Intercontinental transport of nitrogen oxide pollution plumes

We describe the first satellite observation of intercontinental transport of nitrogen oxides emitted by power plants, verified by simulations with a particle tracer model. The analysis of such episodes shows that anthropogenic NOx plumes may influence the atmospheric chemistry thousands of kilometers away from its origin, as well as the ocean they traverse due to nitrogen fertilization. This kind of monitoring became possible by applying an improved algorithm to extract the tropospheric fraction of NO2 from the spectral data coming from the GOME instrument.As an example we show the observation of NO2 in the time period 4-14 May, 1998, from the South African Plateau to Australia which was possible due to favourable weather conditions during that time period which availed the satellite measurement. This episode was also simulated with the Lagrangian particle dispersion model FLEXPART which uses NOx emissions taken from an inventory for industrial emissions in South Africa and is driven with analyses from the European Centre for Medium-RangeWeather Forecasts. Additionally lightning emissions were taken into account by utilizing Lightning Imaging Sensor data. Lightning was found to contribute probably not more than 25% of the resulting concentrations. Both, the measured and simulated emission plume show matching patterns while traversing the Indian Ocean to Australia and show great resemblance to the aerosol and CO2 transport observed by Piketh et al. (2000).

Atmospheric emission of reactive nitrogen during biofuel ethanol production

This paper evaluates emissions to the atmosphere of biologically available nitrogen compounds in a region characterized by intensive sugar cane biofuel ethanol production. Large emissions of NH(3) and NO,, as well as particulate nitrate and ammonium, occur at the harvest when the crop is burned, with the amount of nitrogen released equivalent to similar to 35% of annual fertilizer-N application. Nitrogen oxides concentrations show a positive association with fire frequency, indicating that biomass burning is a major emission source, with mean concentrations of NO, doubling in the dry season relative to the wet season. During the dry season biomass burning is a source of NH3, with other sources (wastes, soil, biogenic) predominant during the wet season. Estimated NO(2)-N, NH(3)-N, NO(3)(-)-N and NH(4)(+)-N emission fluxes from sugar cane burning in a planted area,of ca. 2.2 x 10(6) ha are 11.0, 1.1, 0.2, and 1.2 Gg N yr(-1), respectively.

Measurements and modeling of reactive nitrogen deposition in southeast Brazil

Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)

Combined cycle versus one thousand diesel power plants: pollutant emissions, ecological efficiency and economic analysis

The increase in the use of natural gas in Brazil has stimulated public and private sectors to analyse the possibility of using combined cycle systems for generation of electrical energy. Gas turbine combined cycle power plants are becoming increasingly common due to their high efficiency, short lead times, and ability to meet environmental standards. Power is produced in a generator linked directly to the gas turbine. The gas turbine exhaust gases are sent to a heat recovery steam generator to produce superheated steam that can be used in a steam turbine to produce additional power. In this paper a comparative study between a 1000 MW combined cycle power plant and 1000 kW diesel power plant is presented. In first step, the energetic situation in Brazil, the needs of the electric sector modification and the needs of demand management and integrated means planning are clarified. In another step the characteristics of large and small thermoelectric power plants that use natural gas and diesel fuel, respectively, are presented. The ecological efficiency levels of each type of power plant is considered in the discussion, presenting the emissions of particulate material, sulphur dioxide (SO2), carbon dioxide (CO2) and nitrogen oxides (NOx). (c) 2006 Elsevier Ltd. All rights reserved.

Experimental measurements of the NOx and CO concentrations operating in oscillatory and non-oscillatory burning conditions

The effects of combustion driven acoustic oscillations in carbon monoxide and nitrogen oxides emission rates of a combustor operated with liquefied petroleum gas (LPG) were investigated. Because the fuel does not contain nitrogen, tests were also conducted with ammonia injected in the fuel, in order to study the formation of fuel NOx. The main conclusions were: (a) the pulsating combustion process is more efficient than the non-pulsating one and (b) the pulsating combustion process generates higher rates of NOx, with and without ammonia injection, as shown by CO and NO concentrations as function of the O-2 concentration. An increase in the LPG flow rate, keeping constant the air to fuel ratio, increased the acoustic pressure amplitude and the frequency of oscillation. The injection of ammonia had no influence on either pressure amplitude or frequency. (c) 2005 Elsevier Ltd. All rights reserved.

Laboratory evaluation of Amazon forest biomass burning emissions

Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)

Processos diurnos e noturnos de remoção de NO2 e NH3 atmosféricos na região de Araraquara-SP

Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)

NOx and CO emissions and soot presence in partially premixed acoustically excited flames

The pulsating combustion process has attracted interest in current research because its application in energy generation can offer several advantages, such as fuel economy, reduced pollutants formation, increased rate of convective heat transfer and reduced investment, when compared with other new techniques of combustion. An experimental study has been conducted with the objective of investigating the effects of combustion driven acoustic oscillations in the emission rates of combustion gases, especially carbon monoxide and nitrogen oxides, and soot presence in partial premixed flames in confined partially premixed liquefied petroleum gas flames. The results basically showed that a more uniform fuel/air mixture due to the presence of an acoustic field increases the NOx emissions in operations close to stoichiometric equivalence ratios and the frequency is the most important parameter. Carbon monoxide and soot reduced significantly.

Lightning activity in Brazilian thunderstorms during TROCCINOX: implications for NOx production

During the TROCCINOX field experiment in January and February 2005, the contribution of lightning-induced nitrogen oxides (LNOx) from tropical and subtropical thunderstorms in Southern Brazil was investigated. Airborne trace gas measurements (NO, NOy, CO and O-3) were performed up to 12.5 km with the German research aircraft Falcon. During anvil penetrations in selected tropical and subtropical thunderstorms of 4 and 18 February, NOx mixing ratios were on average enhanced by 0.7-1.2 and 0.2-0.8 nmol mol(-1) totally, respectively. The relative contributions of boundary layer NOx (BL-NOx) and LNOx to anvil-NOx were derived from the NOx-CO correlations. on average similar to 80-90% of the anvil-NOx was attributed to LNOx. A Lightning Location Network (LINET) was set up to monitor the local distribution of cloud-to-ground (CG) and intra-cloud (IC) radiation sources (here called 'strokes') and compared with lightning data from the operational Brazilian network RINDAT (Rede Integrada Nacional de Deteccao de Descargas Atmosfericas). The horizontal LNOx mass flux out of the anvil was determined from the mean LNOx mixing ratio, the horizontal outflow velocity and the size of the vertical cross-section of the anvil, and related to the number of strokes contributing to LNOx. The values of these parameters were derived from the airborne measurements, from lightning and radar observations, and from a trajectory analysis. The amount of LNOx produced per LINET stroke depending on measured peak current was determined. The results were scaled up with the Lightning Imaging Sensor (LIS) flash rate (44 flashes s(-1)) to obtain an estimate of the global LNOx production rate. The final results gave similar to 1 and similar to 2-3 kg(N) per LIS flash based on measurements in three tropical and one subtropical Brazilian thunderstorms, respectively, suggesting that tropical flashes may be less productive than subtropical ones. The equivalent mean annual global LNOx nitrogen mass production rate was estimated to be 1.6 and 3.1 Tg a(-1), respectively. By use of LINET observations in Germany in July 2005, a comparison with the lightning activity in mid-latitude thunderstorms was also performed. In general, the same frequency distribution of stroke peak currents as for tropical thunderstorms over Brazil was found. The different LNOx production rates per stroke in tropical thunderstorms compared with subtropical and mid-latitude thunderstorms seem to be related to the different stroke lengths (inferred from comparison with laboratory data and observed lengths). In comparison, the impact of other lightning parameters as stroke peak current and stroke release height was assessed to be minor. The results from TROCCINOX suggest that the different vertical wind shear may be responsible for the different stroke lengths.

Lightning characteristics observed by a VLF/LF lightning detection network (LINET) in Brazil, Australia, Africa and Germany

This paper describes lightning characteristics as obtained in four sets of lightning measurements during recent field campaigns in different parts of the world from mid-latitudes to the tropics by the novel VLF/LF (very low frequency/low frequency) lightning detection network (LINET). The paper gives a general overview on the approach, and a synopsis of the statistical results for the observation periods as a whole and for one special day in each region. The focus is on the characteristics of lightning which can specifically be observed by this system like intra-cloud and cloud-to-ground stroke statistics, vertical distributions of intra-cloud strokes or peak current distributions. Some conclusions regarding lightning produced NOx are also presented as this was one of the aims of the tropical field campaigns TROCCINOX (Tropical Convection, Cirrus and Nitrogen Oxides Experiment) and TroCCiBras (Tropical Convection and Cirrus Experiment Brazil) in Brazil during January/February 2005, SCOUT-O3 (Stratospheric-Climate Links with Emphasis on the Upper Troposphere and Lower Stratosphere) and TWP-ICE (Tropical Warm Pool-International Cloud Experiment) during November/December 2005 and January/February 2006, respectively, in the Darwin area in N-Australia, and of AMMA (African Monsoon Multidisciplinary Analyses) in W-Africa during June-November 2006.

Experimental aspects of partially premixed pulsating combustion

The pulsating combustion process has won interest in current research due to indications that its application in energy generation can offer several advantages, such as: fuel economy, reduced pollutants formation, increased rate of convective heat transfer and reduced investment, when compared with conventional techniques. An experimental study has been conducted with the objective of investigating the effects of combustion driven acoustic oscillations in the emission rates of combustion gases, especially carbon monoxide and nitrogen oxides. The experiments were conducted in a water-jacketed 1-m long by 25-cm internal diameter stainless steel vertical tube. The combustor operated with liquefied petroleum gas (LPG) in both oscillatory and non oscillatory conditions, under the same input conditions. Part of the reactant mixture was excited acoustically, before the burner exit, by a speaker positioned strategically. The burner was aligned with the chamber longitudinal axis and positioned at its bottom. The experiments were conducted for 0.16 g/s of LPG burning in stoichiometric equivalence ratio. The main conclusions were: a) the pulsating combustion process produces more uniform fuel/air profile than the non pulsating process, b) close to stoichiometric equivalence ratio the pulsating combustion process generates higher rates of NO x; c) the frequency has a strong influence in NO x emission, but the pressure amplitude has a weak influence; d) the presence of the acoustic field may change drastically the combustion gas emissions in diffusion flames, but in pre-mixed flames the influence is not as strong.

Ten years of NO2 comparisons between ground-based SAOZ and satellite instruments (GOME, SCIAMACHY, OMI)

SAOZ (Systeme d'Analyse par Observations Zenithales) is a ground-based UV-Visible zenith-sky spectrometer installed between 1988 and 1995 at a number of NDSC stations at various latitudes on the globe. The instrument is providing ozone and NO2 vertical columns at sunrise and sunset using the Differential Optical Absorption Spectroscopy (DOAS) technique in the visible spectral range. The ERS-2 GOME Ozone Monitoring Experiment (GOME) in 1995 was the first satellite mission to provide a global picture of atmospheric NO 2 with reasonable spatial and temporal resolution. It was then followed by SCanning ImAging spectroMeter for Atmospheric ChartographY (SCIAMACHY) onboard ENVISAT in 2002, and Ozone Monitoring Instrument (OMI) onboard EOS-AURA in 2004, with a similar capacity to monitor total NO 2. All these instruments are nadir viewing mapping spectrometers, applying the DOAS technique in the visible for deriving the NO2 total column. Here we present the results of NO2 long-term comparisons between GOME and SAOZ for the whole period of GOME operation since 1995 at all latitudes - tropics, mid-latitudes and polar regions - in both hemispheres. Comparisons are also shown with the most recently available SCIAMACHY and OMI data in 2004-2005. Overall, the daytime satellite measurements (around noon) are found consistent with sunrise ground-based data, with an average smaller difference at the tropics and mid-latitudes than in the polar areas in the summer. The agreement is even improved after correcting for the NO2 photochemical change between sunrise and the satellite overpass using a box model. However, some seasonal dependence of the difference between ground-based and satellite total NO2 still remains, related to the accuracy of photochemical simulations and the set of NO2 air mass factors used in the retrievals of both systems.

Giant Chemo-Resistance of SnO disk-like structures

Single crystalline SnO micro-disks, synthesized by a carbothermal reduction process, exhibited a nearly 1000-fold increase in resistance upon exposure to 100 ppm of NO2 without addition of catalysts or dopants nor the existence of nano-sized dimensions. Moreover, the SnO displayed a greater than 100-fold selectivity to NO2 over potential interferents including CO, H2 and CH4. The high sensor signal and exceptional selectivity for this novel sensor material are attributed to the existence of a high density of active lone pair electrons on the exposed (0 0 1) planes of the single crystalline SnO disks. This, thereby, identifies new means, not utilizing nano-dimensions, to achieve high gas sensitivity. © 2013 Elsevier B.V. All rights reserved.

Kinetic parameters for thermal decomposition of hydrazine

The propulsion of most of the operating satellites comprises monopropellant (hydrazine - N2H4) or bipropellant (monometilydrazine - MMH and nitrogen tetroxide) chemical systems. When some sample of the propellant tested fails, the entire sample lot shall be rejected, and this action has turned into a health problem due to the high toxicity of N2H 4. Thus, it is interesting to know hydrazine thermal behavior in several storage conditions. The kinetic parameters for thermal decomposition of hydrazine in oxygen and nitrogen atmospheres were determined by Capela-Ribeiro nonlinear isoconversional method. From TG data at heating rates of 5, 10, and 20 C min-1, kinetic parameters could be determined in nitrogen (E = 47.3 ± 3.1 kJ mol-1, lnA = 14.2 ± 0.9 and T b = 69 C) and oxygen (E = 64.9 ± 8.6 kJ mol-1, lnA = 20.7 ± 3.1 and T b = 75 C) atmospheres. It was not possible to identify a specific kinetic model for hydrazine thermal decomposition due to high heterogeneity in reaction; however, experimental f(α)g(α) master-plot curves were closed to F 1/3 model. © 2013 Akadémiai Kiadó, Budapest, Hungary.

Efeito dos óxidos de nitrogênio e de enxofre na corrosão de cobre e zinco: Um experimento para o ensino da corrosão

This paper proposes a didactic experience on the simulation of the atmospheric corrosion of copper and zinc due to the presence of sulfur and nitrogen oxides. Quantitative parameters of corrosion such as gain and loss of mass were determined to assess the variation of the layer thickness of the metal and of the corrosion products. This proposal aims a better understanding of some basic aspects of acid rain formation using fundamental concepts of chemistry such as the reactivity of gases.