Assessing the role of anthropogenic and biogenic sources on PM1 over southern West Africa using aircraft measurements

As part of the Dynamics-Aerosol-Chemistry-Cloud Interactions in West Africa (DACCIWA) project, an airborne campaign was designed to measure a large range of atmospheric constituents, focusing on the effect of anthropogenic emissions on regional climate. The presented study details results of the French ATR42 research aircraft, which aimed to characterize gas-phase, aerosol and cloud properties in the region during the field campaign carried out in June/July 2016 in combination with the German Falcon 20 and the British Twin Otter aircraft. The aircraft flight paths covered large areas of Benin, Togo, Ghana and Côte d'Ivoire, focusing on emissions from large urban conurbations such as Abidjan, Accra and Lomé, as well as remote continental areas and the Gulf of Guinea. This paper focuses on aerosol particle measurements within the boundary layer ( 15 nm) of 735 cm-3 stp. Regarding submicron aerosol composition (considering non-refractory species and black carbon, BC), organic aerosol (OA) is the most abundant species contributing 53 %, followed by SO4 (27 %), NH4 (11 %), BC (6 %), NO3 (2 %) and minor contribution of Cl (< 0.5 %). Average background PM1 in the region was 5.9 μg m-3 stp. During measurements of urban pollution plumes, mainly focusing on the outflow of Abidjan, Accra and Lomé, pollutants are significantly enhanced (e.g. average concentration of CO of 176 ppb, and aerosol particle number concentration of 6500 cm-3 stp), as well as PM1 concentration (11.9 μg m-3 stp). Two classes of organic aerosols were estimated based on C-ToF-AMS: particulate organic nitrates (pONs) and isoprene epoxydiols secondary organic aerosols (IEPOX-SOA). Both classes are usually associated with the formation of particulate matter through complex interactions of anthropogenic and biogenic sources. During DACCIWA, pONs have a fairly small contribution to OA (around 5 %) and are more associated with long-range transport from central Africa than local formation. Conversely, IEPOX-SOA provides a significant contribution to OA (around 24 and 28 % under background and in-plume conditions). Furthermore, the fractional contribution of IEPOX-SOA is largely unaffected by changes in the aerosol composition (particularly the SO4 concentration), which suggests that IEPOX-SOA concentration is mainly driven by pre-existing aerosol surface, instead of aerosol chemical properties. At times of large in-plume SO4 enhancements (above 5 μg m-3), the fractional contribution of IEPOX-SOA to OA increases above 50 %, suggesting only then a change in the IEPOX-SOA-controlling mechanism. It is important to note that IEPOX-SOA constitutes a lower limit to the contribution of biogenic OA, given that other processes (e.g. non-IEPOX isoprene, monoterpene SOA) are likely in the region. Given the significant contribution to aerosol concentration, it is crucial that such complex biogenic-anthropogenic interactions are taken into account in both present-day and future scenario models of this fast-changing, highly sensitive region

Evaluating major anthropogenic VOC emission sources in densely populated Vietnamese cities

Volatile organic compounds (VOCs) play an important role in urban air pollution, both as primary pollutants and through their contribution to the formation of secondary pollutants, such as tropospheric ozone and secondary organic aerosols. In this study, more than 30 VOC species were continuously monitored in the two most populous cities in Vietnam, namely Ho Chi Minh City (HCMC, September-October 2018 and March 2019) and Hanoi (March 2019). In parallel with ambient VOC sampling, grab sampling was used to target the most prevalent regional-specific emission sources and estimate their emission factors (EFs). Emission ratios (ERs) obtained from ambient sampling were compared between Vietnamese cities and other cities across the globe. No significant differences were observed between HCMC and Hanoi, suggesting the presence of similar sources. Moreover, a good global agreement was obtained in the spatial comparison within a factor of 2, with greater ER for aromatics and pentanes obtained in the Vietnamese cities. The detailed analysis of sources included the evaluation of EF from passenger cars, buses, trucks, motorcycles, 3-wheeled motorcycles, waste burning, and coal-burning emissions. Our comparisons between ambient and near-source concentration profiles show that road transport sources are the main contributors to VOC concentrations in Vietnamese cities. VOC emissions were calculated from measured EF and consumption data available in Hanoi and compared with those estimated by a global emission inventory (EDGAR v4.3.2). The total VOC emissions from the road transport sector estimated by the inventory do not agree with those calculated from our observations which showed higher total emissions by a factor of 3. Furthermore, the inventory misrepresented the VOCs speciation, mainly for isoprene, monoterpenes, aromatics, and oxygenated compounds. Accounting for these differences in regional air quality models would lead to improved predictions of their impacts and help to prioritise pollution reduction strategies in the region

Aircraft-based mass balance estimate of methane emissions from offshore gas facilities in the southern North Sea

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.</p

Composition and chemical processing of volatile organic compounds in boundary layer polluted plumes: Insights from an airborne Q-PTR-MS on-board the French ATR-42 aircraft

International audienc

Aerosol distribution in the northern Gulf of Guinea : local anthropogenic sources, long-range transport, and the role of coastal shallow circulations

The complex vertical distribution of aerosols over coastal southernWest Africa (SWA) is investigated using airborne observations and numerical simulations. Observations were gathered on 2 July 2016 offshore of Ghana and Togo, during the field phase of the Dynamics-Aerosol-Chemistry-Cloud Interactions in West Africa project. This was the only flight conducted over the ocean during which a downward-looking lidar was operational. The aerosol loading in the lower troposphere includes emissions from coastal cities (Accra, Lome, Cotonou, and Lagos) as well as biomass burning aerosol and dust associated with long-range transport from central Africa and the Sahara, respectively. Our results indicate that the aerosol distribution on this day is impacted by subsidence associated with zonal and meridional regional-scale overturning circulations associated with the land-sea surface temperature contrast and orography over Ghana and Togo, as typically observed on hot, cloud-free summer days such as 2 July 2016. Furthermore, we show that the zonal circulation evidenced on 2 July is a persistent feature over the Gulf of Guinea during July 2016. Numerical tracer re-lease experiments highlight the dominance of aged emissions from Accra on the observed pollution plume loadings over the ocean, in the area of aircraft operation. The contribution of aged emission from Lome and Cotonou is also evident above the marine boundary layer. Given the general direction of the monsoon flow, the tracer experiments indicate no contribution from Lagos emissions to the atmospheric composition of the area west of Cotonou, where our airborne observations were gathered. The tracer plume does not extend very far south over the ocean (i.e. less than 100 km from Accra), mostly because emissions are transported northeastward near the surface over land and westward above the marine atmospheric boundary layer. The latter is possible due to interactions between the monsoon flow, complex terrain, and land-sea breeze systems, which support the vertical mixing of the urban pollution. This work sheds light on the complex - and to date undocumented - mechanisms by which coastal shallow circulations can distribute atmospheric pollutants over the densely populated SWA region.Peer reviewe

Discovering oxidative potential (OP) drivers of atmospheric PM10, PM2.5, and PM1 simultaneously in North-Eastern Spain

Ambient particulate matter (PM) is a major contributor to air pollution, leading to adverse health effects on the human population. It has been suggested that the oxidative potential (OP, as a tracer of oxidative stress) of PM is a possible determinant of its health impact. In this study, samples of PM10, PM2.5, and PM1 were collected roughly every four days from January 2018 until March 2019 at a Barcelona urban background site and Montseny rural background site in northeastern Spain. We determined the chemical composition of samples, allowing us to perform source apportionment using positive matrix factorization. The OP of PM was determined by measuring reactive oxygen species using dithiothreitol and ascorbic acid assays. Finally, to link the sources with the measured OP, both a Pearson's correlation and a multiple linear regression model were applied to the dataset. The results showed that in Barcelona, the OP of PM10 was much higher than those of PM2.5 and PM1, whereas in Montseny results for all PM sizes were in the same range, but significantly lower than in Barcelona. In Barcelona, several anthropogenic sources were the main drivers of OP in PM10 (Combustion + Road Dust + Heavy Oil + OC-rich) and PM2.5 (Road Dust + Combustion). In contrast, PM1 -associated OP was driven by Industry, with a much lower contribution to PM10 and PM2.5 mass. Meanwhile, Montseny exhibited no clear drivers for OP evolution, likely explaining the lack of a significant difference in OP between PM10, PM2.5, and PM1. Overall, this study indicates that size fraction matters for OP, as a function of the environment typology. In an urban context, OP is driven by the PM10 and PM1 size fractions, whereas only the PM1 fraction is involved in rural environments.The present work was supported by the European Union's Horizon 2020 research and innovation program under grant agreement 101036245 (RI-URBANS); the “Agencia Estatal de Investigación” from the Spanish Ministry of Science and Innovation, and FEDER funds under the projects CAIAC (PID2019-108990RB-I00); and the Generalitat de Catalunya (AGAUR 2017 SGR41) and the Direcció General de Territori.Peer reviewe

High Resolution Dynamical Analysis of Volatile Organic Compounds (VOC) Measurements During the BIO‐MAÏDO Field Campaign (Réunion Island, Indian Ocean)

International audienceVolatile organic compounds (VOCs) in the atmosphere are fundamental in atmospheric chemical oxidation processes and are involved in health and climate impacts (Mellouki et al., 2015; Rumchev et al., 2007; Seinfeld & Pandis, 2016). VOC are emitted by both biogenic and anthropogenic sources and play an important role in atmospheric chemistry in ozone and secondary organic aerosol (SOA) formation