Intercomparison of detection and quantification methods for methane emissions from the natural gas distribution network in Hamburg, Germany

In August and September 2020, three different measurement methods for quantifying methane (CH4) emissions from leaks in urban gas distribution networks were applied and compared in Hamburg, Germany: the “mobile”, “tracer release”, and “suction” methods. The mobile and tracer release methods determine emission rates to the atmosphere from measurements of CH4 mole fractions in the ambient air, and the tracer release method also includes measurement of a gaseous tracer. The suction method determines emission rates by pumping air out of the ground using soil probes that are placed above the suspected leak location. The quantitative intercomparison of the emission rates from the three methods at a small number of locations is challenging because of limitations of the different methods at different types of leak locations. The mobile method was designed to rapidly quantify the average or total emission rate of many gas leaks in a city, but it yields a large emission rate uncertainty for individual leak locations. Emission rates determined for individual leak locations with the tracer release technique are more precise because the simultaneous measurement of the tracer released at a known rate at the emission source eliminates many of the uncertainties encountered with the mobile method. Nevertheless, care must be taken to properly collocate the tracer release and the leak emission points to avoid biases in emission rate estimates. The suction method could not be completed or applied at locations with widespread subsurface CH4 accumulation or due to safety measures. While the number of gas leak locations in this study is small, we observe a correlation between leak emission rate and subsurface accumulation. Wide accumulation places leaks into a safety category that requires immediate repair so that the suction method cannot be applied to these larger leaks in routine operation. This introduces a sampling bias for the suction method in this study towards the low-emission leaks, which do not require immediate repair measures. Given that this study is based on random sampling, such a sampling bias may also exist for the suction method outside of this study. While an investigation of the causal relationship between safety category and leak size is beyond the scope of this study, on average higher emission rates were observed from all three measurement-based quantification methods for leaks with higher safety priority compared to the leaks with lower safety concern. The leak locations where the suction method could not be applied were the biggest emitters, as confirmed by the emission rate quantifications using mobile and tracer methods and an engineering method based on the leak's diameter, pipeline overpressure, and depth at which the pipeline is buried. The corresponding sampling bias for the suction technique led to a low bias in derived emission rates in this study. It is important that future studies using the suction method account for any leaks not quantifiable with this method in order to avoid biases, especially when used to inform emission inventories.</p

Source apportionment of methane emissions from the Upper Silesian Coal Basin using isotopic signatures

Anthropogenic emissions are the primary source of the increase in atmospheric methane (CH4) levels. However, estimates of anthropogenic CH4 emissions still show large uncertainties at global and regional scales. Differences in CH4 isotopic source signatures δ13C and δ2H can help to constrain different source contributions (e.g., fossil, waste, agriculture). The Upper Silesian Coal Basin (USCB) represents one of the largest European CH4 emission regions, with more than 500 Gg CH4 yr−1 released from more than 50 coal mine ventilation shafts, landfills, and wastewater treatment plants. During the CoMet (Carbon Dioxide and Methane Mission) campaign in June 2018 methane observations were conducted from a variety of platforms including aircraft and cars to quantify these emissions. Besides the continuous sampling of atmospheric methane concentration, numerous air samples were taken from inside and around the ventilation shafts (1–2 km distance) and aboard the High Altitude and Long Range Research Aircraft (HALO) and DLR Cessna Caravan aircraft, and they were analyzed in the laboratory for the isotopic composition of CH4. The airborne samples downwind of the USCB contained methane from the entire region and thus enabled determining the mean signature of the USCB accurately. This mean isotopic signature of methane emissions was -50.9±0.7 ‰ for δ13C and -226±9 ‰ for δ2H. This is in the range of previous USCB studies based on samples taken within the mines for δ13C but more depleted in δ2H than reported before. Signatures of methane enhancements sampled upwind of the mines and in the free troposphere clearly showed the influence of biogenic sources. We determined the source signatures of individual coal mine ventilation shafts using ground-based samples. These signatures displayed a considerable range between different mines and also varied for individual shafts from day to day. Different layers of the USCB coal contain thermogenic methane, isotopically similar to natural gas, and methane formed through biogenic carbonate reduction. The signatures vary depending on what layer of coal is mined at the time of sampling. Mean shaft signatures range from −60 ‰ to −42 ‰ for δ13C and from −200 ‰ to −160 ‰ for δ2H. A gradient in the signatures of subregions of the USCB is reflected both in the aircraft data and in the ground samples, with emissions from the southwest being most depleted in δ2H and emissions from the south being most depleted in δ13C, which is probably associated with the structural and lithostratigraphic history of the USCB and generation and migration processes of methane in the coal. The average signature of -49.8±5.7 ‰ in δ13C and -184±32 ‰ in δ2H from the ventilation shafts clearly differs from the USCB regional signature in δ2H. This makes a source attribution using δ2H signatures possible, which would not be possible with only the δ13C isotopic signatures. We assume that the USCB plume mainly contains fossil coal mine methane and biogenic methane from waste treatment, because the USCB is a highly industrialized region with few other possible methane sources. Assuming a biogenic methane signature between and −320 ‰ and −280 ‰ for δ2H, the biogenic methane emissions from the USCB account for 15 %–50 % of total emissions. The uncertainty range shows the need of comprehensive and extensive sampling from all possible source sectors for source apportionment. The share of anthropogenic–biogenic emissions of 0.4 %–14 % from this densely populated industrial region is underestimated in commonly used emission inventories. Generally, this study demonstrates the importance of δ2H-CH4 observations for methane source apportionment in regions with a mix of thermogenic and biogenic sources and, especially in our case, where the δ13C signature of the coal mine gas has a large variability.</p

Street-level methane emissions of Bucharest, Romania and the dominance of urban wastewater

Atmospheric methane (CH4) continues to increase, but there are multiple anthropogenic source categories that can be targeted for cost-effective emissions reduction. Cities emit CH4 to the atmosphere from a mixture of anthropogenic CH4 sources, which include, but are not limited to, fugitive emissions from natural gas distribution systems, wastewater treatment facilities, waste-and rainwater networks, and landfills. Therefore, to target mitigation measures, it is important to locate and quantify local urban emissions to prioritize mitigation opportunities in large cities. Using mobile measurement techniques, we located street-level CH4 leak indications, measured flux rates, and determined potential source origins (using carbon and hydrogen stable isotopic composition along with ethane: CH4 ratios) of CH4 in Bucharest, Romania. We found 969 confirmed CH4 leak indication locations, where the maximum mole fraction elevation (above background) was 38.3 ppm (mean = 0.9 ppm ± 0.1 ppm s.e.; n = 2482). Individual leak indicator fluxes, derived using a previously established empirical relation, ranged up to around 15 metric tons CH4 yr-1 (mean = 0.8 metric tons yr-1 ± 0.05, s.e.; n = 969). The total estimated city emission rate is 1832 tons CH4 yr-1 (min = 1577 t yr-1 and max = 2113 t yr-1). More than half (58%–63%) of the CH4 elevations were attributed to biogenic wastewater, mostly from venting storm grates and manholes connecting to sewer pipelines. Hydrogen isotopic composition of CH4 and ethane:methane ratios were the most useful tracers of CH4 sources, due to similarities in carbon isotope ratios between wastewater gas and natural gas. The annual city-wide CH4 emission estimate of Bucharest exceeded emissions of Hamburg, Germany by 76% and Paris, France by 90%

Street-level methane emissions of Bucharest, Romania and the dominance of urban wastewater.

Atmospheric methane (CH4) continues to increase, but there are multiple anthropogenic source categories that can be targeted for cost-effective emissions reduction. Cities emit CH4 to the atmosphere from a mixture of anthropogenic CH4 sources, which include, but are not limited to, fugitive emissions from natural gas distribution systems, wastewater treatment facilities, waste-and rainwater networks, and landfills. Therefore, to target mitigation measures, it is important to locate and quantify local urban emissions to prioritize mitigation opportunities in large cities. Using mobile measurement techniques, we located street-level CH4 leak indications, measured flux rates, and determined potential source origins (using carbon and hydrogen stable isotopic composition along with ethane: CH4 ratios) of CH4 in Bucharest, Romania. We found 969 confirmed CH4 leak indication locations, where the maximum mole fraction elevation (above background) was 38.3 ppm (mean = 0.9 ppm ± 0.1 ppm s.e.; n = 2482). Individual leak indicator fluxes, derived using a previously established empirical relation, ranged up to around 15 metric tons CH4 yr-1 (mean = 0.8 metric tons yr-1 ± 0.05, s.e.; n = 969). The total estimated city emission rate is 1832 tons CH4 yr-1 (min = 1577 t yr-1 and max = 2113 t yr-1). More than half (58%–63%) of the CH4 elevations were attributed to biogenic wastewater, mostly from venting storm grates and manholes connecting to sewer pipelines. Hydrogen isotopic composition of CH4 and ethane:methane ratios were the most useful tracers of CH4 sources, due to similarities in carbon isotope ratios between wastewater gas and natural gas. The annual city-wide CH4 emission estimate of Bucharest exceeded emissions of Hamburg, Germany by 76% and Paris, France by 90%

Street-level methane emissions of Bucharest, Romania and the dominance of urban wastewater.

Atmospheric methane (CH4) continues to increase, but there are multiple anthropogenic source categories that can be targeted for cost-effective emissions reduction. Cities emit CH4 to the atmosphere from a mixture of anthropogenic CH4 sources, which include, but are not limited to, fugitive emissions from natural gas distribution systems, wastewater treatment facilities, waste-and rainwater networks, and landfills. Therefore, to target mitigation measures, it is important to locate and quantify local urban emissions to prioritize mitigation opportunities in large cities. Using mobile measurement techniques, we located street-level CH4 leak indications, measured flux rates, and determined potential source origins (using carbon and hydrogen stable isotopic composition along with ethane: CH4 ratios) of CH4 in Bucharest, Romania. We found 969 confirmed CH4 leak indication locations, where the maximum mole fraction elevation (above background) was 38.3 ppm (mean = 0.9 ppm ± 0.1 ppm s.e.; n = 2482). Individual leak indicator fluxes, derived using a previously established empirical relation, ranged up to around 15 metric tons CH4 yr-1 (mean = 0.8 metric tons yr-1 ± 0.05, s.e.; n = 969). The total estimated city emission rate is 1832 tons CH4 yr-1 (min = 1577 t yr-1 and max = 2113 t yr-1). More than half (58%–63%) of the CH4 elevations were attributed to biogenic wastewater, mostly from venting storm grates and manholes connecting to sewer pipelines. Hydrogen isotopic composition of CH4 and ethane:methane ratios were the most useful tracers of CH4 sources, due to similarities in carbon isotope ratios between wastewater gas and natural gas. The annual city-wide CH4 emission estimate of Bucharest exceeded emissions of Hamburg, Germany by 76% and Paris, France by 90%

Street-level methane emissions of Bucharest, Romania and the dominance of urban wastewater.

Atmospheric methane (CH4) continues to increase, but there are multiple anthropogenic source categories that can be targeted for cost-effective emissions reduction. Cities emit CH4 to the atmosphere from a mixture of anthropogenic CH4 sources, which include, but are not limited to, fugitive emissions from natural gas distribution systems, wastewater treatment facilities, waste-and rainwater networks, and landfills. Therefore, to target mitigation measures, it is important to locate and quantify local urban emissions to prioritize mitigation opportunities in large cities. Using mobile measurement techniques, we located street-level CH4 leak indications, measured flux rates, and determined potential source origins (using carbon and hydrogen stable isotopic composition along with ethane: CH4 ratios) of CH4 in Bucharest, Romania. We found 969 confirmed CH4 leak indication locations, where the maximum mole fraction elevation (above background) was 38.3 ppm (mean = 0.9 ppm ± 0.1 ppm s.e.; n = 2482). Individual leak indicator fluxes, derived using a previously established empirical relation, ranged up to around 15 metric tons CH4 yr-1 (mean = 0.8 metric tons yr-1 ± 0.05, s.e.; n = 969). The total estimated city emission rate is 1832 tons CH4 yr-1 (min = 1577 t yr-1 and max = 2113 t yr-1). More than half (58%–63%) of the CH4 elevations were attributed to biogenic wastewater, mostly from venting storm grates and manholes connecting to sewer pipelines. Hydrogen isotopic composition of CH4 and ethane:methane ratios were the most useful tracers of CH4 sources, due to similarities in carbon isotope ratios between wastewater gas and natural gas. The annual city-wide CH4 emission estimate of Bucharest exceeded emissions of Hamburg, Germany by 76% and Paris, France by 90%

Street-level methane emissions of Bucharest, Romania and the dominance of urban wastewater.

Atmospheric methane (CH4) continues to increase, but there are multiple anthropogenic source categories that can be targeted for cost-effective emissions reduction. Cities emit CH4 to the atmosphere from a mixture of anthropogenic CH4 sources, which include, but are not limited to, fugitive emissions from natural gas distribution systems, wastewater treatment facilities, waste-and rainwater networks, and landfills. Therefore, to target mitigation measures, it is important to locate and quantify local urban emissions to prioritize mitigation opportunities in large cities. Using mobile measurement techniques, we located street-level CH4 leak indications, measured flux rates, and determined potential source origins (using carbon and hydrogen stable isotopic composition along with ethane: CH4 ratios) of CH4 in Bucharest, Romania. We found 969 confirmed CH4 leak indication locations, where the maximum mole fraction elevation (above background) was 38.3 ppm (mean = 0.9 ppm ± 0.1 ppm s.e.; n = 2482). Individual leak indicator fluxes, derived using a previously established empirical relation, ranged up to around 15 metric tons CH4 yr-1 (mean = 0.8 metric tons yr-1 ± 0.05, s.e.; n = 969). The total estimated city emission rate is 1832 tons CH4 yr-1 (min = 1577 t yr-1 and max = 2113 t yr-1). More than half (58%–63%) of the CH4 elevations were attributed to biogenic wastewater, mostly from venting storm grates and manholes connecting to sewer pipelines. Hydrogen isotopic composition of CH4 and ethane:methane ratios were the most useful tracers of CH4 sources, due to similarities in carbon isotope ratios between wastewater gas and natural gas. The annual city-wide CH4 emission estimate of Bucharest exceeded emissions of Hamburg, Germany by 76% and Paris, France by 90%