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1.
Based on the methodology and default data recommended by IPCC, N2O, NH3 and NOx emissions from fuel combustion, industrial processes, field burning of agricultural residues and fertilization were estimated. Agricultural fertilization is the important contributor of N2O emission to the atmosphere. Fuel combustion, fertilizer application and animal waste were the important sources of NH3 and NOx emissions. Estimates of NH3 and NOx emissions from animal wastes were much lower when Chinese measured nitrogen excrement data were used rather than IPCC default values. The uncertainties in the estimates of N2O, NH3and NOx emissions were also analyzed in this paper.  相似文献   

2.
Increasing concentrations of methane (CH4) in the atmosphere are projected to account for about 25% of the net radiative forcing. Biospheric emissions of CH4 to the atmosphere total approximately 400 Tg C y-1. An estimated 300 Tg of CH4-C y-1 is oxidized in the atmosphere by hydroxyl radicals while about 40 Tg y-1 remains in the atmosphere. Approximately 40 Tg y-1 of the atmospheric burden is oxidized in aerobic soils. Research efforts during the past several years have focused on quantifying CH4 sources while relatively less effort has been directed toward quantifying and understanding the soil sink for atmospheric CH4. Recent research has demonstrated that land use change, including agricultural use of native forest and grassland systems has decreased the soil sink for atmospheric methane. Some agricultural systems consume atmospheric CH4 at rates less than 10% of those found in comparable undisturbed soils. While it has been necessary to change land use practices over the past centuries to meet the required production of food and fiber, we need to recognize and account for impacts of land use change on the biogeochemical nutrient cycles in the biosphere. Changes that have ensued in these cycles have and will impact the atmospheric concentrations of CH4 and N2O. Since CH4 and N2O production and consumption are accomplished by a variety of soil microorganisms, the influence of changing agricultural, forest, and, demographic patterns has been large. Existing management and technological practices may already exist to limit the effect of land use change and agriculture on trace gas fluxes. It is therefore important to understand how management and land use affect trace gas fluxes and to observe the effect of new technology on them. This paper describes the role of aerobic soils in the global CH4 budget and the impact of agriculture on this soil CH4 sink. Examples from field studies made across subarctic, temperate and tropical climate gradients in grasslands are used to demonstrate the influence of nutrient cycle perturbations on the soil consumption of atmospheric CH4 and in increased N2O emissions. This revised version was published online in August 2006 with corrections to the Cover Date.  相似文献   

3.
Emissions of nitrogen compounds from heavily fertilized and irrigated maize fields have been studied in the Southwest of France, over an annual cultivation cycle. Strong nitrous oxide emissions from denitrification were observed after application of nitrogen fertilizer. Flux intensity appears to be stimulated by rain or irrigation. Emission algorithms, taking into account both nitrogen input and soil water content were established on the basis of the experimental data set. They allowed us to estimate annual nitrogen loss in the form of nitrous oxide modulated by rainfall. Production of methane is observed at the level of the water table under anoxic conditions. Nevertheless, the net flux between soil and atmosphere is negative for most of the time. When methane is produced, fluxes were very low due to methane oxidation in the soil surface layer.  相似文献   

4.
According to the revised 1996 IPCC guidelines, several emission factors are needed to calculate national inventories of N2O emissions from agriculture. To estimate the direct N2O emissions from mineral soils, an emission factor of 0.0125 kg N2O-N per kg N applied is currently being used. From recent literature data it was clearly shown that real N2O emissions could differ substantially from this value. Based on the IPCC methodology an inventory of N2O emission from agriculture in Europe (EU-15) has been made. In 1996, the N2O emission was estimated at 672 Gg N2O-N. The N2O emission per country varied between 10 and 177 Gg N2O-N. The N2O emission per ha agricultural land in the various countries varied between 1.7 and 14.2 kg N2O-N ha−1. Highest N2O emissions per ha were found in countries with a high agricultural intensity, such as the Netherlands, Belgium-Luxembourg, Denmark and Germany. Agricultural soils are a sink for atmospheric methane. An oxidation capacity of 2.5 and 1.5 kg CH4 ha−1 yr−1 was put forward for grasslands and arable land, respectively. Based on land use data of 1993, the CH4 sink of agricultural lands in EU-15 was estimated at 303.5 Gg CH4. In general, it could be concluded that N2O emissions from soils (327 Tg CO2 equivalents) are far more important than its sink function for CH4 (6.3 Tg CO2 equivalents). This revised version was published online in August 2006 with corrections to the Cover Date.  相似文献   

5.
Emissions of nitrogen compounds (NO, NH3, N2O and N2) from heavily fertilized (280 kg(N) ha-1) and irrigated maize fields were studied over an annual cultivation cycle in southwestern France. NO and N2O emissions were measured by chamber techniques throughout the year. During fertilization and maize growth periods, chamber measurements were intensified and complemented by flux-gradient micrometeorological measurements of NOx and NH3. The two methods used, Bowen ratio and a simplified aerodynamical techniques, agree quite well and quantify NOx and NH3 flux variations during the period of intense emission which followed fertilizer application. Over a yearly cycle, nitrogen loss in the form of NH3, NO and N2O were calculated using micrometeorological flux measurements and emission algorithms calibrated with field data (chambers). The soil denitrification potential represented by the ratio N2O/(N2O+N2) was measured in the laboratory to calculate potential total gaseous nitrogen loss. Taking into account all uncertainties, the total N loss into the atmosphere represents 30 to 110 kg(N) ha-1 with about less than 1% as NH3, 40% as NO, 14% as N2O and 46% as N2. This is in agreement with the agronomic nitrogen budget based on the N fertilizer input and soil furniture and, on the N-output by crops and crop residues, which displays a net imbalance of 50 to 100 kg(N) ha-1.  相似文献   

6.
Manure storage contributes significantly to greenhouse gas (GHG), NH3 and odour emissions from intensive livestock production. A pilot-scale facility with eight 6.5-m3 slurry storage units was used to quantify emissions of CH4, N2O, NH3, and odorants from pig slurry during winter and summer storage. Pig slurry was stored with or without a straw crust, and with or without interception of precipitation, i.e., four treatments, in two randomized blocks. Emissions of total reduced S (mainly H2S) and p-cresol, but not skatole, were reduced by the straw crust. Total GHG emissions were 0.01–0.02 kg CO2 eq m?3 day?1 during a 45-day winter storage, and 1.1–1.3 kg CO2 eq m?3 day?1 during a 58-day summer storage period independent of storage conditions; the GHG balance was dominated by CH4 emissions. Nitrous oxide emissions occurred only during summer storage where, apparently, emissions were related to the water balance of the surface crust. An N2O emission factor for slurry storage with a straw crust was estimated at 0.002–0.004. There was no evidence for a reduction of CH4 emissions with a crust. Current Intergovernmental Panel on Climate Change recommendations for N2O and CH4 emission factors are discussed.  相似文献   

7.
Strategies used to reduce emissions of N2O and CH4 in rice production normally include irrigation management and fertilization. To date, little information has been published on the measures that can simultaneously reduce both emissions. Effects of application of a urease inhibitor, hydroquinone (HQ), and a nitrification inhibitor, dicyandiamide (DCD) together with urea (U) on N2O and CH4 emission from rice growing were studied in pot experiments. These fertilization treatments were carried out in the presence and absence of wheat straw, applied to the soil surface. Without wheat straw addition, in all treatments with inhibitor(s) the emission of N2O and CH4 was significantly reduced, as compared with the treatment whereby only urea was applied (control). Especially for the U+HQ+DCD treatment, the total emission of N2O and CH4 was about 1/3 and 1/2 of that in the control, respectively. In the presence of wheat straw, the total N2O emission from the U+HQ+DCD treatment was about 1/2 of that from the control. The total CH4 emission was less influenced. Wheat straw addition, however, induced a substantial increase in emissions of N2O and CH4. Hence, simultaneous application of organic materials with a high C/N ratio and N-fertilizer (e.g. urea) is not a suitable method to reduce the N2O and CH4 emission. Application of HQ+DCD together with urea seemed to improve the rice growth and to reduce both emissions. The NO3 -N content of the rice plants and denitrification of (NO3 +NO2 )-N might contribute to the N2O emission from flooded rice fields.  相似文献   

8.
In a 3-year field experiment the effect of the new nitrification inhibitor DMPP (3,4-dimethyl pyrazole phosphate, trade name ENTEC) on the release of N2O and on methane oxidation was examined in comparison to dicyandiamide (DCD). Soil samples were analysed for the concentrations of ammonium, nitrite, nitrate and for the degradation kinetics of DMPP as well as DCD. DMPP decreased the release of N2O by 41% (1997), 47% (1998) and 53% (1999) (with an average of 49%) while DCD reduced N2O emissions by 30% (1997), 22% (1998) and 29% (1999) (with an average of 26%), respectively. Both nitrification inhibitors (NI) failed to affect methane oxidation negatively. The plots that received DCD or DMPP, respectively, even seem to function as enhanced sinks for atmospheric methane. DMPP apparently stimulated methane oxidation by ca. 28% in comparison to the control. The concentrations of ammonium remained unaffected by nitrification inhibitors whereas the amounts of nitrite diminished in the plots treated with DCD by 25% and with DMPP by 20%, respectively. Nitrate concentrations in soil were in both NI treatments 23% lower than in the control. DMPP and DCD did not affect the yields of summer barley, maize and winter wheat significantly. Dicyandiamide was mineralized more rapidly than DMPP (data for the cropping season in 1997 as an example). This revised version was published online in August 2006 with corrections to the Cover Date.  相似文献   

9.
Emissions of ammonia (NH3), nitrous oxide (N2O) and methane (CH4) from uncovered yard areas (hardstandings) of a UK dairy farm were measured between October 1997 and August 1999. Measurements were concentrated after morning milking when the yard had been scraped, and at positions accounting for differences in slurry coverage and manure type. Over two seasons, the mean NH3 emission from a number of season and position categories on the hardstanding were 0.27 g N m−2 h−1 in winter and spring, 0.45 g N m−2 h−1 in summer when the feeding/loafing area was not included, increasing to 1.51 g N m−2 h−1 when this area was included, and 5.0 g N m−2 h−1 for the feeding/loafing area alone. The feeding/loafing area was close to the slurry lagoon where excreta were continuously deposited and not scraped to the slurry lagoon, as was the rest of the hardstanding. A diurnal study of emissions in the summer showed a marked decrease with time after the yard was scraped following the first milking, with emissions increasing again after evening milking when fresh excreta were deposited. Nitrous oxide emissions were more variable than NH3, with an order of magnitude difference between lowest and highest emissions measured at the same time. Mean N2O emission rates were 3.3 μg N m−2 h−1 in winter and spring, 6.5 μg N m−2 h−1 in summer when the feeding/loafing area was not included, increasing to 7.8 μg N m−2 h−1 when this area was included, and 17.9 μg N m−2 h−1 for the feeding/loafing area alone. Large mean methane emissions were measured, 185 mg C m−2 h−1 in winter and spring, decreasing to 57.3 mg C m−2 h−1 in summer when the feeding/loafing area was not included, increasing to 72.9 mg C m−2 h−1 when this area was included, and 151.2 mg C m−2 h−1 for the feeding/loafing area alone. Therefore in summer, emissions measured directly from a dung pat [0–5 cm] that had not been scraped from the loafing area were much greater than from scraped hardstanding areas, but in winter there were still significant emissions from the remaining slurry post-scraping. The experimental design was not sufficient to elucidate the physico-chemical variables controlling the measured emissions, but the data were put into context by estimating the annual emission of these pollutant gases from this one dairy farm. These were estimated at 0.43 t NH3-N y−1, 0.3 kg N2O-N y−1 and 1.0 kg CH4-C y−1. Therefore, uncovered farmyard areas that regularly have excreta deposited on them are significant but previously unaccounted for sources of NH3 loss, less so for N2O and CH4, and require further study to assess the significance of these emission sources within the UK and worldwide. This revised version was published online in August 2006 with corrections to the Cover Date.  相似文献   

10.
N2O和NH3的排放主要来自于机动车尾气排放。本文总结了近十几年来轻型汽油车N2O和NH3排放的研究进展,阐述了两种气态污染副产物在三效催化剂中的形成机理,通过对影响N2O和NH3生成的贵金属种类和含量、载体材料、不同气体组成和浓度、老化条件、不同车辆及测试工况、反应温度等主要影响因素的综述,总结了各要素对N2O和NH3形成的影响,得出N2O和NH3主要在富燃条件下冷启动阶段生成,NO的解离在N2O和NH3的生成中起关键作用;影响N2O和NH3生成的各因素之间相互关联,相互影响;催化剂的老化增加N2O和NH3的排放;贵金属Rh比Pd和Pt更有利于N2O和NH3的分解等结论。发动机、后处理策略系统的升级、更合适测试循环的开发以及催化剂的优化可以进一步降低N2O和NH3的排放。  相似文献   

11.
A novel layered zinc phosphonate, Zn2Cl[O3PCH2N(CH2CH2)2O][O3PCH2NH(CH2CH2)2O] 1 has been synthesized by hydrothermal reaction at 180 °C and structurally characterized by single crystal X-ray diffraction as well as with infrared spectroscopy, elemental analysis and thermogravimetric analysis. The interconnection of Zn(1)O4, Zn(2)O2NCl and CPO3 tetrahedra via corner-sharing forms a double layer structure with a channel system along b-axis direction. The result of connections in this manner is the formation of 8- and 16-atom windows that are parallel to one another and run in the a-axis direction. The morpholinyl groups of the ligands are orientated toward the interlayer space.  相似文献   

12.
The thermal dilatation in (NH3 ·CH3) SnCl6, (NH3 · C2H5) SnCl6 and [N(CH3)] SnCl6 was measured, and as the results it has turned out that (NH3 6·C2H5) SnCl6 and [N(CH3)4]2 SnCl6 undergo the first order transitions at 128 K and 158 K, respectively. The low temperature phases of (NH · C2H5) SnCl6 and [N(CH3)4]2 SnC16 are found to be monoclinic and tetragonal, respectively, No phase transition was observed in (NH3 ·CH3)2 SnCl6 down to 77 K.  相似文献   

13.
Tayyem H  Huq F  Yu JQ  Beale P  Fisher K 《ChemMedChem》2008,3(1):145-151
This paper describes the synthesis, characterisation, and cytotoxicity of a novel trinuclear platinum complex code named TH1. In addition to its activity against human ovarian cancer cell lines: A2780, A2780(cisR), and A2780(ZD0473R), cell uptake, DNA-binding, and the nature of the compound interaction with pBR322 plasmid DNA have been determined. TH1 is found to be significantly more cytotoxic than cisplatin - two times more active than cisplatin against the parent cell line A2780, thirteen times more active against the cisplatin-resistant cell line A2780(cisR) and 11.5 times more active against the cell line A2780(ZD0473R). Whereas the resistance factors for cisplatin as applied to the cell lines A2780 and A2780(cisR), and A2780 and A2780(ZD0473R) are 12.9 and 3.0 respectively, the corresponding values for TH1 are 1.98 and 0.5. The results suggest that TH1 has been able to significantly overcome resistance in A2780(cisR) and A2780(ZD0473R) cell lines. Whereas cisplatin binds with DNA forming mainly intrastrand GG adduct that causes local bending of a DNA strand, TH1 should bind with DNA forming mainly interstrand GG adducts that would cause more of a global change in DNA conformation. Provided it has favourable toxicity profile, TH1 has the potential to be developed into a highly active anticancer drug with a wider spectrum of activity than cisplatin.  相似文献   

14.
The present field study investigated the effects of the system of rice intensification (SRI) on greenhouse gas emissions and rice yield, in the first field trial of its kind in Cambodia. The study was a 2 × 4 factorial design, including SRI and conventional management practices (CMP) with the following treatments: control, composted farmyard manure (FYM), mineral fertiliser (MF) and FYM + MF. The results indicated large seasonal variations of CH4 patterns during the growing season with a peak emission of about 1,300 mg CH4 m?2 day?1 under both production systems 2 weeks after rice transplanting. There was large temporal variability of CH4 fluxes from morning to midday. Emission of N2O was below the detection limit in both systems. Under each production system, the highest seasonal emission of CH4 was under the FYM + MF treatment, namely 282 kg ha?1 under CMP and 213 kg ha?1 under SRI. Total CH4 emission under SRI practices was reduced by 22 % in the FYM treatment, 17 % in the MF treatment and 24 % in the FYM + MF treatment compared to CMP. There was no effect of water management on CH4 emission in the non-fertilized treatment. Grain yields were not significantly affected by the production system. Thus the yield-scaled global warming potential (GWP) was lower under SRI than CMP, namely 21 % in FYM and FYM + MF treatments, and 8 % in MF treatment. The application of mineral fertilisers moderately increased CH4 emission but significantly increased rice yields, resulting in a significantly lower yield-scaled-GWP compared to farmyard manure.  相似文献   

15.
设计、合成了一个新的甲烷单加氧酶(MMO)模型化合物[Fe2(Ⅲ,Ⅲ)L(μ-OAc)2]·PF6,其中L为2,6-二{[(2-羟基-5-叔丁基-苄基)(吡啶-2-甲基)-氨基]-甲基}-4-甲基苯酚。与以往的模型体系[Fe2(Ⅱ,Ⅲ)(bpmp)(μ-OAc)2]·(BPh4)2相比,新模型增加了2个酚配体、2个叔丁基。这些基团的引入提高了中心金属Fe的价态,并增加了配体的电子云密度从而调节了Fe的氧化还原电位。该模型进一步缩小了人工模型体系与甲烷单加氧活性中心(MMOH)的差异。通过红外(IR)、电喷雾电离质谱(ESI-MS)、核磁共振NMR(gCOSY、gHMBC、gHSQC)及电化学对新配体及络合物进行了表征和测试。  相似文献   

16.
The solubilities of gases in ionic liquids are important in evaluating ionic liquids as solvents for reactions involving permanent gases, as gas storage media, and as solvents for gas separations. Gas solubilities are also important in developing methods to separate solutes from ionic liquid solutions. Here we describe our measurements of the solubilities of CO2, CH4, C2H 6, C2H 4, O2, and N2 in 1-hexyl-3-methylpyridinium bis(trifluoromethylsulfonyl)imide and compare these results to our previous investigations. In addition, focus is placed on efforts to tailor ionic liquids to enhance the solubilities of some gases, with particular emphasis on carbon dioxide.  相似文献   

17.
Indium oxide (In2O3) nanocrystals (NCs) have been obtained via atmospheric pressure, chemical vapour deposition (APCVD) on Si(111) via the direct oxidation of In with Ar:10% O2 at 1000 °C but also at temperatures as low as 500 °C by the sublimation of ammonium chloride (NH4Cl) which is incorporated into the In under a gas flow of nitrogen (N2). Similarly InN NCs have also been obtained using sublimation of NH4Cl in a gas flow of NH3. During oxidation of In under a flow of O2 the transfer of In into the gas stream is inhibited by the formation of In2O3 around the In powder which breaks up only at high temperatures, i.e. T > 900 °C, thereby releasing In into the gas stream which can then react with O2 leading to a high yield formation of isolated 500 nm In2O3 octahedrons but also chains of these nanostructures. No such NCs were obtained by direct oxidation for T G < 900 °C. The incorporation of NH4Cl in the In leads to the sublimation of NH4Cl into NH3 and HCl at around 338 °C which in turn produces an efficient dispersion and transfer of the whole In into the gas stream of N2 where it reacts with HCl forming primarily InCl. The latter adsorbs onto the Si(111) where it reacts with H2O and O2 leading to the formation of In2O3 nanopyramids on Si(111). The rest of the InCl is carried downstream, where it solidifies at lower temperatures, and rapidly breaks down into metallic In upon exposure to H2O in the air. Upon carrying out the reaction of In with NH4Cl at 600 °C under NH3 as opposed to N2, we obtain InN nanoparticles on Si(111) with an average diameter of 300 nm.  相似文献   

18.
Fluxes of CH4 and N2O were measured regularly in an agricultural field treated with 280 g m−2 of sewage sludge. In a nearby beech forest N2O and CH4 fluxes were measured in a well-drained (dry) area and in a wet area adjacent to a drainage canal. We observed brief increases of both CH4 and N2O emissions immediately following soil applications of digested sewage sludge. Cumulated values for CH4 emissions over the course of 328 days after sludge applications indicated a small net source in sludge treated plots (7.6 mg C m−2) whereas sludge-free soil constituted a small sink (-0.9 mg C m−2). The CH4 emission amounted 0.01% of the sludge-C. Extrapolated to current rates of sludge applications in Danish agriculture this amounts to 0.1% of the total agricultural derived CH4. Sludge applications did not affect cumulated fluxes of N2O showing 312 mg N2O–N m−2 and 304 mg N m−2 with and without sludge, respectively. Four months after the sludge applications a significant effect on CO2 and NO emissions was still obvious in the field, the latter perhaps due to elevated nitrification. Nitrous oxide emission in the beech forest was about six times smaller (45 mg N m−2) than in the field and independent of drainage status. Methane oxidation was observed all-year round in the forest cumulating to -225 mg C m−2 and -84 mg C m−2 in dry and wet areas. In a model experiment with incubated soil cores, nitrogen amendment (NH4Cl) and perturbation significantly reduced CH4 oxidation in the forest soil, presumably as a result of increased nitrification activity. Sludge also induced net CH4 production in the otherwise strong CH4 oxidising forest soil. This emphasises the potential for CH4 emissions from sewage sludge applications onto land. The study shows, however, that emissions of N2O and CH4 induced by sewage sludge in the field is of minor importance and that factors such as land use (agriculture versus forest) is a much stronger controller on the source/sink strengths of CH4 and N2O. This revised version was published online in August 2006 with corrections to the Cover Date.  相似文献   

19.
In this paper a global reaction kinetic model is used to understand and describe the NOx storage/reduction process in the presence of CO2 and H2O. Experiments have been performed in a packed bed reactor with a Pt–Ba/γ-Al2O3 powder catalyst (1 wt% Pt and 30 wt% Ba) with different lean/rich cycle timings at different temperatures (200, 250, and ) and using different reductants (H2, CO, and C2H4). Model simulations and experimental results are compared. H2O inhibits the NO oxidation capability of the catalyst and no NO2 formation is observed. The rate of NO storage increases with temperature. The reduction of stored NO with H2 is complete for all investigated temperatures. At temperatures above , the water gas shift (WGS) reaction takes place and H2 acts as reductant instead of CO. At , CO and C2H4 are not able to completely regenerate the catalyst. At the higher temperatures, C2H4 is capable of reducing all the stored NO, although C2H4 poisons the Pt sites by carbon decomposition at . The model adequately describes the NO breakthrough profile during 100 min lean exposure as well as the subsequent release and reduction of the stored NO. Further, the model is capable of simulating transient reactor experiments with 240 s lean and 60 s rich cycle timings.  相似文献   

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