Modelling the impacts of emission changes on O3 sensitivity, atmospheric oxidation capacity and pollution transport over the Catalonia region

oai:publications.copernicus.org:egusphere109352Tropospheric ozone (O3) is an important surface pollutant in urban areas, and it has complex formation mechanisms that depend on the atmospheric chemistry and meteorological factors. The severe reductions observed in anthropogenic emissions during the COVID-19 pandemic can further our understanding of the photochemical mechanisms leading to O3 formation and provide guidance for policies aimed at reducing air pollution. In this study, we use the air quality model WRF-Chem coupled with the urban canopy model BEP-BEM to investigate changes in the ozone chemistry over the Metropolitan Area of Barcelona (AMB) and its atmospheric plume moving northwards, which is responsible for the highest number of hourly O3 exceedances in Spain. The trajectories of the air masses from the AMB to the Pyrenees are studied with the Lagrangian particle dispersion model FLEXPART-WRF. The aim is to investigate the response of ozone chemistry to changes in the precursor emissions. The results show that with the reduction in emissions: 1) the ozone chemistry tends to enter the nitrogen oxide (NOx)-limited or transition regimes; however, highly polluted urban areas are still in the Volatile Organic Compounds (VOC)-limited regime, 2) the reduced O3 production is overwhelmed by reduced nitric oxide (NO) titration, resulting in a net increase in the O3 concentration (up to 20 %) in the evening, 3) the increase in the maximum O3 level (up to 6 %) during the lockdown could be attributable to an enhancement in the atmospheric oxidation capacity (AOC), 4) the daily maximum levels of ozone and odd oxygen species (Ox) generally decreased (4 %) in May with the reduced AOC, indicating an improvement in the air quality, and, 5) ozone precursor concentration changes in the AMB contribute to the pollution plume moving along the S&ndash;N valley to the Pyrenees. Our results indicate that O3 abatement strategies cannot rely only on NOx emission control but must include a significant reduction in anthropogenic sources of VOCs (e.g., for power plants and heavy industry). In addition, our results show that mitigation strategies intended to reduce O3 should be designed according to the local meteorology, air transport, particular ozone regimes and AOC of the urban area.</p

Variability of methane fluxes at the Ebro Delta due to rice field: comparison between inventories and Radon Tracer Method based results.

The Ebro River Delta, in the northwestern Mediterranean basin, has an extension of 320 km2 and is mainly covered by rice fields. Rice fields are known to be one of the main sources of anthropogenic methane emissions, and a better estimation of its temporal variability in relation to the different rice cultivation phases is important to help with the implementation of emission reduction strategies (Àgueda et al., 2017), In the framework of the ClimaDat network, an atmospheric station was installed in the middle of the Ebro Delta in 2012. A Picarro G2301 for greenhouse gases (GHG) atmospheric concentrations and an ARMON (Atmospheric Radon Monitor) for atmospheric 222Rn concentrations were collocated among other instruments. Nocturnal hourly atmospheric observations of CH4 and 222Rn measured between 2013 and 2019 were used to apply the Radon Tracer Method (RTM) for retrieving CH4 fluxes over the footprint area. The Ebro River Delta has a reduced dimension and a complex meteorological regime highly influenced by the Ebro channelled winds and the sea breezes, making it difficult to calculate GHG fluxes using global or regional inversion models. However, the use of high-resolution backtrajectories (model WRF-Flexpart) coupled with the traceRadon daily radon flux maps for Europe (Karsten et al., 2022), with a resolution of 0.05 degrees, has allowed the use of the RTM in this complex area. Methane fluxes estimated by RTM were compared with fluxes directly measured with chambers in past studies (Martínez-Eixarch et al., 2018) and with data obtained by the EDGAR inventory (Crippa et al., 2022). Results show a promising agreement between methane fluxes obtained with different methods, and a variability clearly governed by the rice crop cycle which is not reflected in the methane emissions values reported in EDGAR inventories.Peer ReviewedPostprint (published version

Metrology for low-cost CO2 sensors applications: the case of a steady-state through-flow (SS-TF) chamber for CO2 fluxes observations

Soil CO2 emissions are one of the largest contributions to the global carbon cycle, and a full understanding of processes generating them and how climate change may modify them is needed and still uncertain. Thus, a dense spatial and temporal network of CO2 flux measurements from soil could help reduce uncertainty in the global carbon budgets. In the present study, the design, assembly, and calibration of low-cost air enquirer kits, including CO2 and environmental parameters sensors, is presented. Different types of calibrations for the CO2 sensors and their associated errors are calculated. In addition, for the first time, this type of sensor has been applied to design, develop, and test a new steady-state through-flow (SS-TF) chamber for simultaneous measurements of CO2 fluxes in soil and CO2 concentrations in air. The sensors’ responses were corrected for temperature, relative humidity, and pressure conditions in order to reduce the uncertainty in the measured CO2 values and of the following calculated CO2 fluxes based on SS-TF. CO2 soil fluxes measured by the proposed SS-TF and by a standard closed non-steady-state non-through-flow (NSS-NTF) chamber were briefly compared to ensure the reliability of the results. The use of a multiparametric fitting reduced the total uncertainty of the CO2 concentration measurements by 62 %, compared with the uncertainty that occurred when a simple CO2 calibration was applied, and by 90 %, when compared to the uncertainty declared by the manufacturer. The new SSTF system allows the continuous measurement of CO2 fluxes and CO2 ambient air with low cost (EUR ~ 1200), low energy demand (< 5 W), and low maintenance (twice per year due to sensor calibration requirements).Peer ReviewedPostprint (published version

Characterizing the automatic radon flux transfer standard system autoflux: laboratory calibration and field experiments

High-quality, long-term measurements of terrestrial trace gas emissions are important for investigations of atmospheric, geophysical and biological processes to help mitigate climate change and protect the environment and the health of citizens. High-frequency terrestrial fluxes of the radioactive noble gas 222Rn, in particular, are useful for validating radon flux maps and used to evaluate the performance of regional atmospheric models, to improve greenhouse gas emission inventories (by the radon tracer method) and to determine radon priority areas for radiation protection goals. A new automatic radon flux system (Autoflux) was developed as a transfer standard (TS) to assist with establishing a traceability chain for field-based radon flux measurements. The operational characteristics and features of the system were optimized based on a literature review of existing flux measurement systems. To characterize and calibrate Autoflux, a bespoke radon exhalation bed (EB) facility was also constructed with the intended purpose of providing a constant radon exhalation under a specific set of controlled laboratory conditions. The calibrated Autoflux was then used to transfer the derived calibration to a second continuous radon flux system under laboratory conditions; both instruments were then tested in the field and compared with modeled fluxes. This paper presents (i) a literature review of state-of-the-art radon flux systems and EB facilities; (ii) the design, characterization and calibration of a reference radon EB facility; (iii) the design, characterization and calibration of the Autoflux system; (iv) the calibration of a second radon flux system (INTE_Flux) using the EB and Autoflux, with a total uncertainty of 9% (k=1) for an average radon flux of ~1800mBqm-2s-1 under controlled laboratory conditions; and (v) an example application of the calibrated TS and INTE_Flux systems for in situ radon flux measurements, which are then compared with simulated radon fluxes. Calibration of the TS under different environmental conditions and at lower reference fluxes will be the subject of a separate future investigation.Peer ReviewedPostprint (published version

Atmospheric Carbon Dioxide variability at Aigüestortes, Central Pyrenees, Spain

Unidad de excelencia María de Maeztu MdM-2015-0552In order to improve the understanding of the carbon cycle in the Pyrenean region, two atmospheric monitoring mountain stations were set up within the Long-Term Ecological Research node of Aigüestortes i Estany de Sant Maurici at Central Pyrenees, Spain. The atmospheric concentration of carbon dioxide (CO2) was measured over 2008-2014 and 2010-2014 at Estany Llong (ELL) site and Centre de Recerca d'Alta Muntanya (CRAM), respectively. Measurements were carried out fortnightly off-line with high precision instrumentation at ELL and every minute online with a lower precision sensor at CRAM in conjunction with meteorological variables. The two datasets were analyzed in this study, quantifying whenever possible annual growth rates (AGR), seasonal variability, and diurnal amplitudes. Results were also compared with the NOAA Marine Boundary Layer (MBL) reference product and CO2 data from other background monitoring stations. Four-harmonics adjusted CO2 data from ELL showed a high correlation with the NOAA MBL reference product for the same latitude (Spearman's rho ρ = 0.96). In addition, AGRs of CO2 at ELL correlated well with those observed at Mace Head (MHD) station (ρ = 0.94), suggesting that ELL can be considered a background station. Winter CRAM CO2 data was not statistically different from ELL data, while in summer, it was 5.5 ppm lower on average, suggesting a higher photosynthesis uptake. The amplitude of the CO2 diurnal cycle at CRAM was found to be exponentially related to the local mean daily temperature and dependent on forthcoming wind sector (N-NW or E-SE-S-SW). An increase in CRAM CO2 concentrations was observed under N-NW winds during daytime, which could be related to traffic emissions. This study demonstrates that the use of CO2 sensors with low precision but continuously corrected and periodically calibrated can be used for the study of local and regional CO2 sources and sinks

On the interpretation of the atmospheric mechanism transporting the environmental trigger of Kawasaki disease

Unidad de excelencia María de Maeztu MdM-2015-0552Recent advances on the environmental determinants of Kawasaki Disease have pointed to the important role of the atmospheric transport of a still unknown agent potentially triggering the disease. The hypothesis arose from an innovative methodology combining expertise in climate dynamics, the analysis of ocean and atmosphere data, the use of dispersion models and the search for biological agents in air samples. The approach offered a new perspective to reveal the identity of the potential trigger, but at the same time, it increased the level of complexity, which could potentially lead to the misinterpretation of the mechanisms. Some years after it was originally formulated, we here provide a brief clarification on the approach and limits of the methodology in order to prevent an eventual misuse of our research ideas and theory, so that further research can better focus on the knowledge gaps that still remain open

On the interpretation of the atmospheric mechanism transporting the environmental trigger of Kawasaki disease

Unidad de excelencia María de Maeztu MdM-2015-0552Recent advances on the environmental determinants of Kawasaki Disease have pointed to the important role of the atmospheric transport of a still unknown agent potentially triggering the disease. The hypothesis arose from an innovative methodology combining expertise in climate dynamics, the analysis of ocean and atmosphere data, the use of dispersion models and the search for biological agents in air samples. The approach offered a new perspective to reveal the identity of the potential trigger, but at the same time, it increased the level of complexity, which could potentially lead to the misinterpretation of the mechanisms. Some years after it was originally formulated, we here provide a brief clarification on the approach and limits of the methodology in order to prevent an eventual misuse of our research ideas and theory, so that further research can better focus on the knowledge gaps that still remain open

First estimation of CH4fluxes using the222Rn Tracer Method over the central Iberian Peninsula

Emissions of CH4 over the central Iberian Peninsula have been estimated experimentally for the first time using the Radon Tracer Method (RTM), which uses the atmospheric noble radioactive gas 222Rn as an auxiliary tracer. The nocturnal enhancement ratios of atmospheric concentrations of CH4 and 222Rn, continuously measured at the station of Gredos and Iruelas within the IC3 network since 2012, were used to early estimate the methane emissions in this region by multiplying for a constant radon flux. The possible influence of different methane source areas was observed by footprint analysis of FLEXPART with ECMWF meteorological input at 0.2 degrees horizontal resolution. A linear relationship between atmospheric radon and methane concentrations has been found to occur in 20% of the nocturnal episodes and an average methane emission of 0.12 mg m-2 h-1 ± 0.03 (1 s). The data coverage and method is coherent with CH4 fluxes inferred with the same RTM in Germany, Canada and East Asia and our flux estimates are similar to methane emissions reported by the bottom-up inventory EDGARv4.2 .Peer ReviewedPostprint (published version

Quantification of CH4 emissions from waste disposal sites near the city of Madrid using ground- and space-based observations of COCCON, TROPOMI and IASI

The objective of this study is to derive methane (CH4) emissions from three landfills, which are found to be the most significant CH4 sources in the metropolitan area of Madrid in Spain. We derive CH4 emissions from the CH4 enhancements observed by spaceborne and ground-based instruments. We apply satellite-based measurements from the TROPOspheric Monitoring Instrument (TROPOMI) and the Infrared Atmospheric Sounding Interferometer (IASI) together with measurements from the ground-based COllaborative Carbon Column Observing Network (COCCON) instruments. In 2018, a 2-week field campaign for measuring the atmospheric concentrations of greenhouse gases was performed in Madrid in the framework of Monitoring of the Greenhouse Gases Concentrations in Madrid (MEGEI-MAD) project. Five COCCON instruments were deployed at different locations around the Madrid city center, enabling the observation of total column-averaged CH4 mixing ratios (XCH4). Considering the prevalent wind regimes, we calculate the wind-assigned XCH4 anomalies for two opposite wind directions. Pronounced bipolar plumes are found when applying the method to NO2, which implies that our method of wind-assigned anomaly is suitable to estimate enhancements of trace gases at the urban level from satellite-based measurements. For quantifying the CH4 emissions, the wind-assigned plume method is applied to the TROPOMI XCH4 and to the lower tropospheric CH4¿¿dry-air column ratio (TXCH4) of the combined TROPOMI+IASI product.Peer ReviewedArticle signat per 28 Autors/es Qiansi Tu, Frank Hase, Matthias Schneider, Omaira García, Thomas Blumenstock,Tobias Borsdorff, Matthias Frey, Farahnaz Khosrawi, Alba Lorente, Carlos Alberti,Juan J. Bustos, André Butz, Virgilio Carreño, Emilio Cuevas, Roger Curcoll,Christopher J. Diekmann, Darko Dubravica, Benjamin Ert, Carme Estruch,Sergio Fabián León-Luis, Carlos Marrero, Josep-Anton Morgui, Ramón Ramos,Christian Scharun, Carsten Schneider, Eliezer Sepúlveda, Carlos Toledano, Carlos TorresObjectius de Desenvolupament Sostenible::13 - Acció per al ClimaPostprint (published version