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  • 1
    Publication Date: 2010-11-09
    Description: Anthropogenic emissions of air pollutants in China influence not only local and regional environments but also the global atmospheric environment; therefore, it is important to understand how China's air pollutant emissions will change and how they will affect regional air quality in the future. Emission scenarios in 2020 were projected using forecasts of energy consumption and emission control strategies based on emissions in 2005, and on recent development plans for key industries in China. We developed four emission scenarios: REF[0] (current control legislations and implementation status), PC[0] (improvement of energy efficiencies and current environmental legislation), PC[1] (improvement of energy efficiencies and better implementation of environmental legislation), and PC[2] (improvement of energy efficiencies and strict environmental legislation). Under the REF[0] scenario, the emission of SO2, NOx, VOC and NH3 will increase by 17%, 50%, 49% and 18% in 2020, while PM will be reduced by 10% over East China, compared to that in 2005. In PC[2], sustainable energy polices will reduce SO2, NOx and PM10 emissions by 4.1 Tg, 2.6 Tg and 1.8 Tg, respectively; better implementation of current control policies will reduce SO2, NOx and PM10 emission by 2.9 Tg, 1.8 Tg, and 1.4 Tg, respectively; strict emission standards will reduce SO2, NOx and PM10 emissions by 3.2 Tg, 3.9 Tg, and 1.7 Tg, respectively. Under the PC[2] scenario, SO2 and PM10 emissions will decrease by 18% and 38%, while NOx and VOC emissions will increase by 3% and 8%, compared to that in 2005. Future air quality in China was simulated using the Community Multi-scale Air Quality Model (CMAQ) with 2005 emissions and 2020 emission scenarios. Under REF[0] emissions, the concentrations of SO2, NO2, hourly maximum ozone in summer, PM2.5, total sulfur and nitrogen depositions will increase by 5~47%, 45~53%, 8~12%, 4~15%, 4~37% and 7~14%, respectively, over East China. Under the PC[2] emission scenario, the concentrations of SO2, NO2, hourly maximal ozone in summer, PM2.5, total sulfur and nitrogen depositions will change by −28%~16%, −1%~11%, 1%~2%, −24%~−12%, −24%~13%, and 0~3%, respectively. The individual impacts of SO2, NOx, NH3, NMVOC and primary PM emission changes on ozone and PM2.5 concentrations have been analyzed using sensitivity analysis. The results suggest that NOx emission control need to be enhanced during the summertime to obtain both ozone and PM2.5 reduction benefits. NH3 emission controls should also be considered in order to reduce total nitrogen deposition in the future.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 2
    Publication Date: 2009-06-15
    Description: Photodegradation of secondary organic aerosol (SOA) prepared by ozone-initiated oxidation of D-limonene is studied with an action spectroscopy approach, which relies on detection of volatile photoproducts with chemical ionization mass-spectrometry as a function of the UV irradiation wavelength. Efficient photodegradation is observed for a broad range of ozone (0.1–300 ppm) and D-limonene (0.02–3 ppm) concentrations used in the preparation of SOA. The observed photoproducts are dominated by oxygenated C1-C3 compounds such as methanol, formic acid, acetaldehyde, acetic acid, and acetone. The irradiation wavelength dependence of the combined yield of the photoproducts closely tracks the absorption spectrum of the SOA material suggesting that photodegradation is not limited to the UV wavelengths. Kinetic simulations suggest that RO2+HO2/RO2 reactions represent the dominant route to photochemically active carbonyl and peroxide species in the limonene SOA prepared in these experiments. Similar photodegradation processes are likely to occur in realistic SOA produced by OH- or O3-initiated oxidation of biogenic volatile organic compounds in clean air.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 3
    Publication Date: 2011-05-31
    Description: Statistical response surface methodology (RSM) is successfully applied for a Community Multi-scale Air Quality model (CMAQ) analysis of ozone sensitivity studies. Prediction performance has been demonstrated through cross validation, out-of-sample validation and isopleth validation. Sample methods and key parameters, including the maximum numbers of variables involved in statistical interpolation and training samples have been tested and selected through computational experiments. Overall impacts from individual source categories which include local/regional NOx and VOC emission sources and NOx emissions from power plants for three megacities – Beijing, Shanghai and Guangzhou – were evaluated using an RSM analysis of a July 2005 modeling study. NOx control appears to be beneficial for ozone reduction in the downwind areas which usually experience high ozone levels, and NOx control is likely to be more effective than anthropogenic VOC control during periods of heavy photochemical pollution. Regional NOx source categories are strong contributors to surface ozone mixing ratios in three megacities. Local NOx emission control without regional involvement may raise the risk of increasing urban ozone levels due to the VOC-limited conditions. However, local NOx control provides considerable reduction of ozone in upper layers (up to 1 km where the ozone chemistry is NOx-limited) and helps improve regional air quality in downwind areas. Stricter NOx emission control has a substantial effect on ozone reduction because of the shift from VOC-limited to NOx-limited chemistry. Therefore, NOx emission control should be significantly enhanced to reduce ozone pollution in China.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 4
    Publication Date: 2013-08-06
    Description: An accurate description of emissions is crucial for model simulations to reproduce and interpret observed phenomena over extended time periods. In this study, we used an approach based on activity data to develop a consistent series of spatially resolved emissions in the United States from 1990 to 2010. The state-level anthropogenic emissions of SO2, NOx, CO, NMVOC (non-methane volatile organic compounds), NH3, PM10 and PM2.5 for a total of 49 sectors were estimated based on several long-term databases containing information about activities and emission controls. Activity data for energy-related stationary sources were derived from the State Energy Data System. Corresponding emission factors reflecting implemented emission controls were calculated back from the National Emissions Inventory (NEI) for seven years (i.e., 1990, 1995, 1996, 1999, 2001, 2002 and 2005), and constrained by the AP-42 (US EPA's Compilation of Air Pollutant Emissions Factors) dataset. Activity data for mobile sources including different types of highway vehicles and non-highway equipment were obtained from highway statistics reported by the Federal Highway Administration. The trends in emission factors for highway mobile source were informed by the 2011 National Transportation Statistics. Emissions for all non-energy-related sources were either scaled by the growth ratio of activity indicators or adjusted based on the NEI trends report. Because of the strengthened control efforts, particularly for the power sector and mobile sources, emissions of all pollutants except NH3 were reduced by half over the last two decades. The emission trends developed in this study are comparable with the NEI trend report and EDGAR (Emissions Database for Global Atmospheric Research) data, but better constrained by trends in activity data. Reductions in SO2, NOx, CO and EC (speciation of PM2.5 by SMOKE, Sparse Matrix Operator Kernel Emissions) emissions agree well with the observed changes in ambient SO2, NO2, CO and EC concentrations, suggesting that the various controls on emissions implemented over the last two decades are well represented in the emission inventories developed in this study. These inventories were processed by SMOKE and are now ready to be used for regional chemistry transport model simulations over the 1990–2010 period.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 5
    Publication Date: 2011-04-04
    Description: Anthropogenic emissions of air pollutants in China influence not only local and regional environments but also the global atmospheric environment; therefore, it is important to understand how China's air pollutant emissions will change and how they will affect regional air quality in the future. Emission scenarios in 2020 were projected using forecasts of energy consumption and emission control strategies based on emissions in 2005, and on recent development plans for key industries in China. We developed four emission scenarios: REF[0] (current control legislations and implementation status), PC[0] (improvement of energy efficiencies and current environmental legislation), PC[1] (improvement of energy efficiencies and better implementation of environmental legislation), and PC[2] (improvement of energy efficiencies and strict environmental legislation). Under the REF[0] scenario, the emission of SO2, NOx, VOC and NH3 will increase by 17%, 50%, 49% and 18% in 2020, while PM10 emissions will be reduced by 10% over East China, compared to that in 2005. In PC[2], sustainable energy polices will reduce SO2, NOx and PM10 emissions by 4.1 Tg, 2.6 Tg and 1.8 Tg, respectively; better implementation of current control policies will reduce SO2, NOx and PM10 emission by 2.9 Tg, 1.8 Tg, and 1.4 Tg, respectively; strict emission standards will reduce SO2, NOx and PM10 emissions by 3.2 Tg, 3.9 Tg, and 1.7 Tg, respectively. Under the PC[2] scenario, SO2 and PM10 emissions will decrease by 18% and 38%, while NOx and VOC emissions will increase by 3% and 8%, compared to that in 2005. Future air quality in China was simulated using the Community Multi-scale Air Quality Model (CMAQ). Under REF[0] emissions, compared to 2005, the surface concentrations of SO2, NO2, hourly maximum ozone in summer, PM2.5, total sulfur and nitrogen depositions will increase by 28%, 41%, 8%, 8%, 19% and 25%, respectively, over east China. Under the PC[2] emission scenario, the surface concentrations of SO2, PM2.5, total sulfur depositions will decrease by 18%, 16% and 15%, respectively, and the surface concentrations of NO2, nitrate, hourly maximum ozone in summer, total nitrogen depositions will be kept as 2005 level, over east China. The individual impacts of SO2, NOx, NH3, NMVOC and primary PM emission changes on ozone and PM2.5 concentrations have been analyzed using sensitivity analysis. The results suggest that NOx emission control need to be enhanced during the summertime to obtain both ozone and PM2.5 reduction benefits. NH3 emission controls should also be considered in order to reduce both nitrate concentration and total nitrogen deposition in the future.
    Print ISSN: 1680-7316
    Electronic ISSN: 1680-7324
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 6
    Publication Date: 2012-11-23
    Description: An accurate description of emissions is crucial for model simulations to reproduce and interpret observed phenomena over extended time periods. In this study, we used an approach based on activity data to develop a consistent series of spatially resolved emissions in the United States from 1990 to 2010. The state-level anthropogenic emissions of SO2, NOx, CO, NMVOC, NH3, PM10 and PM2.5 for a total of 49 sectors were estimated based on several long-term databases containing information about activities and emission controls. Activity data for energy-related stationary sources were derived from the State Energy Data System. Corresponding emission factors reflecting implemented emission controls were calculated back from the National Emission Inventory (NEI) for seven years (i.e. 1990, 1995, 1996, 1999, 2001, 2002 and 2005), and constrained by the AP-42 (US EPA's Compilation of Air Pollutant Emissions Factors) dataset. Activity data for mobile sources including different types of highway vehicles and non-highway equipments were obtained from highway statistics reported by the Federal Highway Administration. The trends in emission factors for highway mobile source were informed by the 2011 National Transportation Statistics. Emissions for all non-energy related sources were either scaled by the growth ratio of activity indicators or adjusted based on the NEI trends report. Because of the strengthened control efforts, particularly for the power sector and mobile sources, emissions of all pollutants except NH3 were reduced by half over the last two decades. The emission trends developed in this study are comparable with the NEI trend report and EDGAR (Emissions Database for Global Atmospheric Research) data, but better constrained by trends in activity data. Reductions in SO2 and NOx emissions agree well with the observed changes in ambient SO2 and NO2 concentrations, suggesting that the various controls on SO2 and NOx emissions implemented over the last two decades are well represented in the emission inventories developed in this study. These inventories were processed by SMOKE and are now ready to be used for regional chemistry transport model simulations over the 1990–2010 period.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 7
    Publication Date: 2013-09-10
    Description: Long term datasets of all-sky and clear-sky downwelling shortwave (SW) radiation, cloud cover fraction and aerosol optical depth (AOD) are analyzed together with surface concentration from several networks (e.g. SURFRAD, CASTNET, IMPROVE and ARM) in the United States (US). Seven states with varying climatology are selected to better understand the effects of aerosols and clouds on SW radiation. This analysis aims to assess the effects of reductions in anthropogenic aerosol burden resulting from substantial reductions in emissions of sulfur dioxide (SO2) and nitrogen oxides (NOx) over the past 16 yr across the US on trends in SW radiation. The SO2 and NOx emission data show decreasing trends from 1995 to 2010 which indirectly validates the effects of the Clean Air Act (CAA) in the US. Meanwhile, the total column AOD and surface total PM2.5 observations also show decreasing trends in the eastern US but slightly increasing trends in the western US. Moreover, measured surface concentrations of several other pollutants (i.e. SO2, SO4 and NOx) have the same behavior as the AOD and total PM2.5. First, all-sky downwelling SW radiation is assessed together with the cloud cover. Results of this analysis show strong increasing trends in all-sky downwelling SW radiation with decreasing trends in cloud cover. However, since observations of both all-sky direct and diffuse SW radiation are increasing, there may be other factors contributing to the radiation trends in addition to the decreasing trends in overall cloud cover. To investigate the role of direct radiative effects of aerosols, clear-sky downwelling radiation is analyzed so that cloud effects are eliminated. However, similar increasing trends in clear-sky direct and diffuse SW radiation are observed. While significantly decreasing trends in AOD and surface concentration along with increasing SW radiation (both all-sky and clear-sky) in the eastern US during 1995–2010 imply the occurrence of direct aerosol mediated "brightening", the increasing trends of both all-sky and clear sky diffuse SW radiation contradicts this conclusion since diffuse radiation would be expected to decrease as aerosols direct effects decrease. After investigating several confounding factors, the increasing trend in diffuse SW may be due to more high-level cirrus from increasing air traffic over the US. In contrast to the eastern US, radiation observations in the western US do not show any indication of "brightening" which is consistent with the observations (e.g. AOD, PM2.5 and surface concentration) that show the aerosol loading increasing slightly. This outcome is not unexpected because the CAA controls were mainly aimed at reducing air pollutants emission in the eastern US and air pollutant level in the western US are much lower.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 8
    Publication Date: 2013-08-20
    Description: During 1 to 6 May 2011, a dust event was observed in the Yangtze River Delta region (YRD). The highest PM10 concentration reached over 1000 μg m−3 and the visibility was below 3 km. In this study, the Community Multi-scale Air Quality modeling system (CMAQ5.0) coupled with an in-line windblown dust model was used to simulate the formation, spatial and temporal characteristics of this dust event, and analyze its impacts on deposition and photochemistry. The threshold friction velocity for loose smooth surface in the dust model was revised based on Chinese data to improve the model performance. The comparison between predictions and observations indicates the revised model can reproduce the transport and pollution of the event. The simulation results show that the dust event was affected by formation and transport of Mongolian cyclone and cold air. Totally about 695 kt dust particles (PM10) were emitted in Xinjiang Province and Mongolia during 28 to 30 April, the dust band swept northern, eastern China and then arrived in the YRD region on 1 May 2011. The transported dust particles increased the mean surface layer concentrations of PM10 in the YRD region by 372% during 1 to 6 May and the impacts weakened from north to south due to the removal of dust particles along the path. Accompanied by high PM concentration, the dry deposition, wet deposition and total deposition of PM10 in the YRD reached 184.7 kt, 172.6 kt and 357.32 kt, respectively. These deposited particles are very harmful because of their impacts on urban environment as well as air quality and human health when resuspending in the atmosphere. Due to the impacts of mineral dust on atmospheric photolysis, the concentrations of O3 and OH were reduced by 1.5% and 3.1% in the whole China, and by 9.4% and 12.1% in the YRD region, respectively. The work of this manuscript is meaningful for understanding the dust emissions in China as well as for the application of CMAQ in Asia. It is also helpful to understand the formation mechanism and impacts of dust pollution in the YRD.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 9
    Publication Date: 2015-07-01
    Description: Multi-decadal simulations with the coupled WRF-CMAQ model have been conducted to systematically investigate the changes in anthropogenic emissions of SO2 and NOx over the past 21 years (1990–2010) across the United States (US), their impacts on anthropogenic aerosol loading over North America, and subsequent impacts on regional radiation budgets. In particular, this study attempts to determine the consequences of the changes in tropospheric aerosol burden arising from substantial reductions in emissions of SO2 and NOx associated with control measures under the Clean Air Act (CAA) especially on trends in solar radiation. Extensive analyses conducted by Gan et al. (2014) utilizing observations (e.g. SURFRAD, CASTNET, IMPROVE and ARM) over the past 16 years (1995–2010) indicate a shortwave (SW) radiation (both all-sky and clear-sky) "brightening" in the US. The relationship of the radiation brightening trend with decreases in the aerosol burden is less apparent in the western US. One of the main reasons for this is that the emission controls under the CAA were aimed primarily at reducing pollutants in areas violating national air quality standards, most of which were located in the eastern US while the relatively less populated areas in the western US were less polluted at the beginning of this study period. Comparisons of model results with observations of aerosol optical depth (AOD), aerosol concentration, and radiation demonstrate that the coupled WRF-CMAQ model is capable of replicating the trends well even through it tends to underestimate the AOD. In particular, the sulfate concentration predictions were well matched with the observations. The discrenpancies found in the clear-sky diffuse SW radiation are likely due to several factors such as potential increase of ice particles associated with increasing air traffic, the definition of "clear-sky" in the radiation retrieval methodology and aerosol semi-direct and/or indirect effects which cannot be readily isolated from the observed data.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 10
    Publication Date: 2015-05-28
    Description: Satellite remote sensing of tropospheric nitrogen dioxide (NO2) can provide valuable information for estimating surface nitrogen oxides (NOx) emissions. Using an exponentially-modified Gaussian (EMG) method and taking into account the effect of wind on observed NO2 distributions, we estimate three-year moving-average emissions of summertime NOx from 35 US urban areas directly from NO2 retrievals of the Ozone Monitoring Instrument (OMI) during 2005–2014. Following the conclusions of previous studies that the EMG method provides robust and accurate emission estimates under strong-wind conditions, we derive top-down NOx emissions from each urban area by applying the EMG method to OMI data with wind speeds greater than 3–5 m s−1. Meanwhile, we find that OMI NO2 observations under weak-wind conditions (i.e., 〈 3 m s−1) are qualitatively better correlated with the surface NOx source strength in comparison to all-wind OMI maps; and therefore we use them to calculate the satellite-observed NO2 burdens of urban areas and compare with NOx emission estimates. The EMG results show that OMI-derived NOx emissions are highly correlated (R 〉 0.93) with weak-wind OMI NO2 burdens as well as bottom-up NOx emission estimates over 35 urban areas, implying a linear response of the OMI observations to surface emissions under weak-wind conditions. The simultaneous, EMG-obtained, effective NO2 lifetimes (~3.5 ± 1.3 h), however, are biased low in comparison to the summertime NO2 chemical lifetimes. In general, isolated urban areas with NOx emission intensities greater than ~ 2 Mg h−1 produce statistically significant weak-wind signals in three-year average OMI data. From 2005 to 2014, we estimate that total OMI-derived NOx emissions over all selected US urban areas decreased by 49%, consistent with reductions of 43, 47, 49, and 44% in the total bottom-up NOx emissions, the sum of weak-wind OMI NO2 columns, the total weak-wind OMI NO2 burdens, and the averaged NO2 concentrations, respectively, reflecting the success of NOx control programs for both mobile sources and power plants. The decrease rates of these NOx-related quantities are found to be faster (i.e., −6.8 to −9.3% yr−1) before 2010 and slower (i.e., −3.4 to −4.9% yr−1) after 2010. For individual urban areas, we calculate the R values of pair-wise trends among the OMI-derived and bottom-up NOx emissions, the weak-wind OMI NO2 burdens, and ground-based NO2 measurements; and high correlations are found for all urban areas (median R = 0.8), particularly large ones (R up to 0.97). The results of the current work indicate that using the EMG method and considering the wind effect, the OMI data allow for the estimation of NOx emissions from urban areas and the direct constraint of emission trends with reasonable accuracy.
    Electronic ISSN: 1680-7375
    Topics: Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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