Abstract. Aircraft-based measurements of methane (CH 4 ) and other air pollutants in the Athabasca Oil Sands Region (AOSR) were made during a summer intensive field campaign between 13 August and 7 September 2013 in support of the Joint Canada-Alberta Implementation Plan for Oil Sands Monitoring. Chemical signatures were used to identify CH 4 sources from tailings ponds (BTEX VOCs), open pit surface mines (NO y and rBC) and elevated plumes from bitumen upgrading facilities (SO 2 and NO y ). Emission rates of CH 4 were determined for the five primary surface mining facilities in the region using two mass-balance methods. Emission rates from source categories within each facility were estimated when plumes from the sources were spatially separable. Tailings ponds accounted for 45 % of total CH 4 emissions measured from the major surface mining facilities in the region, while emissions from operations in the open pit mines accounted for ∼ 50 %. The average open pit surface mining emission rates ranged from 1.2 to 2.8 t of CH 4 h −1 for different facilities in the AOSR. Amongst the 19 tailings ponds, Mildred Lake Settling Basin, the oldest pond in the region, was found to be responsible for the majority of tailings ponds emissions of CH 4 (> 70 %). The sum of measured emission rates of CH 4 from the five major facilities, 19.2 ± 1.1 t CH 4 h −1 , was similar to a single mass-balance determination of CH 4 from all major sources in the AOSR determined from a single flight downwind of the facilities, 23.7 ± 3.7 t CH 4 h −1 . The measured hourly CH 4 emission rate from all facilities in the AOSR is 48 ± 8 % higher than that extracted for 2013 from the Canadian Greenhouse Gas Reporting Program, a legislated facility-reported emissions inventory, converted to hourly units. The measured emissions correspond to an emissions rate of 0.17 ± 0.01 Tg CH 4 yr −1 if the emissions are assumed as temporally constant, which is an uncertain assumption. The emission rates reported here are relevant for the summer season. In the future, effort should be devoted to measurements in different seasons to further our understanding of the seasonal parameters impacting fugitive emissions of CH 4 and to allow for better estimates of annual emissions and year-to-year variability.

Abstract. Methane emissions in Canada have both anthropogenic and natural sources. Anthropogenic emissions are estimated to be 4.1 Tg a−1 from 2010–2015 in the Canadian Greenhouse Gas Inventory. Natural emissions, which are mostly due to Boreal wetlands, are the largest methane source in Canada and highly uncertain, on the order of ~20 Tg a−1 in biosphere process models. Top-down constraints on Canadian methane emissions using atmospheric observations have been limited by the sparse coverage of both surface and satellite observations. Aircraft studies over the last several years have provided snapshot emissions that have been conflicting with inventory estimates. Here we use surface data from the Environment and Climate Change Canada (ECCC) in situ network and space borne data from the Greenhouse Gases Observing Satellite (GOSAT) to determine 2010–2015 anthropogenic and natural methane emissions in Canada in a Bayesian inverse modelling framework. We use GEOS-Chem to simulate anthropogenic emissions comparable to the Canadian inventory and wetlands emissions using an ensemble of WetCHARTS v1.0 scenarios in addition to other minor natural sources. We conduct a comparative analysis of the monthly natural emissions and yearly anthropogenic emissions optimized by surface and satellite data independently. Mean 2010–2015 posterior emissions using ECCC surface data are 6.0 ± 0.4 Tg a−1 for total anthropogenic and 10.5 ± 1.9 Tg a−1 for total natural emissions, where the error intervals represent the 1-σ spread in yearly posterior results. These results agree with our posterior using GOSAT data of 6.5 ± 0.7 Tg a−1 for total anthropogenic and 11.7 ± 1.2 Tg a−1 for total natural emissions. The seasonal pattern of posterior natural emissions using either dataset shows slower to start emissions in the spring and a less intense peak in the summer compared to the mean of WetCHARTS scenarios. We combine ECCC and GOSAT data to evaluate capabilities for sectoral and provincial level inversions and identify limitations. We estimate Energy + Agriculture emissions to be 5.1 ± 1.0 Tg a−1 which is 59 % higher than the National GHG Inventory. We attribute 39 % higher anthropogenic emissions to Western Canada than the prior. Natural emissions are lower across Canada with large downscaling in the Hudson Bay Lowlands. Inversion results are verified against independent aircraft data in Saskatchewan and surface data in Quebec which show better agreement with posterior emissions. This study shows a readjustment of the Canadian methane budget is necessary to better match atmospheric observations with higher anthropogenic emissions partially offset by lower natural emissions.

Abstract. Sarnia, Ontario, experiences pollutant emissions disproportionate to its relatively small size. The small size of the city limits traditional top-down emission estimate techniques (e.g., satellite) but a low-cost solution for emission monitoring is the mobile MAX-DOAS (Multi-AXis Differential Optical Absorption Spectroscopy). Measurements were made using this technique from 21 March 2017 to 23 March 2017 along various driving routes to retrieve vertical column densities (VCDs) of NO2 and SO2 and to estimate emissions of NOx and SO2 from the Sarnia region. A novel aspect of the current study was the installation of a NOx analyzer in the vehicle to allow real time measurement and characterization of near-surface NOx∕NO2 ratios across the urban plumes, allowing improved accuracy of NOx emission estimates. Confidence in the use of near-surface-measured NOx∕NO2 ratios for estimation of NOx emissions was increased by relatively well-mixed boundary layer conditions. These conditions were indicated by similar temporal trends in NO2 VCDs and mixing ratios when measurements were sufficiently distant from the sources. Leighton ratios within transported plumes indicated peroxy radicals were likely disturbing the NO–NO2–O3 photostationary state through VOC (volatile organic compound) oxidation. The average lower-limit emission estimate of NOx from Sarnia was 1.60±0.34 t h−1 using local 10 m elevation wind-speed measurements. Our estimates were larger than the downscaled annual 2017 NPRI-reported (National Pollution Release Inventory) industrial emissions of 0.9 t NOx h−1. Our lower-limit estimate of SO2 emissions from Sarnia was 1.81±0.83 t SO2 h−1, equal within uncertainty to the 2017 NPRI downscaled value of 1.85 t SO2 h−1. Satellite-derived NO2 VCDs over Sarnia from the ozone monitoring instrument (OMI) were lower than mobile MAX-DOAS VCDs, likely due to the large pixel size relative to the city's size. The results of this study support the utility of the mobile MAX-DOAS method for estimating NOx and SO2 emissions in relatively small, highly industrialized regions, especially when supplemented with mobile NOx measurements.

Abstract. Aircraft-based measurements of methane (CH4) and other air pollutants in the Athabasca Oil 10

Abstract. Vertical profiles of aerosols, NO2, and SO2 were retrieved from Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements at a field site in northern Alberta, Canada, during August and September 2013. The site is approximately 16 km north of two mining operations that are major sources of industrial pollution in the Athabasca oil sands region. Pollution conditions during the study ranged from atmospheric background conditions to heavily polluted with elevated plumes, according to the meteorology. This study aimed to evaluate the performance of the aerosol and trace gas retrievals through comparison with data from a suite of other instruments. Comparisons of aerosol optical depths (AODs) from MAX-DOAS aerosol retrievals, lidar vertical profiles of aerosol extinction, and the AERONET sun photometer indicate good performance by the MAX-DOAS retrievals. These comparisons and modelling of the lidar S ratio highlight the need for accurate knowledge of the temporal variation in the S ratio when comparing MAX-DOAS and lidar data. Comparisons of MAX-DOAS NO2 and SO2 retrievals to Pandora spectral sun photometer vertical column densities (VCDs) and active DOAS mixing ratios indicate good performance of the retrievals, except when vertical profiles of pollutants within the boundary layer varied rapidly, temporally, and spatially. Near-surface retrievals tended to overestimate active DOAS mixing ratios. The MAX-DOAS observed elevated pollution plumes not observed by the active DOAS, highlighting one of the instrument's main advantages. Aircraft measurements of SO2 were used to validate retrieved vertical profiles of SO2. Advantages of the MAX-DOAS instrument include increasing sensitivity towards the surface and the ability to simultaneously retrieve vertical profiles of aerosols and trace gases without requiring additional parameters, such as the S ratio. This complex dataset provided a rare opportunity to evaluate the performance of the MAX-DOAS retrievals under varying atmospheric conditions.