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This research quantifies current sources of non-exhaust particulate matter traffic emissions in London using simultaneous, highly time-resolved, atmospheric particulate matter mass and chemical composition measurements. The measurement campaign ran at Marylebone Road (roadside) and Honor Oak Park (background) urban monitoring sites over a 12-month period between 1 September 2019 and 31 August 2020. The measurement data were used to determine the traffic increment (roadside–background) and covered a range of meteorological conditions, seasons, and driving styles, as well as the influence of the COVID-19 “lockdown” on non-exhaust concentrations. Non-exhaust particulate matter (PM)10 concentrations were calculated using chemical tracer scaling factors for brake wear (barium), tyre wear (zinc), and resuspension (silicon) and as average vehicle fleet non-exhaust emission factors, using a CO2 “dilution approach”. The effect of lockdown, which saw a 32% reduction in traffic volume and a 15% increase in average speed on Marylebone Road, resulted in lower PM10 and PM2.5 traffic increments and brake wear concentrations but similar tyre and resuspension concentrations, confirming that factors that determine non-exhaust emissions are complex. Brake wear was found to be the highest average non-exhaust emission source. In addition, results indicate that non-exhaust emission factors were dependent upon speed and road surface wetness conditions. Further statistical analysis incorporating a wider variability in vehicle mix, speeds, and meteorological conditions, as well as advanced source apportionment of the PM measurement data, were undertaken to enhance our understanding of these important vehicle sources.

Mobile, near-source measurements are broadly used for determining δ13CH4 of individual methane (CH4) emissions sources. To answer the need for robust and comparable measurement methods, we aim to define the best practices to determine isotopic signatures of CH4 sources from atmospheric measurements, considering instrument accuracy and precision. Using the Keeling and Miller-Tans methods, we verify the impact of linear fitting methods, averaging approaches, and for the Miller-Tans method, different background composition. Measurement techniques include Isotope Ratio Mass Spectrometry (IRMS) and Cavity Ring Down Spectroscopy (CRDS). The use of the active AirCore system for sampling, coupled to CRDS for measurement, is examined. Due to their higher precision and accuracy, the chosen data processing strategy does not significantly influence IRMS results. Comparatively lower-precision CRDS measurements are more sensitive to methodological choices. Fitting methods with forced symmetry like Major Axis or Bivariate Correlated Errors and Intrinsic Scatter (BCES) with orthogonal sub-method introduce significant bias in the determined δ13CH4 signatures using measurements from the lower-precision CRDS. The most reliable results are obtained for non-averaged data using fitting methods, which include uncertainties of x- and y-axis values, like York fitting or BCES (Y|X) sub-method, where x is treated as an independent variable. The Ordinary Least Squares method provides sufficiently robust results and can be used to determine δ13CH4 in near-source conditions. The present recommendations are aimed at laboratories measuring δ13CH4 source signatures to encourage consistency in the required methods for data analysis.

Recent climate change mitigation strategies rely on the reduction of methane (CH4) emissions. Carbon and hydrogen isotope ratio (δ13CCH4 and δ2HCH4) measurements can be used to distinguish sources and thus to understand the CH4 budget better. The CH4 emission estimates by models are sensitive to the isotopic signatures assigned to each source category, so it is important to provide representative estimates of the different CH4 source isotopic signatures worldwide. We present new measurements of isotope signatures of various, mainly anthropogenic, CH4 sources in Europe, which represent a substantial contribution to the global dataset of source isotopic measurements from the literature, especially for δ2HCH4. They improve the definition of δ13CCH4 from waste sources, and demonstrate the use of δ2HCH4 for fossil fuel source attribution. We combined our new measurements with the last published database of CH4 isotopic signatures and with additional literature, and present a new global database. We found that microbial sources are generally well characterised. The large variability in fossil fuel isotopic compositions requires particular care in the choice of weighting criteria for the calculation of a representative global value. The global dataset could be further improved by measurements from African, South American, and Asian countries, and more measurements from pyrogenic sources. We improved the source characterisation of CH4 emissions using stable isotopes and associated uncertainty, to be used in top-down studies. We emphasise that an appropriate use of the database requires the analysis of specific parameters in relation to source type and the region of interest. The final version of the European CH4 isotope database coupled with a global inventory of fossil and non-fossil δ13CCH4 and δ2HCH4 source signature measurements is available at https://doi.org/10.24416/UU01-YP43IN (Menoud et al., 2022a).

This study presents the first gaseous formic acid (HC(O)OH) concentration measurements collected over the Fenno-Scandinavian wetlands (67.9–68.0° N, 22.1–27.8° E) as part of the MAMM (Methane and other greenhouse gases in the Arctic-Measurements, process studies and Modelling) aircraft campaigns conducted in August and September 2013. A boundary layer box model approach has been used to calculate a regionally representative (~240 km2) surface flux for HC(O)OH of 0.0098 (±0.0057) mg[HCOOH]·m−2·h−1. A surface-type classification map was used to estimate proportional source contributions to the observed HC(O)OH flux over the measurement region. The removal of expected source contributions (using available literature parameterisations) from the calculated surface flux identified that 75% remained unaccounted for. This may suggest that HC(O)OH emission from wetland within the Fenno-Scandinavian region could contribute up to 29 times higher per unit area than previous theoretical HC(O)OH globally-averaged wetland estimates, highlighting a need for further constrained wetland studies of HC(O)OH emission to better understand its potentially significant impact on the Arctic HC(O)OH budget and consequent impacts on oxidative capacity.

Atmospheric methane (CH4) concentrations have more than doubled since the beginning of the industrial age, making CH4 the second most important anthropogenic greenhouse gas after carbon dioxide (CO2). The oil and gas sector represents one of the major anthropogenic CH4 emitters as it is estimated to account for 22 % of global anthropogenic CH4 emissions. An airborne field campaign was conducted in April–May 2019 to study CH4 emissions from offshore gas facilities in the southern North Sea with the aim of deriving emission estimates using a top-down (measurement-led) approach. We present CH4 fluxes for six UK and five Dutch offshore platforms or platform complexes using the well-established mass balance flux method. We identify specific gas production emissions and emission processes (venting and fugitive or flaring and combustion) using observations of co-emitted ethane (C2H6) and CO2. We compare our top-down estimated fluxes with a ship-based top-down study in the Dutch sector and with bottom-up estimates from a globally gridded annual inventory, UK national annual point-source inventories, and operator-based reporting for individual Dutch facilities. In this study, we find that all the inventories, except for the operator-based facility-level reporting, underestimate measured emissions, with the largest discrepancy observed with the globally gridded inventory. Individual facility reporting, as available for Dutch sites for the specific survey date, shows better agreement with our measurement-based estimates. For all the sampled Dutch installations together, we find that our estimated flux of (122.9 ± 36.8) kg h−1 deviates by a factor of 0.64 (0.33–12) from reported values (192.8 kg h−1). Comparisons with aircraft observations in two other offshore regions (the Norwegian Sea and the Gulf of Mexico) show that measured, absolute facility-level emission rates agree with the general distribution found in other offshore basins despite different production types (oil, gas) and gas production rates, which vary by 2 orders of magnitude. Therefore, mitigation is warranted equally across geographies.

Atmospheric methane (CH4) is the second-most-important anthropogenic greenhouse gas and has a 20-year global warming potential 82 times greater than carbon dioxide (CO2). Anthropogenic sources account for ∼ 60 % of global CH4 emissions, of which 20 % come from oil and gas exploration, production and distribution. High-resolution satellite-based imaging spectrometers are becoming important tools for detecting and monitoring CH4 point source emissions, aiding mitigation. However, validation of these satellite measurements, such as those from the commercial GHGSat satellite constellation, has so far not been documented for active leaks. Here we present the monitoring and quantification, by GHGSat's satellites, of the CH4 emissions from an active gas leak from a downstream natural gas distribution pipeline near Cheltenham, UK, in the spring and summer of 2023 and provide the first validation of the satellite-derived emission estimates using surface-based mobile greenhouse gas surveys. We also use a Lagrangian transport model, the UK Met Office's Numerical Atmospheric-dispersion Modelling Environment (NAME), to estimate the flux from both satellite- and ground-based observation methods and assess the leak's contribution to observed concentrations at a local tall tower site (30 km away). We find GHGSat's emission estimates to be in broad agreement with those made from the in situ measurements. During the study period (March–June 2023) GHGSat's emission estimates are 236–1357 kg CH4 h−1, whereas the mobile surface measurements are 634–846 kg CH4 h−1. The large variability is likely down to variations in flow through the pipe and engineering works across the 11-week period. Modelled flux estimates in NAME are 181–1243 kg CH4 h−1, which are lower than the satellite- and mobile-survey-derived fluxes but are within the uncertainty. After detecting the leak in March 2023, the local utility company was contacted, and the leak was fixed by mid-June 2023. Our results demonstrate that GHGSat's observations can produce flux estimates that broadly agree with surface-based mobile measurements. Validating the accuracy of the information provided by targeted, high-resolution satellite monitoring shows how it can play an important role in identifying emission sources, including unplanned fugitive releases that are inherently challenging to identify, track, and estimate their impact and duration. Rapid, widespread access to such data to inform local action to address fugitive emission sources across the oil and gas supply chain could play a significant role in reducing anthropogenic contributions to climate change.

Currently, the atmospheric methane burden is rising rapidly, but the extent to which shifts in coal production contribute to this rise is not known. Coalbed methane emissions into the atmosphere are poorly characterised, and this study provides representative δ13CCH4 signatures of methane emissions from specific coalfields. Integrated methane emissions from both underground and opencast coal mines in the UK, Australia and Poland were sampled and isotopically characterised. Progression in coal rank and secondary biogenic production of methane due to incursion of water are suggested as the processes affecting the isotopic composition of coal-derived methane. An averaged value of −65 ‰ has been assigned to bituminous coal exploited in open cast mines and of −55 ‰ in deep mines, whereas values of −40 and −30 ‰ can be allocated to anthracite opencast and deep mines respectively. However, the isotopic signatures that are included in global atmospheric modelling of coal emissions should be region- or nation-specific, as greater detail is needed, given the wide global variation in coal type.

The Roc Blanc Pb-Zn-Ag ± Au vein system in the Variscan Central Jebilet massif, Morocco, is confined within the contact metamorphic aureole of S- and I-type calc-alkaline granitic stocks (327 ± 4 to 295 ± 15 Ma) along the Marrakech Shear Zone. Host rocks consist of a succession of greenschist- to amphibolite-facies metasedimentary and metavolcaniclastic rocks of Carboniferous age. The ore mineralogy is predominantly base metal and Ag-bearing sulfides and sulfosalts, intergrown with quartz and carbonates. Late-stage gold mineralization is commonly present as electrum in intimate association with all major generations of sulfide and sulfosalt minerals. Ore-related hydrothermal alteration includes silicification, sericitization, chloritization, and carbonatization. Chlorite and arsenopyrite geothermometry suggest mean temperatures of 364 and 350 °C; respectively. Calculated δ18Ofluid values of 15 to 18‰ are consistent with metamorphic fluid sources, by which the mineralizing fluids were produced during the emplacement of granitic intrusions and subsequent devolatilization of graphitic black shale and interlayered carbonate beds. Lead and strontium isotope data constrain the source of the ore-forming components (i.e., metals and sulfur) to the enclosing host rocks. A decrease in temperature during fluid ascent and subsequent alteration-associated fluid-rock interaction resulted in the deposition of the Pb-Zn-Ag ± Au mineralization in a post-collisional extensional setting.