With the rapid growth in population and economic development, emissions of greenhouse gases (GHGs) from the Indian subcontinent have sharply increased during recent decades. However, evaluation of ...regional fluxes of GHGs and characterization of their spatial and temporal variations by atmospheric inversions remain uncertain due to a sparse regional atmospheric observation network. As a result of an Indo-French collaboration, three new atmospheric stations were established in India at Hanle (HLE), Pondicherry (PON) and Port Blair (PBL), with the objective of monitoring the atmospheric concentrations of GHGs and other trace gases. Here we present the results of the measurements of CO2, CH4, N2O, SF6, CO, and H2 from regular flask sampling at these three stations over the period 2007-2011. For each species, annual means, seasonal cycles and gradients between stations were calculated and related to variations in natural GHG fluxes, anthropogenic emissions, and monsoon circulations. Covariances between species at the synoptic scale were analyzed to investigate the likely source(s) of emissions. The flask measurements of various trace gases at the three stations have the potential to constrain the inversions of fluxes over southern and northeastern India. However, this network of ground stations needs further extension to other parts of India to better constrain the GHG budgets at regional and continental scales.
This study presents two methods for estimating methane emissions from a waste water treatment plant (WWTP) along with results from a measurement campaign at a WWTP in Valence, France. These methods, ...chamber measurements and tracer release, rely on Fourier transform infrared spectroscopy and cavity ring-down spectroscopy instruments. We show that the tracer release method is suitable for quantifying facility- and some process-scale emissions, while the chamber measurements provide insight into individual process emissions. Uncertainties for the two methods are described and discussed. Applying the methods to CH4 emissions of the WWTP, we confirm that the open basins are not a major source of CH4 on the WWTP (about 10 % of the total emissions), but that the pretreatment and sludge treatment are the main emitters. Overall, the waste water treatment plant is representative of an average French WWTP.
To develop an accurate measurement network of greenhouse gases, instruments in the field need to be stable and precise and thus require infrequent calibrations and a low consumption of consumables. ...For about 10 years, cavity ring-down spectroscopy (CRDS) analyzers have been available that meet these stringent requirements for precision and stability. Here, we present the results of tests of CRDS instruments in the laboratory (47 instruments) and in the field (15 instruments). The precision and stability of the measurements are studied. We demonstrate that, thanks to rigorous testing, newer models generally perform better than older models, especially in terms of reproducibility between instruments. In the field, we see the importance of individual diagnostics during the installation phase, and we show the value of calibration and target gases that assess the quality of the data. Finally, we formulate recommendations for use of these analyzers in the field.
To mitigate methane emission from urban natural gas distribution systems, it is crucial to understand local leak rates and occurrence rates. To explore urban methane emissions in cities outside the ...U.S., where significant emissions were found previously, mobile measurements were performed in 12 cities across eight countries. The surveyed cities range from medium size, like Groningen, NL, to large size, like Toronto, CA, and London, UK. Furthermore, this survey spanned across European regions from Barcelona, ES, to Bucharest, RO. The joint analysis of all data allows us to focus on general emission behavior for cities with different infrastructure and environmental conditions. We find that all cities have a spectrum of small, medium, and large methane sources in their domain. The emission rates found follow a heavy-tailed distribution, and the top 10% of emitters account for 60–80% of total emissions, which implies that strategic repair planning could help reduce emissions quickly. Furthermore, we compare our findings with inventory estimates for urban natural gas-related methane emissions from this sector in Europe. While cities with larger reported emissions were found to generally also have larger observed emissions, we find clear discrepancies between observation-based and inventory-based emission estimates for our 12 cities.
Results from the Trainou tall tower measurement station installed in 2006 are presented for atmospheric measurements of CO2, CH4, N2O, SF6, CO, H2 mole fractions and radon-222 activity. Air is ...sampled from four sampling heights (180, 100, 50 and 5 m) of the Trainou 200 m television tower in the Orléans forest in France (47°57'53" N, 2°06'45" E, 131 m a.s.l.). The station is equipped with a custom-built CO2 analyser (CARIBOU), which is based on a commercial non-dispersive, infrared (NDIR) analyser (Licor 6252), and a coupled gas chromatography (GC) system equipped with an electron capture detector (ECD) and a flame ionization detector (FID) (HP6890N, Agilent) and a reduction gas detector (PP1, Peak Performer). Air intakes, pumping and air drying system are shared between the CARIBOU and the GC systems. The ultimately achieved short-term repeatability (1 sigma, over several days) for the GC system is 0.05 ppm for CO2, 1.4 ppb for CH4, 0.25 ppb for N2O, 0.08 ppb for SF6, 0.88 ppb for CO and 3.8 for H2. The repeatability of the CARIBOU CO2 analyser is 0.06 ppm. In addition to the in situ measurements, weekly flask sampling is performed, and flask air samples are analysed at the Laboratoire des Sciences du Climat et de l'Environnement (LSCE) central laboratory for the same species as well for stable isotopes of CO2. The comparison between in situ measurements and the flask sampling showed averaged differences of 0.08 ± 1.40 ppm for CO2, 0.7 ± 7.3 ppb for CH4, 0.6 ± 0.6 ppb for N2O, 0.01 ± 0.10 ppt for SF6, 1.5± 5.3 ppb for CO and 4.8± 6.9 ppb for H2 for the years 2008–2012. At Trainou station, the mean annual increase rates from 2007 to 2011 at the 180 m sampling height were 2.2 ppm yr−1 for CO2, 4 ppb yr−1 for CH4, 0.78 ppb yr−1 for N2O and 0.29 ppt yr−1 for SF6. For all species, the 180 m sampling level showed the smallest diurnal variation. Mean diurnal gradients between the 50 m and the 180 m sampling level reached up to 30 ppm CO2, 15 ppm CH4 or 0.5 ppb N2O during nighttime whereas the mean gradients are smaller than 0.5 ppm for CO2 and 1.5 ppb for CH4 during afternoon.
We present a novel high-resolution inverse modelling system (“FLEXVAR”) based on FLEXPART-COSMO back trajectories driven by COSMO meteorological fields at 7km×7km resolution over the European COSMO-7 ...domain and the four-dimensional variational (4DVAR) data assimilation technique. FLEXVAR is coupled offline with the global inverse modelling system TM5-4DVAR to provide background mole fractions (“baselines”) consistent with the global observations assimilated in TM5-4DVAR. We have applied the FLEXVAR system for the inverse modelling of European CH4 emissions in 2018 using 24 stations with in situ measurements, complemented with data from five stations with discrete air sampling (and additional stations outside the European COSMO-7 domain used for the global TM5-4DVAR inversions). The sensitivity of the FLEXVAR inversions to different approaches to calculate the baselines, different parameterizations of the model representation error, different settings of the prior error covariance parameters, different prior inventories, and different observation data sets are investigated in detail. Furthermore, the FLEXVAR inversions are compared to inversions with the FLEXPART extended Kalman filter (“FLExKF”) system and with TM5-4DVAR inversions at 1∘×1∘ resolution over Europe. The three inverse modelling systems show overall good consistency of the major spatial patterns of the derived inversion increments and in general only relatively small differences in the derived annual total emissions of larger country regions. At the same time, the FLEXVAR inversions at 7km×7km resolution allow the observations to be better reproduced than the TM5-4DVAR simulations at 1∘×1∘. The three inverse models derive higher annual total CH4 emissions in 2018 for Germany, France, and BENELUX compared to the sum of anthropogenic emissions reported to UNFCCC and natural emissions estimated from the Global Carbon Project CH4 inventory, but the uncertainty ranges of top-down and bottom-up total emission estimates overlap for all three country regions. In contrast, the top-down estimates for the sum of emissions from the UK and Ireland agree relatively well with the total of anthropogenic and natural bottom-up inventories.
Methane emissions on the national scale in France in 2012 are inferred by assimilating continuous atmospheric mixing ratio measurements from nine stations of the European network ICOS located in ...France and surrounding countries. To assess the robustness of the fluxes deduced by our inversion system based on an objectified quantification of uncertainties, two complementary inversion set-ups are computed and analysed: (i) a regional run correcting for the spatial distribution of fluxes in France and (ii) a sectorial run correcting fluxes for activity sectors on the national scale. In addition, our results for the two set-ups are compared with fluxes produced in the framework of the inversion inter-comparison exercise of the InGOS project. The seasonal variability in fluxes is consistent between different set-ups, with maximum emissions in summer, likely due to agricultural activity. However, very high monthly posterior uncertainties (up to ≈ 65 to 74 % in the sectorial run in May and June) make it difficult to attribute maximum emissions to a specific sector. On the yearly and national scales, the two inversions range from 3835 to 4050 Gg CH4 and from 3570 to 4190 Gg CH4 for the regional and sectorial runs, respectively, consistently with the InGOS products. These estimates are 25 to 55 % higher than the total national emissions from bottom-up approaches (biogeochemical models from natural emissions, plus inventories for anthropogenic ones), consistently pointing at missing or underestimated sources in the inventories and/or in natural sources. More specifically, in the sectorial set-up, agricultural emissions are inferred as 66% larger than estimates reported to the UNFCCC. Uncertainties in the total annual national budget are 108 and 312 Gg CH4, i.e, 3 to 8 %, for the regional and sectorial runs respectively, smaller than uncertainties in available bottom-up products, proving the added value of top-down atmospheric inversions. Therefore, even though the surface network used in 2012 does not allow us to fully constrain all regions in France accurately, a regional inversion set-up makes it possible to provide estimates of French methane fluxes with an uncertainty in the total budget of less than 10 % on the yearly timescale. Additional sites deployed since 2012 would help to constrain French emissions on finer spatial and temporal scales and attributing missing emissions to specific sectors.
Over the last few decades, in situ measurements of atmospheric N2O mole fractions have been performed using gas chromatographs (GCs) equipped with electron capture detectors. This technique, however, ...becomes very challenging when trying to detect the small variations of N2O as the detectors are highly nonlinear and the GCs at remote stations require a considerable amount of maintenance by qualified technicians to maintain good short-term and long-term repeatability. With new robust optical spectrometers now available for N2O measurements, we aim to identify a robust and stable analyzer that can be integrated into atmospheric monitoring networks, such as the Integrated Carbon Observation System (ICOS). In this study, we present the most complete comparison of N2O analyzers, with seven analyzers that were developed and commercialized by five different companies. Each instrument was characterized during a time period of approximately 8 weeks. The test protocols included the characterization of the short-term and long-term repeatability, drift, temperature dependence, linearity and sensitivity to water vapor. During the test period, ambient air measurements were compared under field conditions at the Gif-sur-Yvette station. All of the analyzers showed a standard deviation better than 0.1 ppb for the 10 min averages. Some analyzers would benefit from improvements in temperature stability to reduce the instrument drift, which could then help in reducing the frequency of calibrations. For most instruments, the water vapor correction algorithms applied by companies are not sufficient for high-precision atmospheric measurements, which results in the need to dry the ambient air prior to analysis.
This study presents a new concept for estimating the pollutant emission rates of a site and its main facilities using a series of atmospheric measurements across the pollutant plumes. This concept ...combines the tracer release method, local-scale atmospheric transport modelling and a statistical atmospheric inversion approach. The conversion between the controlled emission and the measured atmospheric concentrations of the released tracer across the plume places valuable constraints on the atmospheric transport. This is used to optimise the configuration of the transport model parameters and the model uncertainty statistics in the inversion system. The emission rates of all sources are then inverted to optimise the match between the concentrations simulated with the transport model and the pollutants' measured atmospheric concentrations, accounting for the transport model uncertainty. In principle, by using atmospheric transport modelling, this concept does not strongly rely on the good colocation between the tracer and pollutant sources and can be used to monitor multiple sources within a single site, unlike the classical tracer release technique. The statistical inversion framework and the use of the tracer data for the configuration of the transport and inversion modelling systems should ensure that the transport modelling errors are correctly handled in the source estimation. The potential of this new concept is evaluated with a relatively simple practical implementation based on a Gaussian plume model and a series of inversions of controlled methane point sources using acetylene as a tracer gas. The experimental conditions are chosen so that they are suitable for the use of a Gaussian plume model to simulate the atmospheric transport. In these experiments, different configurations of methane and acetylene point source locations are tested to assess the efficiency of the method in comparison to the classic tracer release technique in coping with the distances between the different methane and acetylene sources. The results from these controlled experiments demonstrate that, when the targeted and tracer gases are not well collocated, this new approach provides a better estimate of the emission rates than the tracer release technique. As an example, the relative error between the estimated and actual emission rates is reduced from 32 % with the tracer release technique to 16 % with the combined approach in the case of a tracer located 60 m upwind of a single methane source. Further studies and more complex implementations with more advanced transport models and more advanced optimisations of their configuration will be required to generalise the applicability of the approach and strengthen its robustness.
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