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  • 1
    In: Atmosphere, MDPI AG, Vol. 14, No. 1 ( 2023-01-10), p. 154-
    Abstract: The Chinese government introduced regulations to control emissions and reduce the level of NOx pollutants for the first time with the 12th Five-Year Plan in 2011. Since then, the changes in NOx emissions have been assessed using various approaches to evaluate the impact of the regulations. Complementary to the previous studies, this study estimates anthropogenic NOx emissions in 2015 and 2019 over Eastern China using as a reference the Hemispheric Transport of Air Pollution (HTAP) v2.2 emission inventory for 2010 and the new variational inversion system the Community Inversion Framework (CIF) interfaced with the CHIMERE regional chemistry transport model and OMI satellite observations. We also compared the estimated NOx emissions with the independent Multi-resolution Emission Inventory for China (MEIC) v1.3, from 2015. The inversions show a slight global decrease in NOx emissions (in 2015 and 2019 compared to 2010), mainly limited to the most urbanized and industrialized locations. In the locations such as Baotou, Pearl River Delta, and Wuhan, the estimations in 2015 compared to 2010 are consistent with the target reduction (10%) of the 12th Five-Year Plan. Comparisons between our emission estimates and MEIC emissions in 2015 suggest that our estimates likely underestimate the emission reductions between 2010 and 2015 in the most polluted locations of Eastern China. However, our estimates suggest that the MEIC inventory overestimates emissions in regions where MEIC indicates an increase of the emissions compared to 2010.
    Type of Medium: Online Resource
    ISSN: 2073-4433
    Language: English
    Publisher: MDPI AG
    Publication Date: 2023
    detail.hit.zdb_id: 2605928-9
    SSG: 23
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  • 2
    In: Earth System Science Data, Copernicus GmbH, Vol. 11, No. 3 ( 2019-09-18), p. 1411-1436
    Abstract: Abstract. Atmospheric carbon monoxide (CO) concentrations have been decreasing since 2000, as observed by both satellite- and ground-based instruments, but global bottom-up emission inventories estimate increasing anthropogenic CO emissions concurrently. In this study, we use a multi-species atmospheric Bayesian inversion approach to attribute satellite-observed atmospheric CO variations to its sources and sinks in order to achieve a full closure of the global CO budget during 2000–2017. Our observation constraints include satellite retrievals of the total column mole fraction of CO, formaldehyde (HCHO), and methane (CH4) that are all major components of the atmospheric CO cycle. Three inversions (i.e., 2000–2017, 2005–2017, and 2010–2017) are performed to use the observation data to the maximum extent possible as they become available and assess the consistency of inversion results to the assimilation of more trace gas species. We identify a declining trend in the global CO budget since 2000 (three inversions are broadly consistent during overlapping periods), driven by reduced anthropogenic emissions in the US and Europe (both likely from the transport sector), and in China (likely from industry and residential sectors), as well as by reduced biomass burning emissions globally, especially in equatorial Africa (associated with reduced burned areas). We show that the trends and drivers of the inversion-based CO budget are not affected by the inter-annual variation assumed for prior CO fluxes. All three inversions contradict the global bottom-up inventories in the world's top two emitters: for the sign of anthropogenic emission trends in China (e.g., here -0.8±0.5 % yr−1 since 2000, while the prior gives 1.3±0.4 % yr−1) and for the rate of anthropogenic emission increase in South Asia (e.g., here 1.0±0.6 % yr−1 since 2000, smaller than 3.5±0.4 % yr−1 in the prior inventory). The posterior model CO concentrations and trends agree well with independent ground-based observations and correct the prior model bias. The comparison of the three inversions with different observation constraints further suggests that the most complete constrained inversion that assimilates CO, HCHO, and CH4 has a good representation of the global CO budget, and therefore matches best with independent observations, while the inversion only assimilating CO tends to underestimate both the decrease in anthropogenic CO emissions and the increase in the CO chemical production. The global CO budget data from all three inversions in this study can be accessed from https://doi.org/10.6084/m9.figshare.c.4454453.v1 (Zheng et al., 2019).
    Type of Medium: Online Resource
    ISSN: 1866-3516
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2475469-9
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  • 3
    In: Atmosphere, MDPI AG, Vol. 13, No. 7 ( 2022-07-13), p. 1101-
    Abstract: The objective of this study is to assess and understand the NH3 recent trends and to identify the key components driving its concentrations. We have simulated the seasonal cycle, the interannual variability, and the trends in NH3 vertical column densities (VCD) from 2008 to 2015 over Europe, with the CHIMERE regional chemistry–transport model. We have also confronted the simulations against the Infrared Atmospheric Sounding Interferometer (IASI) satellite observations. IASI often shows a strong maximum in summer in addition to the spring peak, whereas CHIMERE only shows a slight peak in summer some years. This result could point to a misrepresentation of the temporal profile of the NH3 emissions, i.e., to missing emission sources during summertime either due to more than expected fertilizer use or to increased volatilization under warmer conditions. The simulated NH3 VCDs present an increasing trend over continental Europe (+2.7 ± 1.0 %/yr) but also at the national scale for Spain, Germany, UK, France, and Poland. Sensitivity tests indicate that these simulated positive trends are mainly due to (i) the trends in NH3 emissions, found heterogeneous in the EMEP NH3 emissions with strong disparities depending on the country, and (ii) the negative trends in NOx and SOx emissions. The impact of reductions in NO2 and SO2 emissions on NH3 concentrations should therefore be taken into account in future policies. This simulated NH3 VCD increase at the European scale is confirmed by IASI-v3R satellite observations in spring and summer, when ammonia emissions strongly contribute to the annual budget in accordance with crop requirements. Nevertheless, there are remaining differences about the significance and magnitude between the simulated and observed trends at the national scale, and it warrants further investigation.
    Type of Medium: Online Resource
    ISSN: 2073-4433
    Language: English
    Publisher: MDPI AG
    Publication Date: 2022
    detail.hit.zdb_id: 2605928-9
    SSG: 23
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  • 4
    In: Journal of Geophysical Research: Atmospheres, American Geophysical Union (AGU), Vol. 118, No. 9 ( 2013-05-16), p. 3891-3904
    Type of Medium: Online Resource
    ISSN: 2169-897X
    Language: English
    Publisher: American Geophysical Union (AGU)
    Publication Date: 2013
    detail.hit.zdb_id: 710256-2
    detail.hit.zdb_id: 2016800-7
    detail.hit.zdb_id: 2969341-X
    SSG: 16,13
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  • 5
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 19, No. 10 ( 2019-05-20), p. 6701-6716
    Abstract: Abstract. Air pollution reaching hazardous levels in many Chinese cities has been a major concern in China over the past decades. New policies have been applied to regulate anthropogenic pollutant emissions, leading to changes in atmospheric composition and in particulate matter (PM) production. Increasing levels of atmospheric ammonia columns have been observed by satellite during recent years. In particular, observations from the Infrared Atmospheric Sounding Interferometer (IASI) reveal an increase of these columns by 15 % and 65 % from 2011 to 2013 and 2015, respectively, over eastern China. In this paper we performed model simulations for 2011, 2013 and 2015 in order to understand the origin of this increase and to quantify the link between ammonia and the inorganic components of particles: NH4(p)+/SO4(p)2-/NO3(p)-. Interannual change of meteorology can be excluded as a reason: year 2015 meteorology leads to enhanced sulfate production over eastern China, which increases the ammonium and decreases the ammonia content, which is contrary to satellite observations. Reductions in SO2 and NOx emissions from 2011 to 2015 of 37.5 % and 21 % respectively, as constrained from satellite data, lead to decreased inorganic matter (by 14 % for NH4(p)++SO4(p)2-+NO3(p)-). This in turn leads to increased gaseous NH3(g) tropospheric columns by as much as 24 % and 49 % (sampled corresponding to IASI data availability) from 2011 to 2013 and 2015 respectively and thus can explain most of the observed increase.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2019
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 6
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 22 ( 2018-11-20), p. 16439-16459
    Abstract: Abstract. China is a highly polluted region, particularly the North China Plain (NCP). However, emission reductions have been occurring in China for about the last 10 years; these reduction measures have been in effect since 2006 for SO2 emissions and since 2010 for NOx emissions. Recent studies have shown a decrease in the NO2 tropospheric column since 2013 that has been attributed to the reduction in NOx emissions. Quantifying how these emission reductions translate regarding ozone concentrations remains unclear due to apparent inconsistencies between surface and satellite observations. In this study, we use the lower tropospheric (LT) columns (surface – 6 km a.s.l. – above sea level) derived from the IASI-A satellite instrument to describe the variability and trend in LT ozone over the NCP for the 2008–2016 period. First, we investigate the IASI retrieval stability and robustness based on the influence of atmospheric conditions (thermal conditions and aerosol loading) and retrieval sensitivity changes. We compare IASI-A observations with the independent IASI-B instrument aboard the Metop-B satellite as well as comparing them with surface and ozonesonde measurements. The conclusion from this evaluation is that the LT ozone columns retrieved from IASI-A are reliable for deriving a trend representative of the lower/free troposphere (3–5 km). Deseasonalized monthly time series of LT ozone show two distinct periods: the first period (2008–2012) with no significant trend (〈−0.1 % yr−1) and a second period (2013–2016) with a highly significant negative trend of −1.2 % yr−1, which leads to an overall significant trend of −0.77 % yr−1 for the 2008–2016 period. We explore the dynamical and chemical factors that could explain these negative trends using a multivariate linear regression model and chemistry transport model simulations to evaluate the sensitivity of ozone to the reduction in NOx emissions. The results show that the negative trend observed from IASI for the 2013–2016 period is almost equally attributed to large-scale dynamical processes and emissions reduction, with the large El Niño event in 2015–2016 and the reduction of NOx emissions being the main contributors. For the entire 2008–2016 period, large-scale dynamical processes explain more than half of the observed trend, with a possible reduction of the stratosphere–troposphere exchanges being the main contributor. Large-scale transport and advection, evaluated using CO as a proxy, only contributes to a small part of the trends (∼10 %). However, a residual significant negative trend remains; this shows the limitation of linear regression models regarding their ability to account for nonlinear processes such as ozone chemistry and stresses the need for a detailed evaluation of changes in chemical regimes with the altitude.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 7
    In: Earth System Science Data, Copernicus GmbH, Vol. 15, No. 10 ( 2023-10-05), p. 4295-4370
    Abstract: Abstract. Quantification of land surface–atmosphere fluxes of carbon dioxide (CO2) and their trends and uncertainties is essential for monitoring progress of the EU27+UK bloc as it strives to meet ambitious targets determined by both international agreements and internal regulation. This study provides a consolidated synthesis of fossil sources (CO2 fossil) and natural (including formally managed ecosystems) sources and sinks over land (CO2 land) using bottom-up (BU) and top-down (TD) approaches for the European Union and United Kingdom (EU27+UK), updating earlier syntheses (Petrescu et al., 2020, 2021). Given the wide scope of the work and the variety of approaches involved, this study aims to answer essential questions identified in the previous syntheses and understand the differences between datasets, particularly for poorly characterized fluxes from managed and unmanaged ecosystems. The work integrates updated emission inventory data, process-based model results, data-driven categorical model results, and inverse modeling estimates, extending the previous period 1990–2018 to the year 2020 to the extent possible. BU and TD products are compared with the European national greenhouse gas inventory (NGHGI) reported by parties including the year 2019 under the United Nations Framework Convention on Climate Change (UNFCCC). The uncertainties of the EU27+UK NGHGI were evaluated using the standard deviation reported by the EU member states following the guidelines of the Intergovernmental Panel on Climate Change (IPCC) and harmonized by gap-filling procedures. Variation in estimates produced with other methods, such as atmospheric inversion models (TD) or spatially disaggregated inventory datasets (BU), originate from within-model uncertainty related to parameterization as well as structural differences between models. By comparing the NGHGI with other approaches, key sources of differences between estimates arise primarily in activities. System boundaries and emission categories create differences in CO2 fossil datasets, while different land use definitions for reporting emissions from land use, land use change, and forestry (LULUCF) activities result in differences for CO2 land. The latter has important consequences for atmospheric inversions, leading to inversions reporting stronger sinks in vegetation and soils than are reported by the NGHGI. For CO2 fossil emissions, after harmonizing estimates based on common activities and selecting the most recent year available for all datasets, the UNFCCC NGHGI for the EU27+UK accounts for 926 ± 13 Tg C yr−1, while eight other BU sources report a mean value of 948 [937,961] Tg C yr−1 (25th, 75th percentiles). The sole top-down inversion of fossil emissions currently available accounts for 875 Tg C in this same year, a value outside the uncertainty of both the NGHGI and bottom-up ensemble estimates and for which uncertainty estimates are not currently available. For the net CO2 land fluxes, during the most recent 5-year period including the NGHGI estimates, the NGHGI accounted for −91 ± 32 Tg C yr−1, while six other BU approaches reported a mean sink of −62 [-117,-49] Tg C yr−1, and a 15-member ensemble of dynamic global vegetation models (DGVMs) reported −69 [-152,-5] Tg C yr−1. The 5-year mean of three TD regional ensembles combined with one non-ensemble inversion of −73 Tg C yr−1 has a slightly smaller spread (0th–100th percentiles of [-135,+45] Tg C yr−1), and it was calculated after removing net land–atmosphere CO2 fluxes caused by lateral transport of carbon (crop trade, wood trade, river transport, and net uptake from inland water bodies), resulting in increased agreement with the NGHGI and bottom-up approaches. Results at the category level (Forest Land, Cropland, Grassland) generally show good agreement between the NGHGI and category-specific models, but results for DGVMs are mixed. Overall, for both CO2 fossil and net CO2 land fluxes, we find that current independent approaches are consistent with the NGHGI at the scale of the EU27+UK. We conclude that CO2 emissions from fossil sources have decreased over the past 30 years in the EU27+UK, while land fluxes are relatively stable: positive or negative trends larger (smaller) than 0.07 (−0.61) Tg C yr−2 can be ruled out for the NGHGI. In addition, a gap on the order of 1000 Tg C yr−1 between CO2 fossil emissions and net CO2 uptake by the land exists regardless of the type of approach (NGHGI, TD, BU), falling well outside all available estimates of uncertainties. However, uncertainties in top-down approaches to estimate CO2 fossil emissions remain uncharacterized and are likely substantial, in addition to known uncertainties in top-down estimates of the land fluxes. The data used to plot the figures are available at https://doi.org/10.5281/zenodo.8148461 (McGrath et al., 2023).
    Type of Medium: Online Resource
    ISSN: 1866-3516
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2023
    detail.hit.zdb_id: 2475469-9
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  • 8
    In: Atmospheric Measurement Techniques, Copernicus GmbH, Vol. 13, No. 7 ( 2020-07-21), p. 3923-3937
    Abstract: Abstract. In this paper, we present the first multiyear time series of atmospheric ammonia (NH3) ground-based measurements in the Paris region (Créteil, 48.79∘ N, 2.44∘ E, France) retrieved with the midresolution “Observations of the Atmosphere by Solar absorption Infrared Spectroscopy” (OASIS) ground-based Fourier transform infrared solar observatory. Located in an urban region, OASIS has previously been used for monitoring air quality (tropospheric ozone and carbon monoxide) thanks to its specific column sensitivity across the whole troposphere down to the atmospheric boundary layer. A total of 4920 measurements of atmospheric total columns of ammonia have been obtained from 2009 to 2017, with uncertainties ranging from 20 % to 35 %, and have been compared with NH3 concentrations derived from the Infrared Atmospheric Sounding Interferometer (IASI). OASIS ground-based measurements show significant interannual and seasonal variabilities of atmospheric ammonia. NH3 total columns over the Paris megacity (12 million people) vary seasonally by 2 orders of magnitude from approximately 0.1×1016 molec. cm−2 in winter to 10×1016 molec. cm−2 for spring peaks, probably due to springtime spreading of fertilizers on surrounding croplands.
    Type of Medium: Online Resource
    ISSN: 1867-8548
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2505596-3
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  • 9
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 21 ( 2020-11-12), p. 13481-13495
    Abstract: Abstract. Agriculture is the main source of ammonia (NH3) in France, an important gaseous precursor of atmospheric particulate matter (PM). National and global emission inventories are known to have difficulty representing the large spatial and temporal variability inherent to atmospheric NH3. In this study, we compare NH3 emissions in France during spring 2011 from one reference inventory, the TNO inventory, and two alternative inventories that account in different manners for both the spatial and temporal variabilities of the emissions: (i) the NH3SAT satellite-derived inventory based on IASI NH3 columns and (ii) the CADASTRE-CIT inventory that combines NH3 emissions due to nitrogen fertilization calculated with the mechanistic model VOLT'AIR on the database of the CADASTRE_NH3 framework and other source emissions from the CITEPA. The total spring budgets, from March to May 2011, at the national level are higher when calculated with both alternative inventories than with the reference, the difference being more marked with CADASTRE-CIT. NH3SAT and CADASTRE-CIT inventories both yield to large NH3 spring emissions due to fertilization on soils with high pH in the northeastern part of France (65 and 135 kt NH3, respectively, vs. 48 kt NH3 for TNO-GEN), while soil properties are not accounted for by the TNO-GEN methodology. For the other parts of France, the differences are smaller. The timing of fertilization and associated ammonia emissions is closely related to the nitrogen requirements and hence the phenological stage of the crops, and therefore to the crop year's specific weather conditions. Maximum emissions are observed in March for 2011 for some regions for both alternative inventories, while April is the period with maximum emissions for the reference inventory regardless of the region or the year. Comparing the inventories at finer temporal resolutions, typically at daily scale, large differences are found. The convergence of alternative, independent and complementary methods on the spatiotemporal representation of the spring NH3 emissions, particularly over areas where the contribution of mineral fertilizer spreading to the spring budget is strong, encourages further developments in both prospective complementary directions, as this will help improve national NH3 emission inventories.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 10
    Online Resource
    Online Resource
    Copernicus GmbH ; 2016
    In:  Atmospheric Chemistry and Physics Vol. 16, No. 14 ( 2016-07-25), p. 9089-9108
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 16, No. 14 ( 2016-07-25), p. 9089-9108
    Abstract: Abstract. A Bayesian inversion system is used to evaluate the capability of the current global surface network and of the space-borne GOSAT/TANSO-FTS and IASI instruments to quantify surface flux anomalies of methane at various spatial (global, semi-hemispheric and regional) and time (seasonal, yearly, 3-yearly) scales. The evaluation is based on a signal-to-noise ratio analysis, the signal being the methane fluxes inferred from the surface-based inversion from 2000 to 2011 and the noise (i.e., precision) of each of the three observing systems being computed from the Bayesian equation. At the global and semi-hemispheric scales, all observing systems detect flux anomalies at most of the tested timescales. At the regional scale, some seasonal flux anomalies are detected by the three observing systems, but year-to-year anomalies and longer-term trends are only poorly detected. Moreover, reliably detected regions depend on the reference surface-based inversion used as the signal. Indeed, tropical flux inter-annual variability, for instance, can be attributed mostly to Africa in the reference inversion or spread between tropical regions in Africa and America. Our results show that inter-annual analyses of methane emissions inferred by atmospheric inversions should always include an uncertainty assessment and that the attribution of current trends in atmospheric methane to particular regions' needs increased effort, for instance, gathering more observations (in the future) and improving transport models. At all scales, GOSAT generally shows the best performance of the three observing systems.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2016
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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