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.     

Surface Flux Measurements of CO2 and N2O from a Dried Rice Paddy in Japan during a Fallow Winter Season

Abstract

The CO₂ and N₂O soil emissions at a rice paddy in Mase, Japan, were measured by enclosures during a fallow winter season. The Mase site, one of the AsiaFlux Network sites in Japan, has been monitored for moisture, heat, and CO₂ fluxes since August 1999. The paddy soil was found to be a source of both CO₂ and N₂O flux from this experiment. The CO₂ and N₂O fluxes ranged from -27.6 to 160.4μg CO₂/m²/sec (average of 49.1 ± 42.7 μg CO₂/m²/sec) and from -4.4 to 129.5 ng N₂O/m²/sec (average of 40.3 ± 35.6 ng N₂O/m²/sec), respectively. A bimodal trend, which has a sub-peak in the morning around 10:00 a.m. and a primary peak between 2:00 and 3:00 p.m., was observed. Gas fluxes increased with soil temperature, but this temperature dependency seemed to occur only on the calm days. Average CO₂ and N₂O fluxes were 27.7 μg CO₂/m²/sec and 13.4 ng N₂O/m²/sec, with relatively small fluctuation during windy days, while averages of 69.3 μg CO₂/m²/sec and 65.8 ng N₂O/m²/sec were measured during calm days. This relationship was thought to be a result of strong surface winds, which enhance gas exchange between the soil surface and the atmosphere, thus reducing the gas emissions from soil surfaces.     

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 of night-time N2O5 concentrations from ambient NO2 and NO3 radical concentrations and the role of N2O5 in night-time chemistry

Dinitrogen pentoxide (N₂O₅), which is present in equilibrium with NO₃ radicals and NO₂, has been recognized for some time as an intermediate in the NO_x chemistry of night-time atmospheres. However, until the advent of long pathlength spectroscopic techniques for the measurement of atmospheric NO₃ radical concentrations, no reliable method for estimating N₂O₅ concentrations has been available. We have calculated maximum night-time N₂O₅ concentrations from the available experimentally determined concentrations of the NO₃ radical and NO₂ in the U.S. and Germany, and find that N₂O₅ concentrations as high as ~ 15 ppb can occur. We have also estimated removal rates for N₂O₅ and for NO₃ radicals during these nights. From data obtained under conditions devoid of point sources of NO_x, upper limit estimates of the homogeneous rate constant for the reaction of N₂O₅ with water vapor are obtained, leading to the conclusion that the homogeneous gas phase rate constant for this reaction is ⩽ 1 × 10⁻²¹ cm³ molecule⁻¹ s⁻¹ at 298 K, consistent with recent environmental chamber data.     

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。     

污水硝化过程中N2O逸出控制的理论与实践

在污水生物脱氮工艺中,硝化过程是由自养硝化菌和异养硝化菌共同完成的.2类细菌的N2O生成机理及逸出量与系统中溶解氧的高低密切相关.了解硝化系统中的典型菌种自养菌Nitrosomonas europaea和异养菌Alcaligenesfaecalis生成N2O的机理是控制硝化过程中N2O逸出的理论基础,通过筛选优势菌种构建同步硝化-反硝化作用则是控制N2O逸出的新途径.     

Estimates of future co,N2O and NOx emissions from energy combustion

Emissions of CO, N₂O and NO_x from combustion are estimated using a common set of demographic, economic and regulatory assumptions. The estimates represent a sum of emissions from six large geographical regions in which energy use was predicted using an economic forecasting model. Analysis was performed for 1960, 1975, 2000 and 2025. Future global CO emissions from combustion are likely to decrease because of regulation in the developed nations and fuel-switching in the developing nations. Future global N₂O and NO_x combustion emissions are likely to increase unless there is new regulation. The greatest uncertainties in emission estimates arise from not knowing the energy paths China and other developing nations will follow in the pursuit of economic development.     

A calibrated source of N2O5

A calibrated source of N₂O₅ was developed for use in evaluating instruments designed to measure reactive odd-nitrogen species in the atmosphere. The desirable features of the source are the output of a very low mixing ratio of N₂O₅, the measurement of total reactive nitrogen NO_y in the source output, and the use of commercially-available detection and calibration equipment. N₂O₅ was derived from a solid crystalline sample at 192 K. Mixing ratios of N₂O₅ less than 2 ppmv (parts per million by volume) were produced in a small flow ( < 50 STPcc min⁻¹) of He carrier gas. This small flow was then diluted to obtain mixing ratios less than 50 ppbv (parts per billion by volume) in flows greater than 1 STPℓ min⁻¹. The N₂O₅ mixing ratio was determined with an accuracy of ± 15 % by using a thermal dissociator, calibrated NO/N₂ mixtures, and an NO chemiluminescence detector. The level of other reactive nitrogen species in the source output was determined with an Au catalytic converter and the NO detector.     

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.     

Preliminary Measurements of Biogenic Sulfur-Containing Gas Emissions From Soils

Emission factors for particulate matter and carbon monoxide have been measured for wood, anthracite coal, and bituminous coal burned in residential heaters operated at less than 15 kW (50,000 Btu/hr). In these studies the stove effluent is mixed with about four volumes of outside air and samples are collected about two minutes after mixing. The main purpose of using this sampling method is to simulate atmospheric conditions more closely. Particulate samples are collected on 20 × 25 cm filters after cyclone preseparation of particles larger than 4 μm. Carbon monoxide concentrations are measured with Draeger tubes.

Particulate emission factors for wood ranged from 1.6 to 6.4 g/kg (fuel) and were found to depend on the fuel load and the firing rate, as indicated by earlier studies. These values are substantially less than the values obtained previously for stoves operated under similar conditions. The average particulate emission factors for bituminous and anthracite coal are 10.4 and 0.50 g/kg, respectively. Carbon monoxide emission factors for wood, bituminous, and anthracite coal are 100,116, and 21 g/kg, respectively.     

Catalytic reduction of N2O over Ag-Pd/Al2O3 bimetallic catalysts

A study of the catalytic conversion of N2O to N2 over a bimetallic Ag-Pd catalyst is described in this article. Several Ag-Pd catalytic systems were prepared supported on Al2O3 with different ratios and their catalytic activity for the direct decomposition of N2O and their reduction with CO was measured. Based on the experimental results, it was observed that Ag-Pd bimetallic catalyst (5-0.5%) was the most active for both nitrous oxide reduction and direct decomposition. This high activity seems to be connected with a synergistic effect between Ag and Pd.     

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).     

Cold season CH4, CO2 and N2O fluxes from freshwater marshes in northeast China

Cold season (winter and thaw) CH₄, CO₂ and N₂O fluxes from freshwater marshes (47°35′N, 133°31′E, Northeast China) were measured, using the static chamber method. The mean CH₄ and CO₂ fluxes from Carex lasiocarpa (Cl) were 0.5 ± 0.19 and 6.23 ± 1.36 mg C m⁻² h⁻¹, respectively, and those from Deyeuxia angustifoli (Da) were 0.18 ± 0.15 and 5.22 ± 2.48 mg C m⁻² h⁻¹, respectively in winter. There was no significant difference between Cl and Da (p > 0.05). The contributions of winter CH₄ fluxes were about 5.5% and 3% in the Cl and Da, respectively. Marshes are an important potential N₂O sink in winter season in northeast China. During thaw, the CH₄ and CO₂ emissions rapidly increased, 4.5–6 times of winter emissions. Wetland became a source of N₂O. Cold season gases flux from northern wetlands play an important role in the seasonal gas exchange.     

The oxidation of SO2 on carbon particles in the presence of O3, NO2 and N2O

The oxidation of SO₂ on carbon particles at 65 % relative humidity (RH) by O₃, NO₂ and N₂O was investigated gravimetrically and compared with oxidation by air. Approximately 1 mg samples of carbon black were exposed to continuously flowing mixtures of SO₂, SO₂ + O₃, SO₂ + NO₂, and SO₂ + N₂O in air (or in N₂). Both O₃ and NO₂ in the 0.07–10ppmv range with 20–40ppmv SO₂ were found to produce sorption and desorption coverages significantly higher than those for corresponding SO₂ in air exposures. N₂O was determined to be much less effective as an oxidant than O₃ or NO₂. Identical concentrations of O₃ or NO₂ were found to produce equivalent conversions of SO₂ to sulfate on carbon for equal exposure times. Wet chemical analysis of the residue following desorption indicated that sulfate generally accounted for well over half of the retained weight.Exposure at low concentrations (0.10 ppmv SO₂ + 0.02 ppmv O₃ or NO₂), however, appeared to produce little, if any, enhancement in SO₂ transformation when compared with equivalent SO₂ in air. Weight retentions for these runs were very small, however, and measurement errors of up to 25% would be anticipated.     

煤吸附CO2、O2和N2的能力与竞争性差异

应用Materials Studio软件,采用巨正则系综蒙特卡洛方法,依据电厂烟气注入采空区防火与封存实际,对煤吸附CO2、O2和N2的能力与竞争性差异进行分析。由计算结果可知,相比于吸附O2、N2,煤吸附单组分CO2除了范德华能起主要作用,还有很强的静电作用能。由相互作用能和等量吸附热计算结果可知,煤容易吸附CO2,而不容易吸附O2和N2。298.15 K时,CO2对N2和O2吸附选择性及O2对N2的吸附选择性分别为42.396、32.357和1.310,揭示了竞争能力大小为CO2 > O2 > N2。分压分别为CO2 16.5 kPa+N2 79 kPa+O2 4.5 kPa内系统竞争吸附时,受吸附能力、竞争性和分压影响,CO2被大量吸附,而O2吸附抑制。     

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.     

Contributions of Acid Deposition and Natural Processes to Cation Leaching from Forest Soils: A Review

Methods of quantifying the roles of atmospheric acid inputs and internal acid generation by carbonic, organic, and nitric acids are illustrated by reviewing data sets from several intensively studied sites in North America. Some of the sites (tropical, temperate deciduous, and temperate coniferous) received acid precipitation whereas others (northern and subalpine) did not. Natural leaching by carbonic acid dominated soil leaching in the tropical and temperate coniferous sites, nitric acid (caused by nitrification) dominated leaching In an N-fixing temperate deciduous site, and organic acids dominated surface soil leaching in the subalpine site and contributed to leaching of surface soils in several other sites. Only at the temperate deciduous sites did atmospheric acid input play a major role in soil leaching. In no case, however, are the annual net losses of cations regarded as alarming as compared to soil exchangeable cation capital.

These results were used to illustrate the methods of quantifying the effects of atmospheric inputs and internal processes on soil leaching rates, not to draw broad generalizations as to acid rain effects on soils. However, there are predictable patterns in natural soil leaching processes which relate to climate, soil properties, and vegetation that may help in predicting the relative importances of natural vs. atmospheric acid inputs to soil leaching.     

NiO-MgO复合金属氧化物催化分解N2O

采用溶胶凝胶法制备了一系列不同Ni/Mg比的NiO-MgO复合氧化物催化剂,并考察了其N2O催化分解性能。结果表明,NiO-MgO催化剂的N2O催化分解活性明显优于单一NiO和MgO,当MgO含量为5%时,NiO-MgO复合金属氧化物上N2O分解活性最佳。XRD、H2-TPR和XPS结果表明,Ni2+是催化分解N2O的主要活性位点。Mg不作为活性组分,但可通过Ni、Mg之间强烈的相互作用提高催化剂氧化还原能力,进而促进N2O的催化分解。此外,Mg的加入促进了催化剂中NiO的形成。