• Energy Research

Abstract. Multi-annual satellite measurements of tropospheric NO2 columns are used for evaluation of CO2 emission changes in China in the period from 1996 to 2008. Indirect annual top-down estimates of CO2 emissions are derived from the satellite NO2 columns measurements by means of a simple inverse modeling procedure involving simulations performed with the CHIMERE mesoscale chemistry transport model and the CO2 to NOx emission ratios from the Emission Database for Global Atmospheric Research version 4.2 (EDGAR v4.2) global anthropogenic emission inventory. Exponential trends in the normalized time series of annual emission are evaluated separately for the periods from 1996 to 2001 and from 2001 to 2008. The results indicate that the both periods manifest strong positive trends in the CO2 emissions, and that the trend in the second period was significantly larger than the trend in the first period. Specifically, the trends in the first and second periods are estimated to be in the range from 3.7 to 8.0 and from 9.5 to 13.0 percent per year, respectively, taking into account both statistical and probable systematic uncertainties. Comparison of our top-down estimates of the CO2 emission changes with the corresponding bottom-up estimates provided by EDGAR v4.2 and Global Carbon Project (GCP) emission inventories reveals that while acceleration of the CO2 emission growth in the considered period is a common feature of the both kinds of estimates, nonlinearity in the CO2 emission changes may be strongly exaggerated in the emission inventories. Specifically, the atmospheric NO2 observations do not confirm the existence of a sharp bend in the emission inventory data time series in the period from 2000 to 2002. A significant quantitative difference is revealed between the bottom-up and top-down estimates of the CO2 emission trend in the period from 1996 to 2001 (specifically, the trend was not positive according to the emission inventories, but is strongly positive in our estimates). These results confirm the findings of earlier studies which indicated probable large uncertainties in the energy production and other activity data from international energy statistics used as the input information in the emission inventories for China. For the period from 2001 to 2008, the different kinds of estimates agree within the uncertainty range. In general, satellite measurements of tropospheric NO2 are shown to be a useful source of information on CO2 sources colocated with sources of nitrogen oxides; the corresponding potential of these measurements should be exploited further in future studies.

Abstract. Multi-annual satellite measurements of tropospheric NO2 columns are used for evaluation of CO2 emission changes in China in the period from 1996 to 2008. Indirect annual top-down estimates of CO2 emissions are derived from the satellite NO2 columns measurements by means of a simple inverse modeling procedure involving simulations performed with the CHIMERE mesoscale chemistry transport model and the CO2 to NOx emission ratios from the Emission Database for Global Atmospheric Research version 4.2 (EDGAR v4.2) global anthropogenic emission inventory. Exponential trends in the normalized time series of annual emission are evaluated separately for the periods from 1996 to 2001 and from 2001 to 2008. The results indicate that the both periods manifest strong positive trends in the CO2 emissions, and that the trend in the second period was significantly larger than the trend in the first period. Specifically, the trends in the first and second periods are estimated to be in the range from 3.7 to 8.0 and from 9.5 to 13.0 percent per year, respectively, taking into account both statistical and probable systematic uncertainties. Comparison of our top-down estimates of the CO2 emission changes with the corresponding bottom-up estimates provided by EDGAR v4.2 and Global Carbon Project (GCP) emission inventories reveals that while acceleration of the CO2 emission growth in the considered period is a common feature of the both kinds of estimates, nonlinearity in the CO2 emission changes may be strongly exaggerated in the emission inventories. Specifically, the atmospheric NO2 observations do not confirm the existence of a sharp bend in the emission inventory data time series in the period from 2000 to 2002. A significant quantitative difference is revealed between the bottom-up and top-down estimates of the CO2 emission trend in the period from 1996 to 2001 (specifically, the trend was not positive according to the emission inventories, but is strongly positive in our estimates). These results confirm the findings of earlier studies which indicated probable large uncertainties in the energy production and other activity data from international energy statistics used as the input information in the emission inventories for China. For the period from 2001 to 2008, the different kinds of estimates agree within the uncertainty range. In general, satellite measurements of tropospheric NO2 are shown to be a useful source of information on CO2 sources colocated with sources of nitrogen oxides; the corresponding potential of these measurements should be exploited further in future studies.

Emissions from fossil fuel combustion and biomass burning reduce local air quality and affect global tropospheric chemistry. Nitrogen oxides are emitted by all combustion processes and play a key part in the photochemically induced catalytic production of ozone, which results in summer smog and has increased levels of tropospheric ozone globally. Release of nitrogen oxide also results in nitric acid deposition, and--at least locally--increases radiative forcing effects due to the absorption of downward propagating visible light. Nitrogen oxide concentrations in many industrialized countries are expected to decrease, but rapid economic development has the potential to increase significantly the emissions of nitrogen oxides in parts of Asia. Here we present the tropospheric column amounts of nitrogen dioxide retrieved from two satellite instruments GOME and SCIAMACHY over the years 1996-2004. We find substantial reductions in nitrogen dioxide concentrations over some areas of Europe and the USA, but a highly significant increase of about 50 per cent-with an accelerating trend in annual growth rate-over the industrial areas of China, more than recent bottom-up inventories suggest.

Emissions from fossil fuel combustion and biomass burning reduce local air quality and affect global tropospheric chemistry. Nitrogen oxides are emitted by all combustion processes and play a key part in the photochemically induced catalytic production of ozone, which results in summer smog and has increased levels of tropospheric ozone globally. Release of nitrogen oxide also results in nitric acid deposition, and--at least locally--increases radiative forcing effects due to the absorption of downward propagating visible light. Nitrogen oxide concentrations in many industrialized countries are expected to decrease, but rapid economic development has the potential to increase significantly the emissions of nitrogen oxides in parts of Asia. Here we present the tropospheric column amounts of nitrogen dioxide retrieved from two satellite instruments GOME and SCIAMACHY over the years 1996-2004. We find substantial reductions in nitrogen dioxide concentrations over some areas of Europe and the USA, but a highly significant increase of about 50 per cent-with an accelerating trend in annual growth rate-over the industrial areas of China, more than recent bottom-up inventories suggest.

Retrievals of trace gas columns from the measurements of backscattered radiation by GOME (Global Ozone Monitoring Experiment) show that enhanced tropospheric columns of ozone (O3), nitrogen dioxide (NO2) and formaldehyde (HCHO), over the African continent occur frequently. This study focuses on the behaviour of trace gases over Africa in September 1997, a period impacted by the strongest known El Niño phase of the ENSO. It investigates our qualitative and quantitative understanding of the retrieved tropospheric trace gas column densities. The emissions of NOx and volatile organic compounds (VOC) from biomass burning, biogenic sources and lightning and their photochemical transformation have been investigated. By performing a trajectory analysis, the transport of air masses from the different emission regions was analysed and the potential atmospheric spatial distribution determined. BRemen's Atmospheric PHOtochemical model (BRAPHO) was applied to compute the chemistry along a large number of trajectories. From these results, tropospheric column amounts of O3, NO2 and HCHO were derived. Tropospheric trace gas columns retrieved from GOME measurements and those calculated are in reasonable agreement. Their general spatial extent was similar in the lower troposphere but the modeled trace gas columns in the upper troposphere were located south of the retrieved columns. We attribute this behaviour to uncertainties in the ERA-40 meteorological data in the upper troposphere. The significance of biomass burning and of biogenic emissions with respect to HCHO columns over Africa was investigated. The analysis reveals that the total amounts of HCHO generated over Africa during September 1997 as a result of biomass burning and biogenic emissions are similar. However the HCHO from biogenic sources has the highest specific columns and these are located close to their source. In comparison the HCHO from biomass burning is predicted to be produced and transported over a much wider area. Overall all the emission processes mix together to produce the plume of O3.

Retrievals of trace gas columns from the measurements of backscattered radiation by GOME (Global Ozone Monitoring Experiment) show that enhanced tropospheric columns of ozone (O3), nitrogen dioxide (NO2) and formaldehyde (HCHO), over the African continent occur frequently. This study focuses on the behaviour of trace gases over Africa in September 1997, a period impacted by the strongest known El Niño phase of the ENSO. It investigates our qualitative and quantitative understanding of the retrieved tropospheric trace gas column densities. The emissions of NOx and volatile organic compounds (VOC) from biomass burning, biogenic sources and lightning and their photochemical transformation have been investigated. By performing a trajectory analysis, the transport of air masses from the different emission regions was analysed and the potential atmospheric spatial distribution determined. BRemen's Atmospheric PHOtochemical model (BRAPHO) was applied to compute the chemistry along a large number of trajectories. From these results, tropospheric column amounts of O3, NO2 and HCHO were derived. Tropospheric trace gas columns retrieved from GOME measurements and those calculated are in reasonable agreement. Their general spatial extent was similar in the lower troposphere but the modeled trace gas columns in the upper troposphere were located south of the retrieved columns. We attribute this behaviour to uncertainties in the ERA-40 meteorological data in the upper troposphere. The significance of biomass burning and of biogenic emissions with respect to HCHO columns over Africa was investigated. The analysis reveals that the total amounts of HCHO generated over Africa during September 1997 as a result of biomass burning and biogenic emissions are similar. However the HCHO from biogenic sources has the highest specific columns and these are located close to their source. In comparison the HCHO from biomass burning is predicted to be produced and transported over a much wider area. Overall all the emission processes mix together to produce the plume of O3.