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71.
72.
Background, aim, and scope  The fraction of ambient PM10 that is due to the formation of secondary inorganic particulate sulfate and nitrate from the emissions of two large, brown-coal-fired power stations in Saxony (East Germany) is examined. The power stations are equipped with natural-draft cooling towers. The flue gases are directly piped into the cooling towers, thereby receiving an additionally intensified uplift. The exhausted gas-steam mixture contains the gases CO, CO2, NO, NO2, and SO2, the directly emitted primary particles, and additionally, an excess of ‘free’ sulfate ions in water solution, which, after the desulfurization steps, remain non-neutralized by cations. The precursor gases NO2 and SO2 are capable of forming nitric and sulfuric acid by several pathways. The acids can be neutralized by ammonia and generate secondary particulate matter by heterogeneous condensation on preexisting particles. Materials and methods  The simulations are performed by a nested and multi-scale application of the online-coupled model system LM-MUSCAT. The Local Model (LM; recently renamed as COSMO) of the German Weather Service performs the meteorological processes, while the Multi-scale Atmospheric Transport Model (MUSCAT) includes the transport, the gas phase chemistry, as well as the aerosol chemistry (thermodynamic ammonium–sulfate–nitrate–water system). The highest horizontal resolution in the inner region of Saxony is 0.7 km. One summer and one winter episode, each realizing 5 weeks of the year 2002, are simulated twice, with the cooling tower emissions switched on and off, respectively. This procedure serves to identify the direct and indirect influences of the single plumes on the formation and distribution of the secondary inorganic aerosols. Results and conclusions  Surface traces of the individual tower plumes can be located and distinguished, especially in the well-mixed boundary layer in daytime. At night, the plumes are decoupled from the surface. In no case does the resulting contribution of the cooling tower emissions to PM10 significantly exceed 15 μgm−3 at the surface. These extreme values are obtained in narrow plumes on intensive summer conditions, whereas different situations with lower turbulence (night, winter) remain below this value. About 90% of the PM10 concentrations in the plumes are secondarily formed sulfate, mainly ammonium sulfate, and about 10% originate from the primarily emitted particles. Under the assumptions made, ammonium nitrate plays a rather marginal role. Recommendations and perspectives  The analyzed results depend on the specific emission data of power plants with flue gas emissions piped through the cooling towers. The emitted fraction of ‘free’ sulfate ions remaining in excess after the desulfurization steps plays an important role at the formation of secondary aerosols and therefore has to be measured carefully.  相似文献   
73.
The amounts of formaldehyde and nitrous acid (HONO) in gas phase and dews of Santiago de Chile were simultaneously measured. Formaldehyde concentrations values in the liquid phase (dews) correlate fairly well with those in the gaseous phase and are even higher than those expected from gas–dew equilibrium. On the other hand, nitrite concentrations in dews were considerably smaller (ca. 15 times) than those expected from the gas-phase concentrations. This under-saturation is attributed to diffusion limitations due to the relatively large HONO solubility. In agreement with this, under-saturation increases with the rate of dew formation and the pH of the collected waters, factors that should increase the rate of gas to liquid HONO transfer required to reach equilibrium.  相似文献   
74.
The city of Santiago, Chile experiences frequent high pollution episodes and as a consequence very high ozone concentrations, which are associated with health problems including increasing daily mortality and hospital admissions for respiratory illnesses. The development of ozone abatement strategies requires the determination of the potential of each pollutant to produce ozone, taking into account known mechanisms and chemical kinetics in addition to ambient atmospheric conditions. In this study, the photochemical formation of ozone during a summer campaign carried out from March 8–20, 2005 has been investigated using an urban photochemical box model based on the Master Chemical Mechanism (MCMv3.1). The MCM box model has been constrained with 10 min averages of simultaneous measurements of HONO, HCHO, CO, NO, j(O1D), j(NO2), 31 volatile organic compounds (VOCs) and meteorological parameters. The O3–NOx–VOC sensitivities have been determined by simulating ozone formation at different VOC and NOx concentrations. Ozone sensitivity analyses showed that photochemical ozone formation is VOC-limited under average summertime conditions in Santiago. The results of the model simulations have been compared with a set of potential empirical indicator relationships including H2O2/HNO3, HCHO/NOy and O3/NOz. The ozone forming potential of each measured VOC has been determined using the MCM box model. The impacts of the above study on possible summertime ozone control strategies in Santiago are discussed.  相似文献   
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76.
In the present study, photocatalytic reactions of nitrogen oxides (NOx = NO + NO2) were studied on commercial TiO2 doped facade paints in a flow tube photoreactor under simulated atmospheric conditions. Fast photocatalytic conversion of NO and NO2 was observed only for the photocatalytic paints and not for non-catalytic reference paints. Nitrous acid (HONO) was formed in the dark on all paints studied, however, it efficiently decomposes under irradiation only on the photocatalytic samples. Thus, it is concluded that photocatalytic paint surfaces do not represent a daytime source of HONO, in contrast to other recent studies on pure TiO2 surfaces. As main final product, the formation of adsorbed nitric acid/nitrate anion (HNO3/NO3?) was observed with near to unity yield. In addition, traces of H2O2 were observed in the gas phase only in the presence of O2. Formation of the greenhouse gas nitrous oxide (N2O) could be excluded. The uptake kinetics of NO, NO2 and HONO was very fast under atmospheric conditions (e.g. γ(NO + TiO2) > 10?5). Thus, the uptake on urban surfaces (painted houses, etc.) will be limited by transport. For a hypothetically painted street canyon, an average reduction of nitrogen oxide levels of ca. 5% is estimated. Since the harmful HNO3/NO3? is formed on the surface of the photoactive paints, whereas it is formed in the gas phase in the atmosphere, the use of photocatalytic paints may also help to reduce acid deposition, e.g. on plants, or nitric acid related health issues.  相似文献   
77.
Pickering CM  Buckley RC 《Ambio》2010,39(5-6):430-438
Skier numbers, and revenues for the multi-billion-dollar ski industry, are highly sensitive to snow cover. Previous research projected that under climate change, natural snow cover will become inadequate at 65% of sites in the Australian ski resorts by 2020. Resorts plan to compensate for reduced snowfall through additional snowmaking. For the six main resorts, however, this would require over 700 additional snow guns by 2020, requiring approximately US $100 million in capital investment, and 2,500-3,300 ML of water per month, as well as increased energy consumption. This is not practically feasible, especially as less water will be available. Therefore, low altitude ski resorts such as these may not be able to rely on snowmaking even for short-term adaptation to climate change. Instead, they are likely to seek conversion to summer activities and increased property development.  相似文献   
78.
79.
Cai M  Xie Z  Möller A  Yin Z  Huang P  Cai M  Yang H  Sturm R  He J  Ebinghaus R 《Chemosphere》2012,87(9):989-997
Neutral polyfluorinated alkyl substances (PFASs) were measured in high-volume air samples collected on board the research vessel Snow Dragon during the 4th Chinese National Arctic Expedition from the Japan Sea to the Arctic Ocean in 2010. Four volatile and semi-volatile PFASs (fluorotelomer alcohols (FTOHs), fluorotelomer acids (FTAs), perfluoroalkyl sulfonamides (FASAs), and sulfonamidoethanols (FASEs)) were analyzed respectively in the gas and particle phases. FTOHs were the dominant PFASs in the gas phase (61-358 pg m−3), followed by FTAs (5.2-47.9 pg m−3), FASEs (1.9-15.0 pg m−3), and FASAs (0.5-2.1 pg m−3). In the particle phase, the dominant PFAS class was FTOHs (1.0-9.9 pg m−3). The particle-associated fraction followed the general trend of FASEs > FASAs > FTOHs. Compared with other atmospheric PFAS measurements, the ranges of concentrations of ∑FTOH in this study were similar to those reported from Toronto, north America (urban), the northeast Atlantic Ocean, and northern Germany. Significant correlations between FASEs in the gas phase and ambient air temperature indicate that cold surfaces such as sea-ice, snowpack, and surface seawater influence atmospheric FASEs.  相似文献   
80.
Climate change scenarios predict lower flow rates during summer that may lead to higher proportions of wastewater in small and medium sized streams. Moreover, micropollutants (e.g. pharmaceuticals and other contaminants) continuously enter aquatic environments via treated wastewater. However, there is a paucity of knowledge, whether extended exposure to secondary treated wastewater disrupts important ecosystem functions, e.g. leaf breakdown. Therefore, the amphipod shredder Gammarus fossarum was exposed to natural stream water (n = 34) and secondary treated wastewater (n = 32) for four weeks in a semi-static test system under laboratory conditions. G. fossarum exposed to wastewater showed significant reductions in feeding rate (25%), absolute consumption (35%), food assimilation (50%), dry weight (18%) and lipid content (22%). Thus, high proportions of wastewater in the stream flow may affect both the breakdown rates of leaf material and thus the availability of energy for the aquatic food web as well as the energy budget of G. fossarum.  相似文献   
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