Secondary organic aerosol origin in an urban environment: Influence of biogenic and fuel combustion precursors

Source contributions of organic aerosol (OA) are still not fully understood, especially in terms of quantitative distinction between secondary OA formed from anthropogenic precursors vs. that formed from natural precursors. In order to investigate the OA origin, a field campaign was carried out in Barcelona in summer 2013, including two periods characterized by low and high traffic conditions. Volatile organic compound (VOC) concentrations were higher during the second period, especially aromatic hydrocarbons related to traffic emissions, which showed a marked daily cycle peaking during traffic rush hours, similarly to black carbon (BC) concentrations. Biogenic VOC (BVOC) concentrations showed only minor changes from the low to the high traffic period, and their intra-day variability was related to temperature and solar radiation cycles, although a decrease was observed for monoterpenes during the day. The organic carbon (OC) concentrations increased from the first to the second period, and the fraction of non-fossil OC as determined by C analysis increased from 43% to 54% of the total OC. The combination of C analysis and Aerosol Chemical Speciation Monitor (ACSM) OA source apportionment showed that the fossil OC was mainly secondary (>70%) except for the last sample, when the fossil secondary OC only represented 51% of the total fossil OC. The fraction of non-fossil secondary OC increased from 37% of total secondary OC for the first sample to 60% for the last sample. This enhanced formation of non-fossil secondary OA (SOA) could be attributed to the reaction of BVOC precursors with NO emitted from road traffic (or from its nocturnal derivative nitrate that enhances night-time semi-volatile oxygenated OA (SV-OOA)), since NO concentrations increased from 19 to 42 μg m from the first to the last sample

A GIS model-based assessment of the environmental distribution of g-hexachlorocyclohexane in European soils and waters

The MAPPE GIS based multimedia model is used to produce a quantitative description of the behaviour of γ-hexachlorocyclohexane (γ-HCH) in Europe, with emphasis on continental surface waters. The model is found to reasonably reproduce γ-HCH distributions and variations along the years in atmosphere and soil; for continental surface waters, concentrations were reasonably well predicted for year 1995, when lindane was still used in agriculture, while for 2005, assuming severe restrictions in use, yields to substantial underestimation. Much better results were yielded when same mode of release as in 1995 was considered, supporting the conjecture that for γ-HCH, emission data rather that model structure and parameterization can be responsible for wrong estimation of concentrations. Future research should be directed to improve the quality of emission data. Joint interpretation of monitoring and modelling results, highlights that lindane emissions in Europe, despite the marked decreasing trend, persist beyond the provisions of existing legislation. An spatially-explicit multimedia modelling strategy was applied to describe the historical distribution of γ-HCH in European soils and surface waters

Effects of sources and meteorology on particulate matter in the Western Mediterranean Basin: an overview of the DAURE campaign

DAURE (Determination of the Sources of Atmospheric Aerosols in Urban and Rural Environments in the Western Mediterranean) was a multidisciplinary international field campaign aimed at investigating the sources and meteorological controls of particulate matter in the Western Mediterranean Basin (WMB). Measurements were simultaneously performed at an urban-coastal (Barcelona, BCN) and a rural-elevated (Montseny, MSY) site pair in NE Spain during winter and summer. State-of-the-art methods such as 14C analysis, proton-transfer reaction mass spectrometry, and high-resolution aerosol mass spectrometry were applied for the first time in the WMB as part of DAURE. WMB regional pollution episodes were associated with high concentrations of inorganic and organic species formed during the transport to inland areas and built up at regional scales. Winter pollutants accumulation depended on the degree of regional stagnation of an air mass under anticyclonic conditions and the planetary boundary layer height. In summer, regional recirculation and biogenic secondary organic aerosols (SOA) formation mainly determined the regional pollutant concentrations. The contribution from fossil sources to organic carbon (OC) and elemental carbon (EC) and hydrocarbon-like organic aerosol concentrations were higher at BCN compared with MSY due to traffic emissions. The relative contribution of nonfossil OC was higher at MSY especially in summer due to biogenic emissions. The fossil OC/EC ratio at MSY was twice the corresponding ratio at BCN indicating that a substantial fraction of fossil OC was due to fossil SOA. In winter, BCN cooking emissions were identified as an important source of modern carbon in primary organic aerosol

Evaluation of air quality changes in a Chinese megacity over a 15-year period (2006-2021) using PM2.5 receptor modelling

Air quality impairment has a massive impact on human health, with atmospheric particulate matter (PM) playing a major role. The People's Republic of China experienced a trend of increasing PM2.5 concentrations from 2000 to 2013. However, after the application of the Air Pollution Prevention and Control Action Plan and other related control measures, sharp decreases in air pollutant concentrations were particularly evident in the city of Wuhan (central China). This study analysed major changes in PM2.5 concentrations, composition and source apportionment (using receptor modelling) based on Wuhan's PM2.5 chemical speciation datasets from 2006 to 2007, 2019-2021 and contemporaneous gaseous pollutant values. Average SO2 concentrations decreased by 88%, from the first to the second period, mostly due to measures that reduced coal combustion. However, NO2 only declined by 25%, with policy measures likely being undermined by an increased number of vehicles. PM2.5 concentrations decreased by 65%, with the PM constituents each being affected differently. Coal combustion-related element concentrations, OC, SO42-, NH4+, EC, Cl-, Al, Ca, Cu, Fe, Co and NO3- decreased by 22-90%. Secondary inorganic aerosol (SIA) was initially dominated by (NH4)2SO4 (73%) in 2006, but later dominated by NH4NO3 (52%) in 2021. Receptor modelling identified major sources contributing to PM2.5: Mineral, road and desert dust (MRDD), Secondary sulphate (SECS), Secondary nitrate (SECN), Tungsten industry (W), Toxic Elements of Coal (TEC), Iron and Steel (IRONS), Coal Combustion (CC), Residential Heating (RH), Refinery (REF) and Traffic (TRF). In relative proportions, TEC (-83%), SECS (-64%) and SECN (-48%) reduced their contributions to PM2.5 whilst MRDD increased (+62.5%). Thus, the results indicate not only a drastic abatement of PM pollution in Wuhan but also a change in the sources of pollution, which requires further actions to reduce PM2.5 concentrations to health protective values. Secondary PM and fugitive emissions are key components to abate.This research was supported by the National Nature Science Foundation of China (Nos. 41972179, 41972180); the European Union's Horizon 2020 research and innovation program under grant agreement 101036245 (RI-URBANS); and the Generalitat de Catalunya (AGAUR 2021 SGR 00447). The authors would like to express our gratitude to the NOAA Air Resources Laboratory (ARL) for the provision of the HYSPLIT transport and dispersion model.Peer reviewe

Cloud condensation nuclei activation properties of Mediterranean pollen types considering organic chemical composition and surface tension effects

Wind-dispersed pollen grains emitted from vegetation are directly injected into the atmosphere being an important source of natural aerosols globally. These coarse particles of pollen can rupture into smaller particles, known as subpollen particles (SPPs), that may act as cloud condensation nuclei (CCN) and affect the climate. In this study, we characterize and investigate the ability of SPPs of 10 Mediterranean-climate pollen types to activate as CCN. A continuous flow CCN counter (CCNC) was used to measure the activation of size-selected (80, 100 and 200 nm dry mobility diameter) particles at different supersaturations (SS). Hygroscopicity parameter (κ) for each SPP type and size has been calculated using κ-Köhler theory. Organic chemical speciation and protein content has been determined to further characterize pollen solutions. Furthermore, the surface activity of SPPs has also been investigated by using pendant drop tensiometry. All studied SPP samples show critical supersaturation (SSCrit) values that are atmospherically relevant SS conditions. Hygroscopicity κ values are in the range characteristic of organic compounds (0.1–0.3). We found that organic speciation and protein content vary substantially among pollen types, with saccharides and fatty acids being the only organic compounds found in all pollen types. A clear relationship between SPP activation and its organic composition was not observed. This study also reveals that all SPPs investigated reduce the surface tension of water at high concentrations but at diluted concentrations (such as those of activation in the CCNC), the water surface tension value is a good approximation in Köhler theory. Overall, this analysis points out that pollen particles might be an important source of CCN in the atmosphere and should be considered in aerosol-cloud interactions processes.This work was supported by BioCloud project (RTI2018.101154.A.I00) funded by MCIN/AEI/10.13039/501100011033, FEDER “Una manera de hacer Europa” and NUCLEUS project (PID2021-128757OB-I00) funded by MCIN/AEI/10.13039/501100011033 and NextGenerationEU/PRTR. This work received support from the European Union's Horizon 2020 research and innovation program through projects ACTRIS.IMP (grant agreement No 871115) and ATMO_ACCESS (grant agreement No 101008004), by the Spanish Ministry of Science and Innovation through projects ELPIS (PID2020-120015RB-I00) and ACTRIS-España (CGL2017-90884REDT)). By the Junta de Andalucía Excellence, project ADPANE (P20-00136), AEROPRE (P-18-RT-3820) and by University of Granada Plan Propio through Visiting Scholars (PPVS2018-04), Singular Laboratory (LS2022-1) programs and Pre-Competitive Research Projects Pre-Greenmitigation3 (PP2022.PP34). Funding for open access charge, University of Granada/CBUA. Andrea Casans is funded by Spanish ministry of research and innovation under the predoctoral program FPI (PRE2019-090827) funded by MCIN/AEI/10.13039/501100011033, FSE “El FSE invierte en tu futuro”. Fernando Rejano is funded by Spanish ministry of universities through predoctoral grant FPU19/05340. Juan Andrés Casquero-Vera is funded by FJC2021-047873-I, MCIN/AEI/10.13039/501100011033 and NextGenerationEU/PRTR. Elisabeth Andrews is funded in part by NOAA cooperative agreements NA17OAR4320101. Thanks to the NOAA Global Monitoring Laboratory for the use of the CCN counter.Peer reviewe

An Overview of Three Promising Mechanical, Optical, and Biochemical Engineering Approaches to Improve Selective Photothermolysis of Refractory Port Wine Stains

During the last three decades, several laser systems, ancillary technologies, and treatment modalities have been developed for the treatment of port wine stains (PWSs). However, approximately half of the PWS patient population responds suboptimally to laser treatment. Consequently, novel treatment modalities and therapeutic techniques/strategies are required to improve PWS treatment efficacy. This overview therefore focuses on three distinct experimental approaches for the optimization of PWS laser treatment. The approaches are addressed from the perspective of mechanical engineering (the use of local hypobaric pressure to induce vasodilation in the laser-irradiated dermal microcirculation), optical engineering (laser-speckle imaging of post-treatment flow in laser-treated PWS skin), and biochemical engineering (light- and heat-activatable liposomal drug delivery systems to enhance the extent of post-irradiation vascular occlusion)