藻型湖区氧化亚氮排放特征及其影响因素

湖泊等内陆水体是大气N₂O潜在的重要排放源,也是全球N₂O收支估算的重要组成部分。目前全球湖泊普遍面临富营养化和蓝藻暴发等问题,明晰藻型湖泊N₂O排放强度及其环境影响因子对准确估算湖泊N₂O排放和预测其未来变化至关重要。本研究选择太湖藻型湖区为研究对象,同时选取人为活动影响较小的湖心区作为对比区域,基于2011年8月至2013年8月为期2年的逐月连续观测,探讨藻型湖区N₂O排放特征及其影响因素。结果表明,藻型湖区呈现极强的N₂O排放,其排放通量为(4.88±3.05) mmol/(m²·d),是参考区域(湖心:(2.10±4.31) mmol/(m²·d))的2倍多。此外,在藻型湖区中不同点位N₂O排放差异显著,受河流外源输入影响,近岸区是N₂O的热点排放区,其年均排放通量高达10.93 mmol/(m²·d)。连续观测表明N₂     

Nitrous Oxide Emissions in Sewer Systems

Nitrous oxide emissions from urban wastewater were measured in a combined sewer in Bayreuth, Germany. The closed-chamber method was used to evaluate N₂O emissions. Nitrous oxide was analysed by gas chromatography with electron capture detector. Longitudinal and daily variations of N₂O fluxes were determined. N₂O emissions ranged from 0.11…3.8 mg m^?2 h^?1 depending on the level of wastewater in the sewer. Data indicate that N₂O is mainly formed in the biofilm by nitrification and/or denitrification. In laboratory experiments, samples with wastewater and wastewater/biofilm mixture were incubated with and without NaCl. After two hours of incubation, N₂O release was in a range of 42…429 ng N₂O per millilitre wastewater or wastewater/biofilm. Incubated samples without NaCl addition showed no significant difference between wastewater and wastewater/biofilm mixture. If salt (NaCl) was added before incubation, samples with wastewater/biofilm mixture emitted 4.8 times more N₂O than wastewater samples. It is assumed that high concentrations of NaCl inhibit further microbial reduction of N₂O to N₂. Based on the field data, a first estimate for N₂O emission from sewers is 3.5 g N₂O per year and person.     

湖、库水体N2O排放研究进展

湖、库水体是重要的N₂O排放源,在全球氮素循环及全球气候变化中具有重要作用.本文综述了目前有关湖、库水体N₂O排放研究进展,重点介绍湖、库水体N₂O产生和排放的过程、不同时空尺度的排放特征、N₂O排放的影响因子框架及监测方法.湖、库水体N₂O不仅源于内部微生物硝化作用、反硝化作用、硝化-反硝化耦合作用、脱氮作用以及极少数底栖无脊椎动物代谢过程,同时流域上游河流汇入、地表径流输入、污水排放以及地下水排泄等构成湖、库水体N₂O的重要外源,但目前对内源/外源的相对贡献的定量化研究不足;湖、库水体N₂O排放方式包括扩散、植物传输及少量气泡排放,对水库而言,大坝下游水电涡轮机形成的脱气作用可能是N₂O排放的潜在途径.对文献综合分析表明,湖、库水体N₂O排放通常呈现明显的季节变化（夏季>冬季）和日变化,同时在全球（一般低纬度>高纬度）、区域及水体内部等不同尺度上表现出显著的空间变异性;这种时空变异特征主要受到湖、库自身理化因子（温度、营养盐、溶解氧、C/N、水文）、生物因子（水生植物、藻华）以及陆域人类活动（污水排放、农业活动以及城市化等）的影响;湖、库N₂O排放不同监测方法的差异也是潜在的影响因素,传统的漂浮箱法和薄边界层法均可能低估水体N₂O排放通量,未来需将传统的监测方法与新型的涡度相关法相结合,减小监测方法的不确定性.结合当前湖、库水体N₂O排放的研究不足,建议未来可以从湖、库N₂O产生的微生物机制,区域尺度上人类活动与湖、库群N₂O排放的耦合关系,水陆交错带的产、排过程,变化环境下的湖、库N₂O排放以及监测方法等方面深入研究.     

Dissolved nitrous oxide (N2O) dynamics in agricultural field drains and headwater streams in an intensive arable catchment

Indirect nitrous oxide (N₂O) emissions produced by nitrogen (N) leaching into surface water and groundwater bodies are poorly understood in comparison to direct N₂O emissions from soils. In this study, dissolved N₂O concentrations were measured weekly in both lowland headwater streams and subsurface agricultural field drain discharges over a 2‐year period (2013–2015) in an intensive arable catchment, Norfolk, UK. All field drain and stream water samples were found to have dissolved N₂O concentrations higher than the water–air equilibrium concentration, illustrating that all sites were acting as a net source of N₂O emissions to the atmosphere. Soil texture was found to significantly influence field drain N₂O dynamics, with mean concentrations from drains in clay loam soils (5.3 μg N L^?1) being greater than drains in sandy loam soils (4.0 μg N L^?1). Soil texture also impacted upon the relationships between field drain N₂O concentrations and other water quality parameters (pH, flow rate, and nitrate (NO₃) and nitrite (NO₂) concentrations), highlighting possible differences in N₂O production mechanisms in different soil types. Catchment antecedent moisture conditions influenced the storm event mobilisation of N₂O in both field drains and streams, with the greatest concentration increases recorded during precipitation events preceded by prolonged wet conditions. N₂O concentrations also varied seasonally, with the lowest mean concentrations typically occurring during the summer months (JJA). Nitrogen fertiliser application rates and different soil inversion regimes were found to have no effect on dissolved N₂O concentrations, whereas higher N₂O concentrations recorded in field drains under a winter cover crop compared to fallow fields revealed cover crops are an ineffective greenhouse gas emission mitigation strategy. Overall, this study highlights the complex interactions governing the dynamics of dissolved N₂O concentrations in field drains and headwater streams in a lowland intensive agricultural catchment.     

Bacterial biogas production in coastal systems affected by freshwater inputs

The concentrations of two greenhouse gases, nitrous oxide (N₂O) and methane (CH₄), and the bacterial processes involved in their production (nitrification and denitrification for N₂O, and methanogenesis for CH₄), were determined in surface waters of two coastal areas under the influence of freshwater inputs, on one part in the Gulf of Lions and the Rhone River plume, in northwestern Mediterranean Sea, and on the other part in the inner Thermaikos Gulf, in Aegean Sea, eastern Mediterranean Sea. High concentrations of dissolved CH₄ and N₂O were recorded in the surface waters of Gulf of Lions and Gulf of Thermaikos, up to 1300 nM for CH₄, and 40 nM for N₂O. No direct relationship could be found between the concentration and production of the biogases, as they may also be produced in deep water or bottom sediment in shallow areas, or derived from anthropogenic activity or ship contamination in polluted areas. Irrespective of the origin of CH₄ and N₂O, the presence of extremely high concentrations of these two gases in superficial seawater implies that they can easily escape to the atmosphere; consequently, these nearshore waters enriched in greenhouse gases may play an important role in the increase in atmospheric concentration of both CH₄ and N₂O.     

The fluvial flux of particulate organic matter from the UK: the emission factor of soil erosion

Soil erosion has been identified as a potential global carbon sink since eroded organic matter is replaced at source and eroded material is readily buried. However, this argument has relied on poor estimates of the total fate of in‐transit particulates and could erroneously imply soil erosion could be encouraged to generate carbon stores. These previous estimates have not considered that organic matter can also be released to the atmosphere as a range of greenhouse gases, not only carbon dioxide (CO₂), but also the more powerful greenhouse gases methane (CH₄) and nitrous oxide (N₂O). As soil carbon lost by erosion is only replaced by uptake of CO₂, this could represent a considerable imbalance in greenhouse gas warming potential, even if it is not significant in terms of overall carbon flux. This work therefore considers the flux of particulate organic matter through UK rivers with respect to both carbon fluxes and greenhouse gas emissions. The results show that, although emissions to the atmosphere are dominated by CO₂, there are also considerable fluxes of CH₄ and N₂O. The results suggest that soil erosion is a net source of greenhouse gases with median emission factors of 5.5, 4.4 and 0.3 tonnes CO_2eq/yr for one tonne of fluvial carbon, gross carbon erosion and gross soil erosion, respectively. This study concludes that gross soil erosion would therefore only be a net sink of both carbon and greenhouse gases if all the following criteria are met: the gross soil erosion rate were very low (<91 tonnes/km²/yr); the eroded carbon were completely replaced by new soil organic matter; and if less than half of the gross erosion made it into the stream network. By establishing the emission factor for soil erosion, it becomes possible to properly account for the benefits of good soil management in minimizing losses of greenhouse gases to the atmosphere as a by‐product of soil erosion. Copyright © 2015 John Wiley & Sons, Ltd.     

Spatial variability of N2O concentrations and of denitrification-related factors in the surficial groundwater of a catchment in Northern Germany

N₂O concentrations and denitrification-related factors (NO₃, SO₄, dissolved organic carbon (DOC) and CO₂) were investigated in the surface groundwater of a catchment in northern Germany, the Fuhrberger Feld Aquifer (FFA). We sampled 79 plots that were selected according to the three criteria of land use, historical land use conversion (1954–1995) and groundwater level. We sampled three sites within each plot. The sampling depth was 0.5 m below the groundwater surface.We found no indication for the occurrence of autotrophic denitrification in the surface groundwater. Heterotrophic denitrification was identified as the main process for N₂O accumulation. The variability of N₂O concentrations on the plot-scale was extremely high and was poorly explained by the three sampling criteria. Other denitrification-related variables such as NO₃, SO₄ and DOC were less variable. The selection criteria land use and groundwater level clearly influenced the order of magnitude of N₂O concentrations in the surface groundwater. Under arable land, high NO₃ concentrations resulted in high N₂O concentrations. The surface groundwater under forest and pasture was almost NO₃-free and had also very small N₂O concentrations. Plots where the distance from the soil surface to the groundwater surface was large (>1 m up to 3.4 m) showed higher N₂O concentrations in the surface groundwater than plots where the distance was small (<1 m). A larger distance from the soil surface to the groundwater leads to a longer residence time and more decomposition of DOC in the soil. Consequently the less bioavailable DOC could inhibit the efficiency of the heterotrophic denitrification in the groundwater, yielding more N₂O. Elevated organic carbon levels in plots with historic land use conversion (pasture to arable) were very stable and did not influence N₂O concentrations. The high within plot variability showed that an upscaling of N₂O from the plot-scale to the catchment-scale is possible as long as the groundwater level regime and the land use do not change.     

Nitrous oxide in fresh water systems: An estimate for the yield of atmospheric N2O associated with disposal of human waste

The N₂O content of waters in the Potomac and Merrimack Rivers was measured on a number of occasions over the period April to July 1977. The concentrations of dissolved N₂O exceed those which would apply in equilibrium with air by factors ranging from about 46 in the Potomac to 1.2 in the Merrimack. Highest concentrations of dissolved N₂O were associated with sewage discharges from the vicinity of Washington, D.C. and analysis indicates a relatively high yield, 1.3 to 11 percent, for prompt conversion of waste nitrogen to N₂O. The yield could be even higher if bubbles originating in sediments should contain as little as 0.3 percent N₂O. Measurements of dissolved N₂O in fresh water ponds near Boston demonstrate that aquatic systems may provide both strong sources and sinks for atmospheric N₂O.     

N2O emissions from regional agricultural lands A case study of Guizhou Province, southwestern China

To preliminarily study N₂O emissions and the importance of environmental parameters on N₂O flux from subtropical agroecosystem in China, N₂O flux measurements were made at three cultivated agricultural lands in Guizhou Province, southwestern China. Based on the test and validation of daily N₂O flux and its several associated variables between DNDC model and field measurements, DNDC model has been employed to estimate total N₂O emissions from entire agricultural lands and its spatial distribution at county scale in Guizhou in 1995, and to assess the contributions of cropping practices on N₂O emissions.     

The role of vibrationally excited nitrogen in the ionosphere

Theoretical and experimental aspects of the production, transformation, diffusion and loss of N₂ in the upper atmosphere are considered. The N₂-CO₂ near-resonant system in theD andE regions is taken into account. We describe our understanding of the methods necessary to find the vibrational populations of N₂ and CO₂ (asymmetric mode of CO₂). The calculations of the vibrational temperatures in theD, E, andF regions for the mid-latitude ionosphere and an aurora are presented. The connection between the excited species and the 4.26-m radiation intensities is considered. The models for the rate coefficient of the reaction of O⁺ with N₂ and the electron density decrease resulting from N₂ in the F region are discussed.     

The O(1S) dayglow emission as observed by the WIND imaging interferometer on the UARS

Volume emission rate profiles of the O(¹D-¹S) 5577 Å dayglow measured by the WIND imaging interferometer on the Upper Atmosphere Research Satellite are analyzed to examine the O(¹S) excitation mechanisms in the sunlit lower thermosphere and upper mesosphere. The observed emission profiles are compared with theoretical profiles calculated using a model which takes into account all of the known daytime sources of O(¹S). These include photoelectron impact on atomic oxygen, dissociative recombination of O⁺₂, photodissociation of molecular oxygen, energy transfer from metastable N₂(A³⁺_u) and three body recombination of atomic oxygen. Throughout most of the thermosphere the measured and modelled emission rates are in reasonably good agreement, given the limitations of the model, but in the region below 100 km, where the oxygen atom recombination source is likely to dominate, the measured emission rates are considerably larger than those modelled using the MSIS-90 oxygen atom densities. This discrepancy is discussed in terms of possible inadequacies in the MSIS-90 model atmosphere and/or additional sources of O(¹S) at low altitude.     

The oxygen minimum zone (OMZ) off Chile as intense source of CO2 and N2O

The oxygen minimum zones (OMZs) are recognized as intense sources of N₂O greenhouse gas (GHG) and could also be potential sources of CO₂, the most important GHG for the present climate change. This study evaluates, for one of the most intense and shallow OMZ, the Chilean East South Pacific OMZ, the simultaneous N₂O and CO₂ fluxes at the air–sea interface. Four cruises (2000–2002) and 1 year of monitoring (21°–30°–36°S) off Chile allowed the determination of the CO₂ and N₂O concentrations at the sea surface and the analysis of fluxes variations associated with different OMZ configurations. The Chilean OMZ area can be an intense GHG oceanic local source of both N₂O and CO₂. The mean N₂O fluxes are 5–10 times higher than the maximal previous historical source in an OMZ open area as in the Pacific and Indian Oceans. For CO₂, the mean fluxes are also positive and correspond to very high oceanic sources. Even if different coupling and decoupling between N₂O and CO₂ are observed along the Chilean OMZ, 65% of the situations represent high CO₂ and/or N₂O sources. The high GHG sources are associated with coastal upwelling transport of OMZ waters rich in N₂O and probably also in CO₂, located at a shallow depth. The integrated OMZ role on GHG should be better considered to improve our understanding of the past and future atmospheric CO₂ and N₂O evolutions.     

Impact of Hurricane Irene and Tropical Storm Lee on riparian zone hydrology and biogeochemistry

Although riparian zones are well known to reduce nitrogen (N) and phosphorus (P) runoff to streams, they also have the potential to affect greenhouse gas (CO₂, N₂O, and CH₄) fluxes to the atmosphere. Following large storms, soil biogeochemical conditions often become more reduced, especially in oxbow depressions and side channels, which can lead to hot moments of greenhouse gas production. Here, we investigate the impact of the remnants of Hurricane Irene and Tropical Storm Lee on riparian zone hydrology (water table: WT), and biogeochemistry (oxidation‐reduction potential [ORP], dissolved oxygen [DO], NO₃^?, PO₄^3?, CO₂, N₂O, CH₄). Results indicate that large storms have the potential to reset WT levels for weeks to months. Overbank flooding at our site following Irene and Lee led to the infiltration of well‐oxygenated water at depth (higher DO and ORP) while promoting the development of anoxic conditions within soil aggregates near the soil surface (increased N₂O and CH₄ fluxes). A short‐term increase in CO₂ emission was observed following Irene at our site where aerobic respiration was water‐limited. Over a 2‐year period, an oxbow depression exhibited higher WT, higher N₂O and CH₄ fluxes (hot moment), higher CO₂ fluxes (seasonal), and lower NO₃^? concentrations (seasonal) than the rest of the riparian zone. However, neither Irene, nor Lee, nor the oxbow depression significantly impacted PO₄^3?. Dissolved organic carbon, ORP, and DO data illustrate the time‐lag (>20 years) between the creation of an oxbow depression and the development of reducing conditions despite clear differences in riparian zone and oxbow WT dynamics.     

Data modeling and assimilation studies with the MU radar

We report initial results of data modeling and assimilation studies for several MU radar experiments. Various inputs to a one-dimensional ionospheric model are adjusted to provide agreement with observation and also to learn the sensitivity of the model to their variations. Certain observations are also used directly in the model to anchor or constrain its behavior. In particular, studies of the electron density from 100 to 500 km altitude in the ionosphere are carried out with the help of a theoretical model of O⁺, NO⁺, O⁺₂ and N⁺₂ densities and MU radar observations of the power, ion-drift and plasma-temperature profiles. Four typical cases are selected to study quantitatively the effects of the (A) perpendicular-north component of the plasma drift (15 December 1986), (B) atmospheric composition (7 October 1986), (C) solar EUV flux (2 August 1989) and (D) upper-boundary O⁺ density (5 October 1989) on the model N_mF2, h_mF2 and N_e profile, as well as on the neutral wind calculation from h_mF2 and drift data. It is found that the measured vertical ion drift explains quantitatively well the measured h_mF2 (particularly at low solar activity) while the model gives a better match with the measured N_e when it uses the h_mF2-based wind rather than the measured plasma drift. Different model values of the atmospheric O/N₂ ratio and EUV flux and different values of the upper-bound O⁺ density may modify not only N_mF2 markedly but also h_mF2: a lower O/N₂ ratio results in higher h_mF2; the EUVAC model gives higher h_mF2 at high solar activity than does the EUV91 model; with a smaller upper-bound O⁺ density, h_mF2 is lower by day but little changed by night. We specifically note that the meridional wind needed by the model to reproduce the observed h_mF2 differed according to how well the model reproduced the observed N_mF2. The uncertainties in the MSIS86 and EUV model predictions are also discussed. It is found that if the MSIS and EUV91 models are used together, the model gives an N_mF2 higher than that measured at high solar activity. Thus the O/N₂ ratio needs to be reduced from the MSIS value if EUV91 is used. If EUVAC is used, no large modification is required. At equinox for low solar activity, modeling with either EUV model produces N_mF2 values lower than those measured, and so the true O/N₂ ratio may be higher than that given by MSIS model.     

The mobility spectrum and the ion concentration of large ions in air mixed with N2O gas

Summary Using the divided electrode condenser it was possible to detect the large ion groups formed when small amounts of N₂O gas were mixed with atmospheric air. Eight groups appeared with mobilities ranging from 12.50×10^–4 to 0.60×10^–4 cm/sec: volt/cm. When using the whole electrode condenser the results showed an increase in the total ion concentration of these large ions when small amounts of N₂O gas were mixed with air. The results obtained in this work confirm that N₂O gas acts as a nucleus for condensation which is changed into a large ion by appropriating an electrical charge.     

Einfluß einiger Umweltfaktoren auf die N2O-Bildung durch Belebtschlamm unter anoxischen Bedingungen Influence of Some Environmental Conditions on N2O-Release by Activated Sludge under Anoxic Conditions

The release of nitrous oxide during denitrification in activated sludge is influenced by various environmental factors. Experiments with different electron acceptors showed that under anoxic conditions increasing concentrations of nitrate as well as nitrite enhance the production of N₂O. The N₂O concentration in the gas phase increases for 2 h, then decreases. Nitrite causes a higher release of N₂O than nitrate. Acetate in high concentration can stimulate N₂O-release. Without addition of acetate nitrate and nitrite reduction are delayed, and hence N₂O-release and consumption are much slower. In activated sludge sulfide can play a role as an inhibitor of the nitrous oxide reductase (like in soil and pure cultures), but is inactivated very rapidly. Repeated addition of sulfide can cause a new release of nitrous oxide. At low pH (less than 6.5) denitrification is slightly inhibited and N₂O-release is 100 times higher than at pH 7.0 to 8.0. Under oxygen-limiting conditions N₂O-release and denitrification starts at 0.5–1.0 mg/L DO, but it is not always accompanied by accumulation of nitrite. Further reduction of the oxygen concentration reduces N₂O-release.     

Some F2-layer effects during the January06-11,1997 cedar storm period as observed with theMillstoneHill incoherent scatter facility

An observed daytime negative storm effect on 10 January and strongpost-midnight N_m F₂ increases on 7 and 8 January followed by a steep T_e decrease down to T_n are analyzed. Daytime neutral composition and T_n(h) were inferred from incoherent scatter (IS) radar observations using aself-consistent approach to F₂ -layer modelling. Observed daytime T_e , T_i , N_e profiles were corrected for the disturbed day using the calculated ioncomposition. The main reason for the observed N_m F₂ negative storm effectis the O/(N₂ O₂ ) ratio decrease in the thermosphere. The calculated O/N₂ ratio at hm F₂ is less by a factor of 3.7 than MSIS prediction for 10January and is close to MSIS for quiet days. Strong Nm F₂ night-time increase by afactor of 3 is due to a plasma compression mechanism under the action of observed EB drift(westward E-field) moving plasma from higher L shells to lower ones and squeezing it into the F₂ -region. Moderate (1-2)10 ⁸ cm ^-2 s ^-1 O fluxes in agreement with IS observations were shown to be sufficient to account for the night-timeN_m F₂ increase. This elevation in the F₂ -region electron densityis shown to be the main reason for the observed steep Te post-midnight decrease. 1999 ElsevierScience Ltd. All rights reserved.     

Measurement of O(1D) formation by ozone photolysis in the troposphere

An actinometric method to determine the rate constantk _1D of O(¹D) formation by ozone photolysis in the troposphere and at higher altitudes is presented. N₂O is used as a scavenger gas for O(¹D), and the molecular nitrogen product measured after gas chromatographic separation. First results of the method for ground level and for 26 km altitude are reported and compared with theoretical estimates ofk _1D for these levels.     

Modelling F2-layer seasonal trends and day-to-day variability driven by coupling with the lower atmosphere

This paper presents results from the TIME-GCM-CCM3 thermosphere–ionosphere–lower atmosphere flux-coupled model, and investigates how well the model simulates known F2-layer day/night and seasonal behaviour and patterns of day-to-day variability at seven ionosonde stations. Of the many possible contributors to F2-layer variability, the present work includes only the influence of ‘meteorological’ disturbances transmitted from lower levels in the atmosphere, solar and geomagnetic conditions being held at constant levels throughout a model year.In comparison to ionosonde data, TIME-GCM-CCM3 models the peak electron density (NmF2) quite well, except for overemphasizing the daytime summer/winter anomaly in both hemispheres and seriously underestimating night NmF2 in summer. The peak height hmF2 is satisfactorily modelled by day, except that the model does not reproduce its observed semiannual variation. Nighttime values of hmF2 are much too low, thus causing low model values of night NmF2. Comparison of the variations of NmF2 and the neutral [O/N₂] ratio supports the idea that both annual and semiannual variations of F2-layer electron density are largely caused by changes of neutral composition, which in turn are driven by the global thermospheric circulation.Finally, the paper describes and discusses the characteristics of the F2-layer response to the imposed ‘meteorological’ disturbances. The ionospheric response is evaluated as the standard deviations of five ionospheric parameters for each station within 11-day blocks of data. At any one station, the patterns of variability show some coherence between different parameters, such as peak electron density and the neutral atomic/molecular ratio. Coherence between stations is found only between the closest pairs, some 2500 km apart, which is presumably related to the scale size of the ‘meteorological’ disturbances. The F2-layer day-to-day variability appears to be related more to variations in winds than to variations of thermospheric composition.