Ethane measurement by Picarro CRDS G2201-i in laboratory and field conditions: potential and limitations

Atmospheric ethane can be used as a tracer to distinguish methane sources, both at the local and global scale. Currently, ethane can be measured in the field using flasks or in situ analyzers. In our study, we characterized the CRDS Picarro G2201-i instrument, originally designed to measure isotopic CH4 and CO2, for measurements of ethane-to-methane ratio in mobile-measurement scenarios, near sources and under field conditions. We evaluated the limitations and potential of using the CRDS G2201-i to measure the ethane-to-methane ratio, thus extending the instrument application to simultaneously measure two methane source proxies in the field: carbon isotopic ratio and the ethane-to-methane ratio. First, laboratory tests were run to characterize the instrument in stationary conditions. Subsequently, the instrument performance was tested in field conditions as part of a controlled release experiment. Finally, the instrument was tested during mobile measurements focused on gas compressor stations. The results from the field were afterwards compared with the results obtained from instruments specifically designed for ethane measurements. Our study shows the potential of using the CRDS G2201-i instrument in a mobile configuration to determine the ethane-to-methane ratio in methane plumes under measurement conditions with an ethane uncertainty of 50 ppb. Assuming typical ethane-to-methane ratios ranging between 0 and 0.1 ppb ppb(-1), we conclude that the instrument can accurately estimate the "true" ethane-to-methane ratio within 1 sigma uncertainty when CH4 enhancements are at least 1 ppm, as can be found in the vicinity of strongly emitting sites such as natural gas compressor stations and roadside gas pipeline leaks

Detection and long-term quantification of methane emissions from an active landfill

Landfills are a significant source of fugitive methane (CH4) emissions, which should be precisely and regularly monitored to reduce and mitigate net greenhouse gas emissions. In this study, we present long-term, in situ, near-surface, mobile atmospheric CH4 mole fraction measurements (complemented by meteorological measurements from a fixed station) from 21 campaigns that cover approximately 4 years from September 2016 to December 2020. These campaigns were utilized to regularly quantify the total CH4 emissions from an active landfill in France. We use a simple atmospheric inversion approach based on a Gaussian plume dispersion model to derive CH4 emissions. Together with the measurements near the soil surface, mainly dedicated to the identification of sources within the landfill, measurements of CH4 made on the landfill perimeter (near-field) helped us to identify the main emission areas and to provide some qualitative insights about the rank of their contributions to total emissions from the landfill. The two main area sources correspond, respectively, to a covered waste sector with infrastructure with sporadic leakages (such as wells, tanks, pipes, etc.) and to the last active sector receiving waste during most of the measurement campaigns. However, we hardly managed to extract a signal representative of the overall landfill emissions from the near-field measurements, which limited our ability to derive robust estimates of the emissions when assimilating them in the atmospheric inversions. The analysis shows that the inversions based on the measurements from a remote road further away from the landfill (far-field) yielded reliable estimates of the total emissions but provided less information on the spatial variability of emissions within the landfill. This demonstrates the complementarity between the near- and far-field measurements. According to these inversions, the total CH4 emissions have a large temporal variability and range from ∼ 0.4 to ∼ 7 t CH4 d−1, with an average value of ∼ 2.1 t CH4 d−1. We find a weak negative correlation between these estimates of the CH4 emissions and atmospheric pressure for the active landfill. However, this weak emission–pressure relationship is based on a relatively small sample of reliable emission estimates with large sampling gaps. More frequent robust estimations are required to better understand this relationship for an active landfill.</p

The fingerprint of the summer 2018 drought in Europe on ground-based atmospheric CO2 measurements

During the summer of 2018, a widespread drought developed over Northern and Central Europe. The increase in temperature and the reduction of soil moisture have influenced carbon dioxide (CO2) exchange between the atmosphere and terrestrial ecosystems in various ways, such as a reduction of photosynthesis, changes in ecosystem respiration, or allowing more frequent fires. In this study, we characterize the resulting perturbation of the atmospheric CO2 seasonal cycles. 2018 has a good coverage of European regions affected by drought, allowing the investigation of how ecosystem flux anomalies impacted spatial CO2 gradients between stations. This density of stations is unprecedented compared to previous drought events in 2003 and 2015, particularly thanks to the deployment of the Integrated Carbon Observation System (ICOS) network of atmospheric greenhouse gas monitoring stations in recent years. Seasonal CO2 cycles from 48 European stations were available for 2017 and 2018.The UK sites were funded by the UK Department of Business, Energy and Industrial Strategy (formerly the Department of Energy and Climate Change) through contracts TRN1028/06/2015 and TRN1537/06/2018. The stations at the ClimaDat Network in Spain have received funding from the ‘la Caixa’ Foundation, under agreement 2010-002624

Methane emission estimates using chamber and tracer release experiments for a municipal waste water treatment plant

International audienceThis 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 CH 4 emissions of the WWTP, we confirm that the open basins are not a major source of CH 4 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

Estimation of waste water treatment plant methane emissions: methodology and results from a short campaign

International audienceThis paper describes different methods to estimate methane emissions at different scales. These methods are applied to a waste water treatment plant (WWTP) located in Valence, France. We show that Fourier Transform Infrared (FTIR) measurements as well as Cavity Ring Down Spectroscopy (CRDS) can be used to measure emissions from the process to the regional scale. To estimate the total emissions, we investigate a tracer release method (using C2H2) and the Radon tracer method (using 222Rn). For process-scale emissions, both tracer release and chamber techniques were used. We show that the tracer release method is suitable to quantify facility- and some process-scale emissions, while the Radon tracer method encompasses not only the treatment station but also a large area around. Thus the Radon tracer method is more representative of the regional emissions around the city. Uncertainties for each method are described. Applying the methods to CH4 emissions, we find that the main source of emissions of the plant was not identified with certainty during this short campaign, although the primary source of emissions is likely to be from solid sludge. Overall, the waste water treatment plant represents a small part (3%) of the methane emissions of the city of Valence and its surroundings,which is in agreement with the national inventories

Comprehensive laboratory and field testing of cavity ring-down spectroscopy analyzers measuring H₂O, CO₂, CH₄ and CO

International audienceTo 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

How a European network may help with estimating methane emissions on the French national scale

International audienceMethane emissions on the national scale in France in 2012 are inferred by assimilating continuous atmospheric mixing ratio measurements from nine stations of the Euro-pean 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 setups 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 setups 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 setups , 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 CH 4 and from 3570 to 4190 Gg CH 4 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 setup , 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 CH 4 , 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 setup 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

Long-lived atmospheric trace gases measurements in flask samples from three stations in India

International audienceWith 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 CO 2 , CH 4 , N 2 O, SF 6 , CO, and H 2 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

Simulating CH 4 and CO 2 over South and East Asia using the zoomed chemistry transport model LMDz-INCA

International audienceThe increasing availability of atmospheric measurements of greenhouse gases (GHGs) from surface stations can improve the retrieval of their fluxes at higher spatial and temporal resolutions by inversions, provided that transport models are able to properly represent the variability of concentrations observed at different stations. South and East Asia (SEA; the study area in this paper including the regions of South Asia and East Asia) is a region with large and very uncertain emissions of carbon dioxide (CO 2) and methane (CH 4), the most potent anthropogenic GHGs. Monitoring networks have expanded greatly during the past decade in this region, which should contribute to reducing uncertainties in estimates of regional GHG budgets. In this study, we simulate concentrations of CH 4 and CO 2 using zoomed versions (abbreviated as "ZAs") of the global chemistry transport model LMDz-INCA, which have fine horizontal resolutions of ∼ 0.66 • in longitude and ∼ 0.51 • in latitude over SEA and coarser resolutions elsewhere. The concentrations of CH 4 and CO 2 simulated from ZAs are compared to those from the same model but with standard model grids of 2.50 • in longitude and 1.27 • in latitude (abbreviated as "STs"), both prescribed with the same natural and anthropogenic fluxes. Model performance is evaluated for each model version at multi-annual, seasonal, synoptic and diurnal scales, against a unique observation dataset including 39 global and regional stations over SEA and around the world. Results show that ZAs improve the overall representation of CH 4 annual gradients between stations in SEA, with reduction of RMSE by 16-20 % compared to STs. The model improvement mainly results from reduction in representation error at finer horizontal resolutions and thus better characterization of the CH 4 concentration gradients related to scattered distributed emission sources. However, the performance of ZAs at a specific station as compared to STs is more sensitive to errors in meteorological forcings and surface fluxes, especially when short-term variabilities or stations close to source regions are examined. This highlights the importance of accurate a priori CH 4 surface fluxes in high-resolution transport modeling and inverse studies, particularly regarding locations and magnitudes of emission hotspots. Model perfor-Published by Copernicus Publications on behalf of the European Geosciences Union. 9476 X. Lin et al.: Chemistry transport model LMDz-INCA mance for CO 2 suggests that the CO 2 surface fluxes have not been prescribed with sufficient accuracy and resolution, especially the spatiotemporally varying carbon exchange between land surface and atmosphere. In addition, the representation of the CH 4 and CO 2 short-term variabilities is also limited by model's ability to simulate boundary layer mixing and mesoscale transport in complex terrains, emphasizing the need to improve sub-grid physical parameterizations in addition to refinement of model resolutions