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The formation and aging mechanism of secondary organic aerosol (SOA) and its influencing factors have attracted increasing attention in recent years because of their effects on climate change, atmospheric quality and human health. However, there are still large errors between air quality model simulation results and field observations. The currently undetected components during the formation and aging of SOA due to the limitation of current monitoring techniques and the interactions among multiple SOA formation influencing factors might be the main reasons for the differences. In this paper, we present a detailed review of the complex dynamic physical and chemical processes and the corresponding influencing factors involved in SOA formation and aging. And all these results were mainly based the studies of photochemical smog chamber simulation. Although the properties of precursor volatile organic compounds (VOCs), oxidants (such as OH radicals), and atmospheric environmental factors (such as NOx, SO2, NH3, light intensity, temperature, humidity and seed aerosols) jointly influence the products and yield of SOA, the nucleation and vapor pressure of these products were found to be the most fundamental aspects when interpreting the dynamics of the SOA formation and aging process. The development of techniques for measuring intermediate species in SOA generation processes and the study of SOA generation and aging mechanism in complex systems should be important topics of future SOA research. 相似文献
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Yongpeng Ji Xingyu Chen Yuqi Xiao Yuemeng Ji Weina Zhang Jiaxin Wang Jiangyao Chen Guiying Li Taicheng An 《环境科学学报(英文版)》2021,33(7):56-63
Mineral particles are ubiquitous in the atmosphere and exhibit an important effect on the photooxidation of volatile organic compounds (VOCs). However, the role of mineral particles in the photochemical oxidation mechanism of VOCs remains unclear. Hence, the photooxidation reactions of acrolein (ARL) with OH radical (OH) in the presence and absence of SiO2 were investigated by theoretical approach. The gas-phase reaction without SiO2 has two distinct pathways (H-abstraction and OH-addition pathways), and carbonyl-H-abstraction is the dominant pathway. In the presence of SiO2, the reaction mechanism is changed, i.e., the dominant pathway from carbonyl-H-abstraction to OH-addition to carbonyl C-atom. The energy barrier of OH-addition to carbonyl C-atom deceases 21.33 kcal/mol when SiO2 is added. Carbonyl H-atom of ARL is occupied by SiO2 via hydrogen bond, and carbonyl C-atom is activated by SiO2. Hence, the main product changes from H-abstraction product to OH-adduct in the presence of SiO2. The OH-adduct exhibits a thermodynamic feasibility to yield HO2 radical and carboxylic acid via the subsequent reactions with O2, with implications for O3 formation and surface acidity of mineral particles. 相似文献
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Hydroxylated polybrominated diphenyl ethers (HO-PBDEs) have received significant attention due to their toxicities and universal presence in the environmental matrices. However, their origins are not fully understood. We explored the feasibility of the generation of HO-PBDEs through photochemical processes from bromophenol, a commonly detected pollutant with anthropogenic source in freshwater and natural source in the marine environment. The results showed that when 2,4-dibromophenol (2,4-diBP) was irradiated in aquatic solutions under simulated sunlight, significant amounts of 2′-hydroxy-2,3′,4,5′-tetrabromodipheyl ether (2′-HO-BDE68) were rapidly formed as the dimeric product of 2,4-diBP. The formation of 2′-HO-BDE68 intensified with the increase of light intensity and with the initial concentration increase of 2,4-diBP, whereas it weakened with an increase in pH. Moreover, Fe(III) and fulvic acid played important roles in the formation of 2′-HO-BDE68. This study provides important insight into a possible source of HO-PBDEs from bromophenols in natural aquatic systems through photochemical approaches. 相似文献
26.
Effects of excited-state structures and properties on photochemical degradation of polybrominated diphenyl ethers: a TDDFT study 总被引:1,自引:0,他引:1
This study presents new insight into the photochemical degradation of polybrominated diphenyl ethers (PBDEs), and it provides details about the structures and properties of 27 PBDE congeners in the electronically excited state using the time-dependent density functional theory method. Each PBDE congener exhibited remarkably different geometries in the ground state and the excited state. The significant lengthening of C-Br bond in each PBDE congener was observed in the excited state for the first time by theoretical calculation, which is directly involved in the photochemistry reductive debromination of n-BDE to (n−1)-BDE. Generally, the lengthening of C-Br bonds cannot occur at the para position. Furthermore, the calculated results demonstrated that the photoreactivity of PBDEs increased with an increase of bromination degree. It was also found that the pattern of Br substituents had an effect upon the photoreactivity of PBDEs. These findings suggest that the information obtained in the excited state is crucial to the mechanism explanation of the photochemical degradation of PBDEs. 相似文献
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论述了汽车公害的危害性及减少汽车污染的各种综合防治方法-排气净化,革新燃烧系统及发动机等,并展望未来将采用的低污染代用燃料及低污染发动机或无污染动力源. 相似文献
28.
Mort Webster Junsang Nam Yosuke Kimura Harvey Jeffries William Vizuete David T. Allen 《Atmospheric environment (Oxford, England : 1994)》2007,41(40):9580-9593
Ambient observations have indicated that high concentrations of ozone observed in the Houston/Galveston area are associated with plumes of highly reactive hydrocarbons, mixed with NOx, from industrial facilities. Ambient observations and industrial process data, such as mass flow rates for industrial flares, indicate that the VOCs associated with these industrial emissions can have significant temporal variability. To characterize the effect of this variability in emissions on ozone formation in Houston, data were collected on the temporal variability of industrial emissions or emission surrogates (e.g., mass flow rates to flares). The observed emissions variability was then used to construct regionwide emission inventories with variable industrial emissions, and the impacts of the variability on ozone formation were examined for two types of meteorological conditions, both of which lead to high ozone concentrations in Houston. The air quality simulations indicate that variability in industrial emissions has the potential to cause increases and decreases of 10–52 ppb (13–316%), or more, in ozone concentration. The largest of these differences are restricted to regions of 10–20 km2, but the variability also has the potential to increase regionwide maxima in ozone concentrations by up to 12 ppb. 相似文献
29.
铁(Ⅲ)氧化物对染料溶液的光化学脱色研究 总被引:3,自引:0,他引:3
将铁氧化物引入染料溶液挑化学脱色研究,在高压汞灯照射下,比较了铁氧化物对活性艳红X-3B水溶液的脱色效果,结果满意,其中am-Fe(OH)3的脱色作用尤为突出,光照10min后脱色率为985,动力学研究表明:在染料浓工于60mg/L,pH2-4的条件下,α-FeOOH的活性艳红产溶液的光化学脱色对动力学零级反应; 相似文献
30.
光化学法降解水中氯代苯酚的研究进展 总被引:11,自引:0,他引:11
氯代苯酚(一氯、二氯、三氯、四氯和五氯苯酚)是一类重要的有机污染物。文章综合评述了它们在水中光化学降解的国内外研究进展,并比较各种高级氧化技术(UV、UV/H2O2、UV/O3、UV/H2O2/Fe(Ⅱ/Ⅲ)、UV/TiO2)降解这些有机物的效率与影响因素,分析了它们的降解产物和分布及其反应机理。 相似文献