A2O工艺中N2O的产生与逸散特征

目前污水处理过程中产生温室气体的问题已经引起普遍关注。本文通过实验室小试,研究了不同污水水质条件下A2O工艺中N2O的产生特征,以及氧化亚氮还原酶编码基因nosZ含量对N2O产生量的影响。结果表明,在A2O工艺中的各单元均有N2O产生,其中厌氧池产生量最大,约占总产生量的32％～85％;A2O工艺产生的N2O主要通过逸散进入大气,少量随二沉池出水进入到环境中。N2O的产生量与污泥中nosZ的含量成负相关,而碳源和DO对含有nosZ基因的反硝化细菌有明显的影响,低DO环境和充足的碳源能够极大的促进其含量的提高,从而显著减少N2O的产生量。     

An inventory of N(2)O emissions from agriculture in China using precipitation-rectified emission factor and background emission

Fertilized agricultural soils are a major anthropogenic source of atmospheric N₂O. A credible national inventory of agricultural N₂O emission would benefit its global strength estimate. We compiled a worldwide database of N₂O emissions from fertilized fields that were consecutively measured for more than or close to one year. Both nitrogen input (N) and precipitation (P) were found to be largely responsible for temporal and spatial variabilities in annual N₂O fluxes (N₂O–N). Thus, we established an empirical model (N₂O–N = 1.49 P + 0.0186 P · N), in which both emission factor and background emission for N₂O were rectified by precipitation. In this model, annual N₂O emission consists of a background emission of 1.49 P and a fertilizer-induced emission of 0.0186 P · N. We used this model to develop a spatial inventory at the 10 × 10 km scale of direct N₂O emissions from agriculture in China. N₂O emissions from rice paddies were separately quantified using a cropping-specific emission factor. Annual fertilizer-induced N₂O emissions amounted to 198.89 Gg N₂O–N in 1997, consisting of 18.50 Gg N₂O–N from rice paddies and 180.39 Gg N₂O–N from fertilized uplands. Annual background emissions and total emissions of N₂O from agriculture were estimated to be 92.78 Gg N₂O–N and 291.67 Gg N₂O–N, respectively. The annual direct N₂O emission accounted for 0.92% of the applied N with an uncertainty of 29%. The highest N₂O fluxes occurred in East China as compared with the least fluxes in West China.     

Developing spatially stratified N(2)O emission factors for Europe

We investigate the possibility to replace the – so-called – Tier 1 IPCC approach to estimate soil N₂O emissions with stratified emissions factors that take into account both N-input and the spatial variability of the environmental conditions within the countries of the European Union, using the DNDC-Europe model. Spatial variability in model simulations is high and corresponds to the variability reported in literature for field data. Our results indicate that (a) much of the observed variability in N₂O fluxes reflects the response of soils to external conditions, (b) it is likely that national inventories tend to overestimate the uncertainties in their estimated direct N₂O emissions from arable soils; (c) on average over Europe, the fertilizer-induced emissions (FIE) coincide with the IPCC factors, but they display large spatial variations. Therefore, at scales of individual countries or smaller, a stratified approach considering fertilizer type, soil characteristics and climatic parameters is preferable.     

同步硝化反硝化工艺中DO浓度对N2O产生量的影响

采用序批式生物膜反应器（SBBR）,在连续曝气全程好氧的运行条件下,考察不同溶解氧浓度对同步硝化反硝化脱氮性能及N2O产量的影响。控制溶解氧浓度恒定在1、2、2.5和3 mg/L。结果表明,DO为2 mg/L和2.5 mg/L时,氨氮去除率分别为97.9%和98.5%,同步硝化反硝化率均为99%。DO为2 mg/L时,系统中N2O产生量最低,为0.423 mg/L,占氨氮去除量的1.4%;DO为3 mg/L时N2O的产生量最高,为2.01 mg/L,是DO为2 mg/L时的4.75倍。系统中亚硝酸盐的存在可能是高溶解氧条件下N2O产量增加的主要原因,同步过程中没有NOx-的积累即稳定的SND系统有利于降低生物脱氮过程中N2O的产生量。     

Evaluation of N2O emission from rainfed wheat field in northwest agricultural land in China

Environmental Science and Pollution Research - The net greenhouse gas (NGHG) emissions and net greenhouse gas intensity (NGHGI) were investigated via the determination of nitrous oxide (N2O)...     

Effects of environmental factors on N2O emission from and CH4 uptake by the typical grasslands in the Inner Mongolia

The fluxes of N2O emission from and CH4 uptake by the typical semi-arid grasslands in the Inner Mongolia, China were measured in 1998-1999. Three steppes, i.e. the ungrazed Leymus chinensis (LC), the moderately grazed Leymus chinensis (LC) and the ungrazed Stipa grandis (SG), were investigated, at a measurement frequency of once per week in the growing seasons and once per month in the non-growing seasons of the LC steppes. In addition, four diurnal-cycles of the growing seasons of the LC steppes, each in an individual stage of grass growth, were measured. The investigated steppes play a role of source for the atmospheric N2O and sink for the atmospheric CH4, with a N2O emission flux of 0.06-0.21 kg N ha(-1) yr(-1) and a CH4 uptake flux of 1.8-2.3 kg C ha(-1) yr(-1). Soil moisture primarily and positively regulates the spatial and seasonal variability of N2O emission. The usual difference in soil moisture among various semi-arid steppes does not lead to significantly different CH4 uptake intensities. Soil moisture, however, negatively regulates the seasonal variability in CH4 uptake. Soil temperature of the most top layer might be the primary driving factor for CH4 uptake when soil moisture is relatively low. The annual net emission of N2O and CH4 from the ungrazed LC steppe, the moderately grazed LC steppe and the ungrazed SG steppe is at a CO2 equivalent rate of 7.7, 0.8 and -7.5 kg CO2-C ha(-1) yr(-1), respectively, which is at an ignorable level. This implies that the role of the semi-arid grasslands in the atmospheric greenhouse effect in terms of net emission of greenhouse gases (CO2, CH4 and N2O) may exclusively depend upon the net exchange of net ecosystem CO2 exchange.     

Effects of biochar on nitrification and denitrification-mediated N2O emissions and the associated microbial community in an agricultural soil

Environmental Science and Pollution Research - Nitrous oxide (N2O) is a strong greenhouse gas, and it is of great significance for N2O reduction to study the effects of biochar on its production...     

Aqueous-phase nitration of phenol by N2O5 and ClNO2

Nitrophenols are present in the atmospheric gas phase and in cloud and rainwater. Their formation via aqueous-phase reactions of phenol with the nitronium ion, NO₂⁺, arising from N₂O₅ and ClNO₂ partitioning into the aqueous phase, has been proposed but not verified experimentally. Here, we demonstrate for the first time that gaseous N₂O₅ and ClNO₂ partitioning into dilute aqueous solutions of phenol yields 2- and 4-nitrophenol (and 4-nitrosophenol), but no dinitrophenol isomers. The rate of nitration does not vary significantly between 5 and 20 °C, presumably because of opposing temperature dependences in Henry's law partitioning and reaction rate coefficients. The rate coefficient for reaction of NO₂⁺ with phenol could not be directly quantified but is evidently large enough for this reaction to compete effectively with the reaction between NO₂⁺ and water and to provide a feasible route to nitrophenol production in the atmosphere.     

进水氨氮负荷对污水生物脱氮过程中N_2O释放的影响

进水氨氮负荷是污水生物脱氮过程中N2O释放的重要影响因素。在稳定运行的序列间歇式活性污泥反应器(SBR)内,考察了进水氨氮负荷对污水生物脱氮过程中N2O释放速率、累积释放量和转化率的影响。结果显示,相比于缺氧段,进水氨氮负荷的增加对好氧段N2O的释放有较大影响,且N2O的释放速率、累积释放量和转化率均随进水氨氮负荷的增加而增大。当进水氨氮负荷从45.6g/(m3·d)增加到78.6g/(m3·d)时,系统的总N2O累积释放量和总N2O转化率增加并不明显,仅增加3.95mg、0.99百分点;而当进水氨氮负荷从78.6g/(m3·d)增加到117.6g/(m3·d)时,系统的总N2O累积释放量和总N2O转化率分别增加了25.24mg、4.49百分点。因此,在实际污水处理过程中,当进水氨氮负荷偏高(117.6g/(m3·d))时,系统的N2O释放量可能大幅增加,需要采取减少进水氨氮负荷的方法来避免N2O释放。     

N2O profiles in the enhanced CANON process via long-term N2H4 addition: minimized N2O production and the influence of exogenous N2H4 on N2O sources

Environmental Science and Pollution Research - Production of the greenhouse gas nitrous oxide (N2O) from the completely autotrophic nitrogen removal over nitrite (CANON) process is of growing...     

Estimation and projection of nitrous oxide (N2O) emissions from anthropogenic sources in Taiwan

Taiwan is a densely populated and developed country with more than 97% of energy consumption supplied by imported fuels. Greenhouse gas emissions are thus becoming significant environmental issues in the country. Using the Intergovernmental Panel on Climate Change (IPCC) recommended methodologies, anthropogenic emissions of nitrous oxide (N2O) in Taiwan during 2000-2003 were estimated to be around 41 thousand metric tons annually. About 87% of N2O emissions come from agriculture, 7% from the energy sector, 3% from industrial processes sector, 3% from waste sector. On the basis of N2O emissions in 2000, projections for the year 2010 show that emissions were estimated to decline by about 6% mainly due to agricultural changes in response to the entry of WTO in 2002. In contrast to projections for the year 2020, N2O emissions were projected to grow by about 17%. This is based on the reasonable scenario that a new adipic acid/nitric acid plant will be probably started after 2010.     

Spatiotemporal variations of nitrous oxide (N2O) emissions from two reservoirs in SW China

Greenhouse gas emissions from hydroelectric dams have recently given rise to controversies about whether hydropower still provides clean energy. China has a large number of dams used for energy supply and irrigation, but few studies have been carried out on aquatic nitrous oxide (N₂O) variation and its emissions in Chinese river-reservoir systems. In this study, N₂O spatiotemporal variations were investigated monthly in two reservoirs along the Wujiang River, Southwest China, and the emission fluxes of N₂O were estimated. N₂O production in the reservoirs tended to be dominated by nitrification, according to the correlation between N₂O and other parameters. N₂O saturation in the surface water of the Wujiangdu reservoir ranged from 214% to 662%, with an average fluctuation of 388%, while in the Hongjiadu reservoir, it ranged from 201% to 484%, with an average fluctuation of 312%. The dissolved N₂O in both reservoirs was over-saturated with respect to atmospheric equilibrium levels, suggesting that the reservoirs were net sources of N₂O emissions to the atmosphere. The averaged N₂O emission flux in the Wujiangdu reservoir was 0.64 μmol m^?2 h^?1, while it was 0.45 μmol m^?2 h^?1 in the Hongjiadu reservoir, indicating that these two reservoirs had moderate N₂O emission fluxes as compared to other lakes in the world. Downstream water of the dams had quite high levels of N₂O saturation, and the estimated annual N₂O emissions from hydropower generation were 3.60 × 10⁵ and 2.15 × 10⁵ mol N₂O for the Wujiangdu and the Hongjiadu reservoir, respectively. These fluxes were similar to the total N₂O emissions from the reservoir surfaces, suggesting that water released from reservoirs would be another important way for N₂O to diffuse into the atmosphere. It can be concluded that dam construction significantly changes the water environment, especially in terms of nutrient status and physicochemical conditions, which have obvious influences on the N₂O spatiotemporal variations and emissions.     

Estimations of Real-World N2O Emissions from Road Vehicles by Means of Measurements in a Traffic Tunnel

Abstract

Ambient air measurements of N₂O, NO_x, CO, and HC based on grab sampling were conducted in a major traffic tunnel in Sweden, that carries up to 4,000 vehicles per hour, in order to estimate real-world emissions of N₂O for road traffic. Two different methods—relative and mass balance—were used to calculate a N₂O emission factor for the mixed vehicle fleet, which gave an average emission factor, at average speeds of 30-70 km/h, of approximately 25 mg N₂O/ km, with a range of 7-56 mg/km.     

Estimations of real-world N2O emissions from road vehicles by means of measurements in a traffic tunnel

Ambient air measurements of N2O, NOx, CO, and HC based on grab sampling were conducted in a major traffic tunnel in Sweden, that carries up to 4,000 vehicles per hour, in order to estimate real-world emissions of N2O for road traffic. Two different methods--relative and mass balance-were used to calculate a N2O emission factor for the mixed vehicle fleet, which gave an average emission factor, at average speeds of 30-70 km/h, of approximately 25 mg N2O/ km, with a range of 7-56 mg/km.     

Hydrodechlorination of dichlorobiphenyls over Ni-Mo/Al2O3 catalysts prepared by spray-drying method

The hydrodechlorination (HDCl) process of 2,3-, 2,4- and 2,5-dichlorobiphenyls was studied over a sulphided Ni-Mo/Al(2)O(3) catalyst in a stirred autoclave at a hydrogen pressure of 3 MPa. The catalysts were prepared by spray-drying. They were characterized by N(2) adsorption, thermogravimetry and scanning electron microscopy with X-ray microanalysis. The reaction temperature of the catalytic HDCl process was varied in the range of 230-290 degrees C. Polychlorinated biphenyls (PCBs) free transformer oil was used as reaction medium. The HDCl degree of dichlorobiphenyl isomers was in the range of 82-93%. The efficiency in the chlorine removal was found to be related to the position of the substituted chlorine atom and decreased as follows 2,4-dichlorobiphenyl approximately 2,5-dichlorobiphenyl>2,3-dichlorobiphenyl. For comparison, the HDCl process of 2,3-dichlorobiphenyl (2,3-PCB) without catalyst was also studied. The chlorine removal was 85% for the catalytic HDCl of 2,3-PCB whereas non-catalytic process led only to 16% of dechlorination in the same operating conditions, i.e. at 290 degrees C after 120 min. Monodichlorobiphenyls were not detected in the reaction products. The data for both catalytic and non-catalytic conversion of 2,3-PCB fit to a first-order model. Kinetic constants and the activation energy of the overall HDCl reaction of 2,3-PCB to biphenyl were evaluated. Compared to non-catalytic process, a nearly threefold decrease in the activation energy was observed in the presence of Ni-Mo/Al(2)O(3) catalyst prepared by spray-drying (48 kJ mol(-1) vs. 124 kJ mol(-1)).     

Combination of wet irrigation and nitrification inhibitor reduced nitrous oxide and methane emissions from a rice cropping system

Environmental Science and Pollution Research - To conserve water resources and guarantee food security, a new technology termed as “wet irrigation” is developed and practiced in rice...     

低COD/N-NH_4比废水的同时硝化反硝化生物处理策略

从生化反应计量学出发 ,提出了对低 COD/ N- NH4比废水可以通过控制营养配比、调控溶解氧浓度和控制生物硝化及生物反硝化 ,经过 NO- 2 途径进行同时硝化反硝化的生物处理策略。对香港低 COD/ N- NH4比的垃圾渗漏水用同时硝化反硝化处理的成功实例进行了讨论     

Influence of environmental factors on net N2 and N2O production in sediment of freshwater rivers

Denitrification is an important N removal process in aquatic systems but is also implicated as a potential source of global N₂O emissions. However, the key factors controlling this process as well as N₂O emissions remain unclear. In this study, we identified the main factors that regulate the production of net N₂ and N₂O in sediments collected from rivers with a large amount of sewage input in the Taihu Lake region. Net N₂ and N₂O production were strongly associated with the addition of NO₃ ^?-N and NH₄ ⁺-N. Specifically, NO₃ ^?-N controlled net N₂ production following Michaelis–Menten kinetics. The maximum rate of net N₂ production (V _max) was 116.3 μmol N₂-N m^?2 h^?1, and the apparent half-saturation concentration (k _m) was 0.65 mg N L^?1. N₂O to N₂ ratios increased from 0.18?±?0.03 to 0.68?±?0.16 with the addition of NO₃ ^?-N, suggesting that increasing NO₃ ^?-N concentrations favored the production of N₂O more than N₂. The addition of acetate enhanced net N₂ production and N₂O to N₂ ratios, but the ratios decreased by about 59.5 % when acetate concentrations increased from 50 to 100 mg C L^?1, suggesting that the increase of N₂O to N₂ ratios had more to do with the net N₂ production rate rather than acetate addition in this experiment. The addition of Cl^? did not affect the net N₂ production rates, but significantly enhanced N₂O to N₂ ratios (the ratios increased from 0.02?±?0.00 to 0.10?±?0.00), demonstrating that the high salinity effect might have a significant regional effect on N₂O production. Our results suggest that the presence of N-enriching sewage discharges appear to stimulate N removal but also increase N₂O to N₂ ratios.     

CH4 and N2O emissions from Spartina alterniflora and Phragmites australis in experimental mesocosms

Spartina alterniflora, a perennial grass with C(4)-photosynthesis, shows great invading potential in the coastal ecosystems in the east of China. We compared trace gas emissions from S. alterniflora with those from a native C(3) plant, Phragmites australis, by establishing brackish marsh mesocosms to experimentally assess the effects of plant species (S. alterniflora vs. P. australis), flooding status (submerged vs. non-submerged), and clipping (plants clipped or not) on trace gas emissions. The results show that trace gas emission rates were higher in S. alterniflora than P. australis mesocosms due to the higher biomass and density of the former, which could fix more available substrates to the soil and potentially emit more trace gases. Meanwhile, trace gas emission rates were higher in non-submerged than submerged soils, suggesting that water might act as a diffusion barrier in the brackish marsh mesocosms. Interestingly, methane (CH(4)) emission rates were lower in clipped non-submerged mesocosms than in non-clipped submerged mesocosms, but nitrous oxide (N(2)O) emissions were enhanced. CH(4) emissions were significantly correlated with the plant biomass and stem density (R(2)>0.48, P<0.05) for both species, suggesting that both the two species might play important roles in CH(4) production and transport and also act as suppliers of easily available substrates for the methanogenic bacteria in wetland ecosystems. N(2)O emissions, however, were not significantly correlated with plant biomass and density (P>0.05).