Articles | Volume 21, issue 12
https://doi.org/10.5194/acp-21-9309-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-9309-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Non-linear response of PM2.5 to changes in NOx and NH3 emissions in the Po basin (Italy): consequences for air quality plans
Philippe Thunis
CORRESPONDING AUTHOR
European Commission, Joint Research Centre, Ispra, Italy
Alain Clappier
Université de Strasbourg, Laboratoire Image Ville Environnement, Strasbourg, France
Matthias Beekmann
Université de Paris and Université Paris-Est Créteil, CNRS, LISA, F-75013 Paris, France
Jean Philippe Putaud
European Commission, Joint Research Centre, Ispra, Italy
Cornelis Cuvelier
European Commission, Joint Research Centre, Ispra, Italy
retired
Jessie Madrazo
Signa Terre SA, Geneva, Switzerland
Alexander de Meij
MetClim, Varese, Italy
Related authors
Alexander de Meij, Cornelis Cuvelier, Philippe Thunis, and Enrico Pisoni
Geosci. Model Dev., 18, 4231–4245, https://doi.org/10.5194/gmd-18-4231-2025, https://doi.org/10.5194/gmd-18-4231-2025, 2025
Short summary
Short summary
We assess relevance and utility indicators by evaluating nine Copernicus Atmospheric Monitoring Service models in calculated air pollutant values. For NO2, the results highlight difficulties at traffic stations. For PM2.5 and PM10 the bias and winter–summer gradients reveal issues. O3 evaluation shows that seasonal gradients are useful. Overall, the indicators reveal model limitations, yet there is a need to reconsider the strictness of some indicators for certain pollutants.
Philippe Thunis, Jeroen Kuenen, Enrico Pisoni, Bertrand Bessagnet, Manjola Banja, Lech Gawuc, Karol Szymankiewicz, Diego Guizardi, Monica Crippa, Susana Lopez-Aparicio, Marc Guevara, Alexander De Meij, Sabine Schindlbacher, and Alain Clappier
Geosci. Model Dev., 17, 3631–3643, https://doi.org/10.5194/gmd-17-3631-2024, https://doi.org/10.5194/gmd-17-3631-2024, 2024
Short summary
Short summary
An ensemble emission inventory is created with the aim of monitoring the status and progress made with the development of EU-wide inventories. This emission ensemble serves as a common benchmark for the screening and allows for the comparison of more than two inventories at a time. Because the emission “truth” is unknown, the approach does not tell which inventory is the closest to reality, but it identifies inconsistencies that require special attention.
Alexander de Meij, Cornelis Cuvelier, Philippe Thunis, Enrico Pisoni, and Bertrand Bessagnet
Geosci. Model Dev., 17, 587–606, https://doi.org/10.5194/gmd-17-587-2024, https://doi.org/10.5194/gmd-17-587-2024, 2024
Short summary
Short summary
In our study the robustness of the model responses to emission reductions in the EU is assessed when the emission data are changed. Our findings are particularly important to better understand the uncertainties associated to the emission inventories and how these uncertainties impact the level of accuracy of the resulting air quality modelling, which is a key for designing air quality plans. Also crucial is the choice of indicator to avoid misleading interpretations of the results.
Lina Vitali, Kees Cuvelier, Antonio Piersanti, Alexandra Monteiro, Mario Adani, Roberta Amorati, Agnieszka Bartocha, Alessandro D'Ausilio, Paweł Durka, Carla Gama, Giulia Giovannini, Stijn Janssen, Tomasz Przybyła, Michele Stortini, Stijn Vranckx, and Philippe Thunis
Geosci. Model Dev., 16, 6029–6047, https://doi.org/10.5194/gmd-16-6029-2023, https://doi.org/10.5194/gmd-16-6029-2023, 2023
Short summary
Short summary
Air quality forecasting models play a key role in fostering short-term measures aimed at reducing human exposure to air pollution. Together with this role comes the need for a thorough assessment of the model performances to build confidence in models’ capabilities, in particular when model applications support policymaking. In this paper, we propose an evaluation methodology and test it on several domains across Europe, highlighting its strengths and room for improvement.
Philippe Thunis, Alain Clappier, Enrico Pisoni, Bertrand Bessagnet, Jeroen Kuenen, Marc Guevara, and Susana Lopez-Aparicio
Geosci. Model Dev., 15, 5271–5286, https://doi.org/10.5194/gmd-15-5271-2022, https://doi.org/10.5194/gmd-15-5271-2022, 2022
Short summary
Short summary
In this work, we propose a screening method to improve the quality of emission inventories, which are responsible for large uncertainties in air-quality modeling. The first step of screening consists of keeping only emission contributions that are relevant enough. In a second step, the method identifies large differences that provide evidence of methodological divergence or errors. We used the approach to compare two versions of the CAMS-REG European-scale inventory over 150 European cities.
Philippe Thunis, Alain Clappier, Alexander de Meij, Enrico Pisoni, Bertrand Bessagnet, and Leonor Tarrason
Atmos. Chem. Phys., 21, 18195–18212, https://doi.org/10.5194/acp-21-18195-2021, https://doi.org/10.5194/acp-21-18195-2021, 2021
Short summary
Short summary
Air pollution's origin in cities is still a point of discussion, and approaches to assess the city's responsibility for its pollution are not harmonized and thus not comparable, resulting in sometimes contradicting interpretations. We show that methodological choices can easily lead to differences of a factor of 2 in terms of responsibility outcome and stress that methodological choices and assumptions most often lead to a systematic and important underestimation of the city's responsibility.
Wenche Aas, Thérèse Salameh, Robert Wegener, Heidi Hellén, Jean-Luc Jaffrezo, Pontus Roldin, Elisabeth Alonso-Blanco, Andres Alastuey, Crist Amelynck, Jgor Arduini, Benjamin Bergmans, Marie Bertrand, Agnes Borbon, Efstratios Bourtsoukidis, Laetitia Bouvier, David Butterfield, Iris Buxbaum, Darius Ceburnis, Anja Claude, Aurélie Colomb, Sophie Darfeuil, James Dernie, Maximilien Desservettaz, Elías Díaz-Ramiro, Marvin Dufresne, René Dubus, Mario Duval, Marie Dury, Anna Font, Kirsten Fossum, Evelyn Freney, Gotzon Gangoiti, Yao Ge, Maria Carmen Gomez, Francisco J. Gómez-Moreno, Marie Gohy, Valérie Gros, Paul Hamer, Bryan Hellack, Hartmut Herrmann, Robert Holla, Adéla Holubová, Niels Jensen, Tuija Jokinen, Matthew Jones, Uwe Käfer, Lukas Kesper, Dieter Klemp, Dagmar Kubistin, Angela Marinoni, Martina Mazzini, Vy Ngoc Thuy Dinh, Jurgita Ovadnevaite, Tuukka Petäjä, Miguel Portillo-Estrada, Jitka Přívozníková, Jean-Philippe Putaud, Stefan Reimann, Laura Renzi, Veronique Riffault, Stuart Ritchie, Chris Robins, Begoña Artíñano Rodríguez de Torres, Laurent Poulain, Julian Rüdiger, Agnieszka Sanocka, Estibaliz Saez de Camara Oleaga, Niels Schoon, Roger Seco, Ivan Simmons, Leïla Simon, David Simpson, Emmanuel Tison, August Thomasson, Svetlana Tsyro, Marsailidh Twigg, Toni Tykkä, Bert Verreyken, Ana Maria Yáñez-Serrano, Sverre Solberg, Karen Yeung, Ilona Ylivinkka, Karl Espen Yttri, Ågot Watne, and Katie Williams
EGUsphere, https://doi.org/10.5194/egusphere-2025-6166, https://doi.org/10.5194/egusphere-2025-6166, 2025
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
Short summary
A one-week intensive VOC and organic-tracer campaign during the 2022 European heatwave showed contributions from both biogenic and anthropogenic sources to ozone and SOA peaks, while model–observation differences underline the need for better characterization of sources and formation pathways.
Alexander de Meij, Cornelis Cuvelier, Philippe Thunis, and Enrico Pisoni
Geosci. Model Dev., 18, 4231–4245, https://doi.org/10.5194/gmd-18-4231-2025, https://doi.org/10.5194/gmd-18-4231-2025, 2025
Short summary
Short summary
We assess relevance and utility indicators by evaluating nine Copernicus Atmospheric Monitoring Service models in calculated air pollutant values. For NO2, the results highlight difficulties at traffic stations. For PM2.5 and PM10 the bias and winter–summer gradients reveal issues. O3 evaluation shows that seasonal gradients are useful. Overall, the indicators reveal model limitations, yet there is a need to reconsider the strictness of some indicators for certain pollutants.
Hector Navarro-Barboza, Jordi Rovira, Vincenzo Obiso, Andrea Pozzer, Marta Via, Andres Alastuey, Xavier Querol, Noemi Perez, Marjan Savadkoohi, Gang Chen, Jesus Yus-Díez, Matic Ivancic, Martin Rigler, Konstantinos Eleftheriadis, Stergios Vratolis, Olga Zografou, Maria Gini, Benjamin Chazeau, Nicolas Marchand, Andre S. H. Prevot, Kaspar Dallenbach, Mikael Ehn, Krista Luoma, Tuukka Petäjä, Anna Tobler, Jaroslaw Necki, Minna Aurela, Hilkka Timonen, Jarkko Niemi, Olivier Favez, Jean-Eudes Petit, Jean-Philippe Putaud, Christoph Hueglin, Nicolas Pascal, Aurélien Chauvigné, Sébastien Conil, Marco Pandolfi, and Oriol Jorba
Atmos. Chem. Phys., 25, 2667–2694, https://doi.org/10.5194/acp-25-2667-2025, https://doi.org/10.5194/acp-25-2667-2025, 2025
Short summary
Short summary
Brown carbon (BrC) absorbs ultraviolet (UV) and visible light, influencing climate. This study explores BrC's imaginary refractive index (k) using data from 12 European sites. Residential emissions are a major organic aerosol (OA) source in winter, while secondary organic aerosol (SOA) dominates in summer. Source-specific k values were derived, improving model accuracy. The findings highlight BrC's climate impact and emphasize source-specific constraints in atmospheric models.
Pamela A. Dominutti, Jean-Luc Jaffrezo, Anouk Marsal, Takoua Mhadhbi, Rhabira Elazzouzi, Camille Rak, Fabrizia Cavalli, Jean-Philippe Putaud, Aikaterini Bougiatioti, Nikolaos Mihalopoulos, Despina Paraskevopoulou, Ian Mudway, Athanasios Nenes, Kaspar R. Daellenbach, Catherine Banach, Steven J. Campbell, Hana Cigánková, Daniele Contini, Greg Evans, Maria Georgopoulou, Manuella Ghanem, Drew A. Glencross, Maria Rachele Guascito, Hartmut Herrmann, Saima Iram, Maja Jovanović, Milena Jovašević-Stojanović, Markus Kalberer, Ingeborg M. Kooter, Suzanne E. Paulson, Anil Patel, Esperanza Perdrix, Maria Chiara Pietrogrande, Pavel Mikuška, Jean-Jacques Sauvain, Katerina Seitanidi, Pourya Shahpoury, Eduardo J. d. S. Souza, Sarah Steimer, Svetlana Stevanovic, Guillaume Suarez, P. S. Ganesh Subramanian, Battist Utinger, Marloes F. van Os, Vishal Verma, Xing Wang, Rodney J. Weber, Yuhan Yang, Xavier Querol, Gerard Hoek, Roy M. Harrison, and Gaëlle Uzu
Atmos. Meas. Tech., 18, 177–195, https://doi.org/10.5194/amt-18-177-2025, https://doi.org/10.5194/amt-18-177-2025, 2025
Short summary
Short summary
In this work, 20 labs worldwide collaborated to evaluate the measurement of air pollution's oxidative potential (OP), a key indicator of its harmful effects. The study aimed to identify disparities in the widely used OP dithiothreitol assay and assess the consistency of OP among labs using the same protocol. The results showed that half of the labs achieved acceptable results. However, variability was also found, highlighting the need for standardisation in OP procedures.
Philippe Thunis, Jeroen Kuenen, Enrico Pisoni, Bertrand Bessagnet, Manjola Banja, Lech Gawuc, Karol Szymankiewicz, Diego Guizardi, Monica Crippa, Susana Lopez-Aparicio, Marc Guevara, Alexander De Meij, Sabine Schindlbacher, and Alain Clappier
Geosci. Model Dev., 17, 3631–3643, https://doi.org/10.5194/gmd-17-3631-2024, https://doi.org/10.5194/gmd-17-3631-2024, 2024
Short summary
Short summary
An ensemble emission inventory is created with the aim of monitoring the status and progress made with the development of EU-wide inventories. This emission ensemble serves as a common benchmark for the screening and allows for the comparison of more than two inventories at a time. Because the emission “truth” is unknown, the approach does not tell which inventory is the closest to reality, but it identifies inconsistencies that require special attention.
Alexander de Meij, Cornelis Cuvelier, Philippe Thunis, Enrico Pisoni, and Bertrand Bessagnet
Geosci. Model Dev., 17, 587–606, https://doi.org/10.5194/gmd-17-587-2024, https://doi.org/10.5194/gmd-17-587-2024, 2024
Short summary
Short summary
In our study the robustness of the model responses to emission reductions in the EU is assessed when the emission data are changed. Our findings are particularly important to better understand the uncertainties associated to the emission inventories and how these uncertainties impact the level of accuracy of the resulting air quality modelling, which is a key for designing air quality plans. Also crucial is the choice of indicator to avoid misleading interpretations of the results.
Lina Vitali, Kees Cuvelier, Antonio Piersanti, Alexandra Monteiro, Mario Adani, Roberta Amorati, Agnieszka Bartocha, Alessandro D'Ausilio, Paweł Durka, Carla Gama, Giulia Giovannini, Stijn Janssen, Tomasz Przybyła, Michele Stortini, Stijn Vranckx, and Philippe Thunis
Geosci. Model Dev., 16, 6029–6047, https://doi.org/10.5194/gmd-16-6029-2023, https://doi.org/10.5194/gmd-16-6029-2023, 2023
Short summary
Short summary
Air quality forecasting models play a key role in fostering short-term measures aimed at reducing human exposure to air pollution. Together with this role comes the need for a thorough assessment of the model performances to build confidence in models’ capabilities, in particular when model applications support policymaking. In this paper, we propose an evaluation methodology and test it on several domains across Europe, highlighting its strengths and room for improvement.
Jean-Philippe Putaud, Enrico Pisoni, Alexander Mangold, Christoph Hueglin, Jean Sciare, Michael Pikridas, Chrysanthos Savvides, Jakub Ondracek, Saliou Mbengue, Alfred Wiedensohler, Kay Weinhold, Maik Merkel, Laurent Poulain, Dominik van Pinxteren, Hartmut Herrmann, Andreas Massling, Claus Nordstroem, Andrés Alastuey, Cristina Reche, Noemí Pérez, Sonia Castillo, Mar Sorribas, Jose Antonio Adame, Tuukka Petaja, Katrianne Lehtipalo, Jarkko Niemi, Véronique Riffault, Joel F. de Brito, Augustin Colette, Olivier Favez, Jean-Eudes Petit, Valérie Gros, Maria I. Gini, Stergios Vratolis, Konstantinos Eleftheriadis, Evangelia Diapouli, Hugo Denier van der Gon, Karl Espen Yttri, and Wenche Aas
Atmos. Chem. Phys., 23, 10145–10161, https://doi.org/10.5194/acp-23-10145-2023, https://doi.org/10.5194/acp-23-10145-2023, 2023
Short summary
Short summary
Many European people are still exposed to levels of air pollution that can affect their health. COVID-19 lockdowns in 2020 were used to assess the impact of the reduction in human mobility on air pollution across Europe by comparing measurement data with values that would be expected if no lockdown had occurred. We show that lockdown measures did not lead to consistent decreases in the concentrations of fine particulate matter suspended in the air, and we investigate why.
Philippe Thunis, Alain Clappier, Enrico Pisoni, Bertrand Bessagnet, Jeroen Kuenen, Marc Guevara, and Susana Lopez-Aparicio
Geosci. Model Dev., 15, 5271–5286, https://doi.org/10.5194/gmd-15-5271-2022, https://doi.org/10.5194/gmd-15-5271-2022, 2022
Short summary
Short summary
In this work, we propose a screening method to improve the quality of emission inventories, which are responsible for large uncertainties in air-quality modeling. The first step of screening consists of keeping only emission contributions that are relevant enough. In a second step, the method identifies large differences that provide evidence of methodological divergence or errors. We used the approach to compare two versions of the CAMS-REG European-scale inventory over 150 European cities.
Svetlana Tsyro, Wenche Aas, Augustin Colette, Camilla Andersson, Bertrand Bessagnet, Giancarlo Ciarelli, Florian Couvidat, Kees Cuvelier, Astrid Manders, Kathleen Mar, Mihaela Mircea, Noelia Otero, Maria-Teresa Pay, Valentin Raffort, Yelva Roustan, Mark R. Theobald, Marta G. Vivanco, Hilde Fagerli, Peter Wind, Gino Briganti, Andrea Cappelletti, Massimo D'Isidoro, and Mario Adani
Atmos. Chem. Phys., 22, 7207–7257, https://doi.org/10.5194/acp-22-7207-2022, https://doi.org/10.5194/acp-22-7207-2022, 2022
Short summary
Short summary
Particulate matter (PM) air pollution causes adverse health effects. In Europe, the emissions caused by anthropogenic activities have been reduced in the last decades. To assess the efficiency of emission reductions in improving air quality, we have studied the evolution of PM pollution in Europe. Simulations with six air quality models and observational data indicate a decrease in PM concentrations by 10 % to 30 % across Europe from 2000 to 2010, which is mainly a result of emission reductions.
Philippe Thunis, Alain Clappier, Alexander de Meij, Enrico Pisoni, Bertrand Bessagnet, and Leonor Tarrason
Atmos. Chem. Phys., 21, 18195–18212, https://doi.org/10.5194/acp-21-18195-2021, https://doi.org/10.5194/acp-21-18195-2021, 2021
Short summary
Short summary
Air pollution's origin in cities is still a point of discussion, and approaches to assess the city's responsibility for its pollution are not harmonized and thus not comparable, resulting in sometimes contradicting interpretations. We show that methodological choices can easily lead to differences of a factor of 2 in terms of responsibility outcome and stress that methodological choices and assumptions most often lead to a systematic and important underestimation of the city's responsibility.
Clémence Rose, Martine Collaud Coen, Elisabeth Andrews, Yong Lin, Isaline Bossert, Cathrine Lund Myhre, Thomas Tuch, Alfred Wiedensohler, Markus Fiebig, Pasi Aalto, Andrés Alastuey, Elisabeth Alonso-Blanco, Marcos Andrade, Begoña Artíñano, Todor Arsov, Urs Baltensperger, Susanne Bastian, Olaf Bath, Johan Paul Beukes, Benjamin T. Brem, Nicolas Bukowiecki, Juan Andrés Casquero-Vera, Sébastien Conil, Konstantinos Eleftheriadis, Olivier Favez, Harald Flentje, Maria I. Gini, Francisco Javier Gómez-Moreno, Martin Gysel-Beer, Anna Gannet Hallar, Ivo Kalapov, Nikos Kalivitis, Anne Kasper-Giebl, Melita Keywood, Jeong Eun Kim, Sang-Woo Kim, Adam Kristensson, Markku Kulmala, Heikki Lihavainen, Neng-Huei Lin, Hassan Lyamani, Angela Marinoni, Sebastiao Martins Dos Santos, Olga L. Mayol-Bracero, Frank Meinhardt, Maik Merkel, Jean-Marc Metzger, Nikolaos Mihalopoulos, Jakub Ondracek, Marco Pandolfi, Noemi Pérez, Tuukka Petäjä, Jean-Eudes Petit, David Picard, Jean-Marc Pichon, Veronique Pont, Jean-Philippe Putaud, Fabienne Reisen, Karine Sellegri, Sangeeta Sharma, Gerhard Schauer, Patrick Sheridan, James Patrick Sherman, Andreas Schwerin, Ralf Sohmer, Mar Sorribas, Junying Sun, Pierre Tulet, Ville Vakkari, Pieter Gideon van Zyl, Fernando Velarde, Paolo Villani, Stergios Vratolis, Zdenek Wagner, Sheng-Hsiang Wang, Kay Weinhold, Rolf Weller, Margarita Yela, Vladimir Zdimal, and Paolo Laj
Atmos. Chem. Phys., 21, 17185–17223, https://doi.org/10.5194/acp-21-17185-2021, https://doi.org/10.5194/acp-21-17185-2021, 2021
Short summary
Short summary
Aerosol particles are a complex component of the atmospheric system the effects of which are among the most uncertain in climate change projections. Using data collected at 62 stations, this study provides the most up-to-date picture of the spatial distribution of particle number concentration and size distribution worldwide, with the aim of contributing to better representation of aerosols and their interactions with clouds in models and, therefore, better evaluation of their impact on climate.
Claudio A. Belis, Guido Pirovano, Maria Gabriella Villani, Giuseppe Calori, Nicola Pepe, and Jean Philippe Putaud
Geosci. Model Dev., 14, 4731–4750, https://doi.org/10.5194/gmd-14-4731-2021, https://doi.org/10.5194/gmd-14-4731-2021, 2021
Short summary
Short summary
The study presents an in-depth analysis of the implications that using different CTM source apportionment approaches (tagged species and brute force) have for the source allocation of secondary inorganic aerosol, an important component of PM10 and PM2.5. A set of runs combining different emission levels and models was carried out, aiming to describe the situations in which strong non-linearity may lead the two approaches to deliver different results and when they are expected to be comparable.
Jean-Philippe Putaud, Luca Pozzoli, Enrico Pisoni, Sebastiao Martins Dos Santos, Friedrich Lagler, Guido Lanzani, Umberto Dal Santo, and Augustin Colette
Atmos. Chem. Phys., 21, 7597–7609, https://doi.org/10.5194/acp-21-7597-2021, https://doi.org/10.5194/acp-21-7597-2021, 2021
Short summary
Short summary
To determine the impact of the COVID lockdown on air quality in northern Italy, measurements of atmospheric pollutants (NO2, PM10, O3, NO, SO2 ) were compared to the output of a model ignoring the lockdown. We found that NO2 decreased on average by −30 % to −40 %. Unlike NO2, PM10 was not significantly affected due to the compensation of decreased emissions from traffic by increased emissions from domestic heating and/or by changes in atmospheric chemistry enhancing secondary aerosol formation.
Rosaria E. Pileci, Robin L. Modini, Michele Bertò, Jinfeng Yuan, Joel C. Corbin, Angela Marinoni, Bas Henzing, Marcel M. Moerman, Jean P. Putaud, Gerald Spindler, Birgit Wehner, Thomas Müller, Thomas Tuch, Arianna Trentini, Marco Zanatta, Urs Baltensperger, and Martin Gysel-Beer
Atmos. Meas. Tech., 14, 1379–1403, https://doi.org/10.5194/amt-14-1379-2021, https://doi.org/10.5194/amt-14-1379-2021, 2021
Short summary
Short summary
Black carbon (BC), which is an important constituent of atmospheric aerosols, remains difficult to quantify due to various limitations of available methods. This study provides an extensive comparison of co-located field measurements, applying two methods based on different principles. It was shown that both methods indeed quantify the same aerosol property – BC mass concentration. The level of agreement that can be expected was quantified, and some reasons for discrepancy were identified.
Nikolaos Evangeliou, Stephen M. Platt, Sabine Eckhardt, Cathrine Lund Myhre, Paolo Laj, Lucas Alados-Arboledas, John Backman, Benjamin T. Brem, Markus Fiebig, Harald Flentje, Angela Marinoni, Marco Pandolfi, Jesus Yus-Dìez, Natalia Prats, Jean P. Putaud, Karine Sellegri, Mar Sorribas, Konstantinos Eleftheriadis, Stergios Vratolis, Alfred Wiedensohler, and Andreas Stohl
Atmos. Chem. Phys., 21, 2675–2692, https://doi.org/10.5194/acp-21-2675-2021, https://doi.org/10.5194/acp-21-2675-2021, 2021
Short summary
Short summary
Following the transmission of SARS-CoV-2 to Europe, social distancing rules were introduced to prevent further spread. We investigate the impacts of the European lockdowns on black carbon (BC) emissions by means of in situ observations and inverse modelling. BC emissions declined by 23 kt in Europe during the lockdowns as compared with previous years and by 11 % as compared to the period prior to lockdowns. Residential combustion prevailed in Eastern Europe, as confirmed by remote sensing data.
Cited articles
Andersson-Sköld, Y. and Simpson, D.: Comparison of the chemical schemes
of the EMEP MSC-W and the IVL photochemical trajectory models, Atmos.
Environ., 33, 1111–1129, 1999.
Ansari, A. S. and Pandis, S.: Response of inorganic PM to precursor
concentrations, Environ. Sci. Technol., 32, 2706–2714, 1998.
Beekmann, M., Prévôt, A. S. H., Drewnick, F., Sciare, J., Pandis, S. N., Denier van der Gon, H. A. C., Crippa, M., Freutel, F., Poulain, L., Ghersi, V., Rodriguez, E., Beirle, S., Zotter, P., von der Weiden-Reinmüller, S.-L., Bressi, M., Fountoukis, C., Petetin, H., Szidat, S., Schneider, J., Rosso, A., El Haddad, I., Megaritis, A., Zhang, Q. J., Michoud, V., Slowik, J. G., Moukhtar, S., Kolmonen, P., Stohl, A., Eckhardt, S., Borbon, A., Gros, V., Marchand, N., Jaffrezo, J. L., Schwarzenboeck, A., Colomb, A., Wiedensohler, A., Borrmann, S., Lawrence, M., Baklanov, A., and Baltensperger, U.: In situ, satellite measurement and model evidence on the dominant regional contribution to fine particulate matter levels in the Paris megacity, Atmos. Chem. Phys., 15, 9577–9591, https://doi.org/10.5194/acp-15-9577-2015, 2015.
Bergström, R., Denier van der Gon, H. A. C., Prévôt, A. S. H., Yttri, K. E., and Simpson, D.: Modelling of organic aerosols over Europe (2002–2007) using a volatility basis set (VBS) framework: application of different assumptions regarding the formation of secondary organic aerosol, Atmos. Chem. Phys., 12, 8499–8527, https://doi.org/10.5194/acp-12-8499-2012, 2012.
Bessagnet, B., Beauchamp, M., Guerreiro, C., de Leeuw, F., Tsyro, S., Colette, A., Meleux, F., Rouïl, L., Ruyssenaars, P., Sauter, F., Velders, G. J. M., Foltescu, V. L., and van Aardenne, J.: Can further mitigation
of ammonia emissions reduce exceedances of particulate matter air quality
standards?, Environ. Sci. Policy, 44, 149–163,
https://doi.org/10.1016/j.envsci.2014.07.011, 2014.
Binkowski, F. and Shankar, U.: The Regional Particulate Matter Model. 1. Model description and preliminary results, J. Geophys. Res., 100, 26191–26209, 1995.
Blanchard, C. L. and Hidy, G. M.: Effects of Changes in Sulfate, Ammonia,and
Nitric Acid on Particulate Nitrate Concentrations in the South-eastern
United States, J. Air Waste Manage., 53, 283–290, 2003.
Carnevale, C., Pisoni, E., and Volta, M.: A non-linear analysis to detect
the origin of PM10 concentrations in Northern Italy, Sci. Total Environ., 409, 182–191, 2020.
Clappier, A., Thunis, P., Putaud, J. P., Beekmann, M., and De Meij, A.:
Analysis of the chemical regimes and non-linearity associated to PM2.5 in
Europe, Environment International, accepted, 2021.
de Meij, A., Krol, M., Dentener, F., Vignati, E., Cuvelier, C., and Thunis, P.: The sensitivity of aerosol in Europe to two different emission inventories and temporal distribution of emissions, Atmos. Chem. Phys., 6, 4287–4309, https://doi.org/10.5194/acp-6-4287-2006, 2006.
De Meij, A., Thunis, P., Bessagnet, B., and Cuvelier, C.: The sensitivity of
the CHIMERE model to emissions reduction scenarios on air quality in
Northern Italy, Atmos. Environ., 43, 1897–1907, 2009.
Dodge, M. C.: Effect of selected parameters on predictions of a
photochemical model, US Environmental Protection Agency, EPA-600/3-77/048,
Research Triangle Park, NC, USA, 1977.
Donahue, N. M., Robinson, A. L., and Pandis, S. N.: Atmospheric organic particulate matter: From smoke to secondary organic aerosol, Atmos. Environ., 43, 94–106, https://doi.org/10.1016/j.atmosenv.2008.09.055, 2009.
EDGAR: Emission Database for Global Atmospheric research,
available at: https://edgar.jrc.ec.europa.eu/ (last access: 25 November 2020), 2020.
EEA: Air quality in Europe — 2020 report, EEA Report No 11/2020, available at: https://www.eea.europa.eu/publications/air-quality-in-europe-2020-report (last access: 4 June 2021), 2020.
EMEP: Transboundary acidification and eutrophication and ground level
ozone in Europe: Unified EMEP model description, EMEP/MSC-W Report 1/2003, available at: https://emep.int/publ/reports/2003/emep_report_1_part1_2003.pdf (last access: 1 June 2021), 2003.
EMEP: EMEP/MSC-W Model – User's Guide July 2011, available at: https://wiki.met.no/_media/emep/page1/userguide_062011.pdf (last access: 1 June 2021), 2011.
Fagerli, H., Simpson, D., and Tsyro, S.: Unified EMEP model: Updates. In
EMEP Status Report 1/2004, Transboundary acidification, eutrophication and
ground level ozone in Europe. Status Report 1/2004, 11–18, The
Norwegian Meteorological Institute, Oslo, Norway, 2004.
Feng, T., Li, G., Cao, J., Bei, N., Shen, Z., Zhou, W., Liu, S., Zhang, T., Wang, Y., Huang, R.-J., Tie, X., and Molina, L. T.: Simulations of organic aerosol concentrations during springtime in the Guanzhong Basin, China, Atmos. Chem. Phys., 16, 10045–10061, https://doi.org/10.5194/acp-16-10045-2016, 2016.
Feng, T., Zhao, S., Bei, N., Wu, J., Liu, S., Li, X., Liu, L., Qian, Y., Yang, Q., Wang, Y., Zhou, W., Cao, J., and Li, G.: Secondary organic aerosol enhanced by increasing atmospheric oxidizing capacity in Beijing–Tianjin–Hebei (BTH), China, Atmos. Chem. Phys., 19, 7429–7443, https://doi.org/10.5194/acp-19-7429-2019, 2019.
Fu, X., Wang, S., Xing, J., Zhang, X., Wang, T., and Hao, J.: Increasing
Ammonia Concentrations Reduce the Effectiveness of Particle Pollution
Control Achieved via SO2 and NOx Emissions Reduction in East China, Environ.
Sci. Tech. Let., 4, 221–227, https://doi.org/10.1021/acs.estlett.7b00143,
2017.
Fu, X., Wang, T., Gao, J., Wang, P., Liu, Y., Wang, S., Zhao, B., and Xue, L.: Persistent Heavy
Winter Nitrate Pollution Driven by Increased Photochemical Oxidants in
Northern China, Environ. Sci. Technol., 54, 3881–3889, https://doi.org/10.1021/acs.est.9b07248, 2020.
Guo, H., Otjes, R., Schlag, P., Kiendler-Scharr, A., Nenes, A., and Weber, R. J.: Effectiveness of ammonia reduction on control of fine particle nitrate, Atmos. Chem. Phys., 18, 12241–12256, https://doi.org/10.5194/acp-18-12241-2018, 2018.
Hakimzadeh, M., Soleimanian, E., Mousavi, A., Borgini, A., De Marco, C., Ruprecht, A., and Sioutas, C.: The impact of biomass burning on the oxidative
potential of PM2.5 in the metropolitan area of Milan, Atmos.
Environ., 224, 117328, https://doi.org/10.1016/j.atmosenv.2020.117328, 2020.
Huang, L., Wang Q., Wang Y., Emery C., Zhu, A., Zhua, Y., Yin, S., and Yarwood, G., Zhang, K., and Lim, L.: Simulation of secondary organic aerosol over
the Yangtze River Delta region: The impacts from the emissions of
intermediate volatility organic compounds and the SOA modeling framework,
Atmos. Environ., 246, 118079, https://doi.org/10.1016/j.atmosenv.2020.118079, 2020.
Kenagy, H. S., Sparks, T. L., Ebben, C. J., Wooldrige, P. J., Lopez-Hilfiker, F. D., Lee, B. H., Thornton, J. A., McDuffie, E. E., Fibiger, D. L., Brown, S. S., Montzka, D. D., Weinheimer, A. J., Schroder, J. C., Campuzano-Jost, P., Day, D. A., Jimenez, J. L., Dibb, J. E., Campos, T., Shah, V., Jaeglé, L., and Cohen, R. C.: NOx lifetime and NOy partitioning
during WINTER, J. Geophys. Res.-Atmos., 123,
9813–9827, https://doi.org/10.1029/2018JD028736, 2018.
Kleinman, L. I.: Seasonal dependence of boundary layer peroxide
concentration: The low and high NOx regimes, J. Geophys. Res, 96,
20721–20733, 1991.
Kroll, J. H. and Seinfeld, J. H.: Chemistry of secondary organic aerosol:
Formation and evolution of low-volatility organics in the atmosphere,
Atmos. Environ., 42, 3593–3624, 2008.
Lachatre, M., Fortems-Cheiney, A., Foret, G., Siour, G., Dufour, G., Clarisse, L., Clerbaux, C., Coheur, P.-F., Van Damme, M., and Beekmann, M.: The unintended consequence of SO2 and NO2 regulations over China: increase of ammonia levels and impact on PM2.5 concentrations, Atmos. Chem. Phys., 19, 6701–6716, https://doi.org/10.5194/acp-19-6701-2019, 2019.
Larsen, B., Gilardoni, S., Stenström, K., Niedzialek, J., Jimenez, J.,
and Belis, C.: Sources for PM air pollution in the Po Plain, Italy: II.
Probabilistic uncertainty characterization and sensitivity analysis of
secondary and primary sources, Atmos. Environ., 50,
203–213, https://doi.org/10.1016/j.atmosenv.2011.12.038, 2012.
Le, T., Wang, Y., Liu, L., Yang, J., Yung, Y., Li, G., and Seinfeld, J.:
Unexpected air pollution with marked emission reductions during the COVID-19
outbreak in China, Science, 369, eabb7431, doi;10.1126/science.abb7431, 2020.
Leung, D., Shi, H., Zhao, B., Wang, J., Ding, E.M., Gu, Y., Zheng, H., Chen,
G., Liou, K. N., Wang, S., Fast, J. D., Zheng, G., Jiang, J., Li, X., and
Jiang, J. H.: Wintertime Particulate Matter Decrease Buffered by Unfavorable
Chemical Processes Despite Emissions Reductions in China, Geophys. Res. Lett., 47,
14, https://doi.org/10.1029/2020GL087721, 2020.
Li, G., Zavala, M., Lei, W., Tsimpidi, A. P., Karydis, V. A., Pandis, S. N., Canagaratna, M. R., and Molina, L. T.: Simulations of organic aerosol concentrations in Mexico City using the WRF-CHEM model during the MCMA-2006/MILAGRO campaign, Atmos. Chem. Phys., 11, 3789–3809, https://doi.org/10.5194/acp-11-3789-2011, 2011.
Logan, J. A.: An analysis of ozonesonde data for the troposhere: Recommendations for testing 3-D models and development of a gridded climatology for troposheric ozone, J. Geophys. Res., 10, 115–116, 1998.
Makar, P. A., Moran, M. D., Zheng, Q., Cousineau, S., Sassi, M., Duhamel, A., Besner, M., Davignon, D., Crevier, L.-P., and Bouchet, V. S.: Modelling the impacts of ammonia emissions reductions on North American air quality, Atmos. Chem. Phys., 9, 7183–7212, https://doi.org/10.5194/acp-9-7183-2009, 2009.
Nenes, A., Pandis, S. N., Weber, R. J., and Russell, A.: Aerosol pH and liquid water content determine when particulate matter is sensitive to ammonia and nitrate availability, Atmos. Chem. Phys., 20, 3249–3258, https://doi.org/10.5194/acp-20-3249-2020, 2020.
Norwegian Meteorological Institute (Met.no): Open Source EMEP/MSC-W model, available at: https://github.com/metno/emep-ctm, last access: 4 June 2021.
Pay, M. T., Jimenez-Guerrero, P., and Baldasano, J. M.: Assessing sensitivity
regimes of secondary inorganic aerosol formation in Europe with the
CALIOPE-EU modeling system, Atmos. Environ., 51, 146–164, 2012.
Pernigotti, D., Georgieva, E., Thunis, P., and Bessagnet, B: Impact of
meteorological modelling on air quality: Summer and winter episodes in the
Po valley (Northern Italy), Int. J. Envir. Poll., 50, 111–119, 2014.
Petetin, H., Sciare, J., Bressi, M., Gros, V., Rosso, A., Sanchez, O., Sarda-Estève, R., Petit, J.-E., and Beekmann, M.: Assessing the ammonium nitrate formation regime in the Paris megacity and its representation in the CHIMERE model, Atmos. Chem. Phys., 16, 10419–10440, https://doi.org/10.5194/acp-16-10419-2016, 2016.
Pinder, R. W., Gilliland, A. B., and Dennis, R. L.: Environmental impact of
atmospheric NH3 emissions under present and future conditions in the eastern
United States, Geophys. Res. Lett., 35, L12808, https://doi.org/10.1029/2008GL033732, 2008.
Pozzer, A., Tsimpidi, A. P., Karydis, V. A., de Meij, A., and Lelieveld, J.: Impact of agricultural emission reductions on fine-particulate matter and public health, Atmos. Chem. Phys., 17, 12813–12826, https://doi.org/10.5194/acp-17-12813-2017, 2017.
Putaud, J.-P., Pozzoli, L., Pisoni, E., Martins Dos Santos, S., Lagler, F., Lanzani, G., Dal Santo, U., and Colette, A.: Impacts of the COVID-19 lockdown on air pollution at regional and urban background sites in northern Italy, Atmos. Chem. Phys., 21, 7597–7609, https://doi.org/10.5194/acp-21-7597-2021, 2021.
Raffaelli, K., Deserti, M., Stortini, M., Amorati, R., Vasconi, M., and Giovannini, G.: Improving Air Quality in the Po Valley, Italy: Some Results
by the LIFE-IP-PREPAIR Project, Atmosphere, 11, 429, https://doi.org/10.3390/atmos11040429, 2020.
Ricciardelli, I., Bacco D., Rinaldi M., Bonafe G., Scotto F., Trentini, A., Bertacci, G., Ugolini, P., Zigola, C., Rovere, F., Maccone, C., Pironi, C., and Poluzzi, V.: A three-year investigation of daily PM2.5 main
chemical components in four sites: the routine measurement program of the
Supersito Project (Po Valley, Italy), Atmos. Environ., 152, 418e430, https://doi.org/10.1016/J.ATMOSENV.2016.12.052, 2017.
Robinson, A. L., Donahue, N. M., Shrivastava, M. K., Weitkamp, E. A., Sage, A. M., Grieshop, A. P., Lane, T. E., Pierce, J. R., and Pandis, S. N.: Rethinking Organic Aerosols: Semivolatile Emissions and Photochemical Aging, Science, 315, 1259–1262, https://doi.org/10.1126/science.1133061, 2007.
Seinfeld, J. H. and Pandis, S. N.: Atmospheric Chemistry and Physics: From
Air Pollution to Global Change, 2nd edn., J. Wiley and Sons, New York, 2006.
Shah, V., Jaeglé, L., Thornton, J. A., Lopez-Hilfiker, F. D., Lee, B. H., Schroder, J. C., Campuzano-Jost, P., Jimenez, J. L., Guo, H., Sullivan, A. P., Weber, R. J., Green, J. R., Fiddler, M. N., Bililign, S., Campos, T. L., Stell, M., Weinheimer, A. J., Montzka, D. D., and Brown, S. S.: Chemical feedbacks weaken
the wintertime response of particulate sulfate and nitrate to emissions
reductions over the eastern United States, P. Natl. Acad. Sci. USA, 115, 8110–8115, https://doi.org/10.1073/pnas.1803295115, 2018.
Sheng, F., Jingjing, L., Yu., C., Fu-Ming, T., Xuemei, D., and Jing-yao, L.:
Theoretical study of the oxidation reactions of sulfurous acid/sulfite with
ozone to produce sulfuric acid/sulfate with atmospheric implications, RSC
Advances, 8, 7988–7996, https://doi.org/10.1039/C8RA00411K, 2018.
Shrivastava, M., Cappa, C. D., Fan, J., Goldstein, A. H., Guenther, A. B., Jimenez, J. L., Kuang, C., Laskin, A., Martin, S. T., Ng, N. L., Petaja, T., Pierce, J. R., Rasch, P. J., Roldin, P., Seinfeld, J. H., Shilling, J., Smith, J. N., Thornton, J. A., Volkamer, R., Wang, J., Worsnop, D. R., Zaveri, R. A., Zelenyuk, A., and Zhang, Q.: Recent advances in understanding secondary organic
aerosol: Implications for global climate forcing, Rev. Geophys.,
55, 509–559, https://doi.org/10.1002/2016RG000540, 2017.
Simpson, D., Fagerli, H., Jonson, J. E., Tsyro, S., Wind, P., and Tuovinen,
J. P.: The EMEP Unified Eulerian Model. Model Description, EMEP MSC-W Report
1/2003, The Norwegian Meteorological Institute, Oslo, Norway, 2003.
Simpson, D., Benedictow, A., Berge, H., Bergström, R., Emberson, L. D., Fagerli, H., Flechard, C. R., Hayman, G. D., Gauss, M., Jonson, J. E., Jenkin, M. E., Nyíri, A., Richter, C., Semeena, V. S., Tsyro, S., Tuovinen, J.-P., Valdebenito, Á., and Wind, P.: The EMEP MSC-W chemical transport model – technical description, Atmos. Chem. Phys., 12, 7825–7865, https://doi.org/10.5194/acp-12-7825-2012, 2012.
Stein, U. and Alpert, P.: Factor separation in numerical simulations, J.
Atmos. Sci., 50, 2107–2115, 1993.
Thunis, P. and Clappier, A.: Indicators to support the dynamic evaluation
of air quality models, Atmos. Environ., 98, 402–409, 2014.
Thunis, P., Pernigotti, D., Cuvelier, C., Georgieva, E., Gsella, A., De
Meij, A., Pirovano, G., Balzarini, A., Riva, G. M., Carnevale, C., Pisoni,
E., Volta, M., Bessagnet, B., Kerschbaumer, A.,Viaene, P., De Ridder, K.,
Nyiri, A., and Wind, P.: POMI: A Model Intercomparison exercise over the Po
valley, Air Qual. Atmos. Hlth, 6, 701–715, https://doi.org/10.1007/s11869-013-0211-1,
2013.
Thunis, P., Clappier, A., Pisoni, E., and Degraeuwe, B.: Quantification of
non-linearities as a function of time averaging in regional air quality
modeling applications, Atmos. Environ., 103, 263–275, 2015.
Tsigaridis, K., Daskalakis, N., Kanakidou, M., Adams, P. J., Artaxo, P., Bahadur, R., Balkanski, Y., Bauer, S. E., Bellouin, N., Benedetti, A., Bergman, T., Berntsen, T. K., Beukes, J. P., Bian, H., Carslaw, K. S., Chin, M., Curci, G., Diehl, T., Easter, R. C., Ghan, S. J., Gong, S. L., Hodzic, A., Hoyle, C. R., Iversen, T., Jathar, S., Jimenez, J. L., Kaiser, J. W., Kirkevåg, A., Koch, D., Kokkola, H., Lee, Y. H., Lin, G., Liu, X., Luo, G., Ma, X., Mann, G. W., Mihalopoulos, N., Morcrette, J.-J., Müller, J.-F., Myhre, G., Myriokefalitakis, S., Ng, N. L., O'Donnell, D., Penner, J. E., Pozzoli, L., Pringle, K. J., Russell, L. M., Schulz, M., Sciare, J., Seland, Ø., Shindell, D. T., Sillman, S., Skeie, R. B., Spracklen, D., Stavrakou, T., Steenrod, S. D., Takemura, T., Tiitta, P., Tilmes, S., Tost, H., van Noije, T., van Zyl, P. G., von Salzen, K., Yu, F., Wang, Z., Wang, Z., Zaveri, R. A., Zhang, H., Zhang, K., Zhang, Q., and Zhang, X.: The AeroCom evaluation and intercomparison of organic aerosol in global models, Atmos. Chem. Phys., 14, 10845–10895, https://doi.org/10.5194/acp-14-10845-2014, 2014.
Tsimpidi, A. P., Karydis, V. A., Zavala, M., Lei, W., Molina, L., Ulbrich, I. M., Jimenez, J. L., and Pandis, S. N.: Evaluation of the volatility basis-set approach for the simulation of organic aerosol formation in the Mexico City metropolitan area, Atmos. Chem. Phys., 10, 525–546, https://doi.org/10.5194/acp-10-525-2010, 2010.
Tsimpidi, A. P., Karydis, V. A., Pandis, S. N., and Lelieveld, J.: Global combustion sources of organic aerosols: model comparison with 84 AMS factor-analysis data sets, Atmos. Chem. Phys., 16, 8939–8962, https://doi.org/10.5194/acp-16-8939-2016, 2016.
Vahedpour, M., Goodarzi, M., Hajari, N., and Nazari, F.: Struct. Chem., 22,
817—822, 2011.
Watson, J. G., Chow, J. C., Lurmann, F. W., and Musarra, S. P.: Ammonium
Nitrate, Nitric Acid, and Ammonia Equilibrium in Wintertime Phoenix,
Arizona, Air & Waste, 44, 405–412, https://doi.org/10.1080/1073161X.1994.10467262, 1994.
Womack, C. C., McDuffie, E. E., Edwards, P. M., Bares, R., de Gouw, J. A.,
Docherty, K. S., Dube, W. P., Fibiger, D. L., Franchin, A., Gilman, J. B.,
Goldberger, L., Lee, B. H., Lin, J. C., Long, R., Middlebrook, A. M.,
Millet, D. B., Moravek, A., Murphy, J. G., Quinn, P. K., Riedel, T. P.,
Roberts, J. M., Thornton, J. A., Valin, L. C., Veres, P. R., Whitehill, A.
R., Wild, R. J., Warneke, C., Yuan, B., Baasandorj, M., and Brown, S. S.: An
odd oxygen framework for wintertime ammonium nitrate aerosol pollution in
urban areas: NOx and VOC control as mitigation strategies, Geophys. Res.
Lett., 46, 4971–4979,
https://doi.org/10.1029/2019GL082028, 2019.
Xing, J., Ding, D., Wang, S., Zhao, B., Jang, C., Wu, W., Zhang, F., Zhu, Y., and Hao, J.: Quantification of the enhanced effectiveness of NOx control from simultaneous reductions of VOC and NH3 for reducing air pollution in the Beijing–Tianjin–Hebei region, China, Atmos. Chem. Phys., 18, 7799–7814, https://doi.org/10.5194/acp-18-7799-2018, 2018.
Short summary
Modelling simulations are used to identify the most efficient emission reduction strategies to reduce PM2.5 concentration levels in northern Italy. Results show contrasting chemical regimes and important non-linearities during wintertime, with the striking result that PM2.5 levels may increase when NOx reductions are applied in NOx-rich areas – a process that may have contributed to the absence of significant PM2.5 decrease during the COVID-19 lockdowns in many European cities.
Modelling simulations are used to identify the most efficient emission reduction strategies to...
Altmetrics
Final-revised paper
Preprint