gaseous N2O5, the significance of the observed N2O formation for the outside atmosphere is thought to be dependent on the adsorption properties of H2O and NH3 on a surface. A number of NH3 and H2O adsorption measurements on several materials are discussed.  相似文献   

17.
基于典型城市站太原站2018年3月—2019年2月的大气CO2在线观测资料,利用筛分法(Meteorological filtering method, MET)和黑碳示踪法(Black Carbon tracer, BC)进行本底/非本底的筛分,得到了本底浓度的变化特征。结果表明,太原大气CO2浓度季均值冬季最高,夏季最低;不同季节呈“单峰型”日变化特征,日振幅均在26.0×10-6以上;4个季节CO2浓度与地面风速存在显著负相关关系;CO2浓度抬升区域主要受当地工业布局的影响,最大抬升幅度在秋季达17.4×10-6;使用气象筛分法(MET)得到年均本底浓度为(431.4±19.9)×10-6,人为排放等对其影响为23.5×10-6,年振幅比同纬度其它本底站大,为34.5×10-6;黑碳示踪法(BC)得到冬季季均本底浓度为(445.0±22.9)×10-6,比MET筛...  相似文献   

18.
净生态系统碳通量(NEE)的计算对于准确模拟区域碳通量和大气CO2浓度的时空变化至关重要。本文利用中尺度大气-温室气体耦合模式WRF-GHG(Weather Research and Forecasting Model with Greenhouse Gases Module),对2010年7月28日至2010年8月2日期间影响长江三角洲地区大气CO2浓度及时空分布的各种过程进行了详尽模拟。结果表明,植被光合呼吸模型(VPRM)能模拟不同植被下垫面NEE的日变化;WRF-GHG模拟的大气CO2浓度日变化与观测相吻合,但低估了大气CO2浓度5~15 ppm(ppm表示10-6),这可能与人为排放源的低估、VPRM参数的不确定性以及气象场模拟的不准确性有关。太湖和植被覆盖较好的地区如浙江北部山区是该地区的主要碳汇,而城市为CO2的主要排放源。太湖和陆地生态系统对区域内碳循环起到一定的调节作用,减缓区域大气CO2浓度的升高。此外,局地气象条件如湖陆风对太湖周边地区大气CO2浓度有显著影响。  相似文献   

19.
In the tropical rain forests of the Congo during the dry season, from June to September 1987, carboxylic acid partial pressures (P gas) in the air above the canopy, at ground level, and at the boundary layer, were estimated from water samples such as fog and rainwater. The concentrations of these acids were also measured in the sap of tree leaves. Tree leaves act as a sink or as a source if the acid P gas is greater of lower than the acid concentrations in molecular form in sap. For each of these soluble gases, there is a value of P gas where the exchange is nul. This is called the compensation point. Values of the compensation point for some tree leaves were evaluated according to Henry's law. Henry's law coefficients at ppm levels were redetermined for formic (HCOOH), acetic (CH3COOH), propionic (CH3CH2COOH), and isobutyric (CH3CH(CH3)COOH) acids.By comparison of P gas and compensation points, it is concluded that the forest was a potential source for these acids. The soil-or the litter-acts as a significant source of a carboxylic acid of C3 or C4 atoms in the aliphatic chain. This carboxylic acid, not yet fully characterized, could play an important role in the rain acidity in forested zones of the equatorial areas.The direct emission of these carboxylic acids by vegetation was the main source in the boundary layer above the forest. The average emissions were 3.1×109, 7.8×109, and 8.4×109 molecules cm-2 s-1 for HCOOH, CH3COOH, and CH3CH2COOH, respectively. The savanna is an exogenous source of HCOOH and CH3CH2COOH during moderately rainy days for 30% of the time. The ozonolysis of isoprene seems to be a small source of HCOOH.  相似文献   

20.
From the IGAC-DEBITS Africa network (IDAF), data sets on precipitation chemistry collected from the ‘wet savanna ecosystem’ site of Lamto (Côte d'Ivoire), are analyzed (1995–2002). Inorganic (Ca2 +, Mg2 +, Na+, K+, NH4 +, Cl?, SO4 2 ?, NO3 ?) and organic (HCOO?, CH3COO?) ions content were determined using Ion Chromatography. The analyzed 631 rainfall events represent 8420.9 mm of rainfall from a 9631.1 mm total. The precipitation chemistry at Lamto is influenced by four main sources: natural biogenic emissions from savanna soils (NO x and NH3), biomass burning (savanna and domestic fires), terrigeneous particles emissions from dry savanna soils, and marine compounds embedded in the summer monsoon. The inter-annual variability of the weighted volume mean concentration of chemical species linked with wet deposition fluctuates by ～ 20% over the period. Ammonium concentration is found to be the highest (17.6 μ eq.l? 1) from all IDAF sites belonging to the West Africa ecosystems. Ammonia sources are from domestic animals, fertilizers and biomass burning. In spite of the high potential acidity of 30.5 μ eq.l? 1 from NO3 ?, SO4 2 ?, HCOO? and CH3COO?, a relatively weak acidity is measured: 6.9 μ eq.l? 1. The 40% acid neutralization is explained by the acid gas – alkaline soil particles interaction. The remaining neutralization is from inclusion of gaseous ammonia. When results from Lamto, are compared with those from Banizoumbou (dry savanna) and Zoetele (equatorial forest), a regional view for wet tropospheric chemistry processes is obtained. The high concentration of the particulate phase in precipitation emphasizes the importance of multiphases processes between gases and particles in the atmospheric chemistry of the West Africa ecosystems. For example, the nss Ca2 + precipitation content, main indicator of terrigeneous particles, goes from 30.8 μ eq.l? 1 in dry savanna to 9.2 μ eq.l? 1 at Lamto and 8.9 μ eq.l? 1 in the Cameroon forest. A similar gradient is obtained for rainfall mineral particles precipitation content with contribution of 80% in dry savanna, 40% in wet savanna, and 20% in the equatorial forest.  相似文献   

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