Articles | Volume 17, issue 4
Atmos. Chem. Phys., 17, 2817–2838, 2017
Atmos. Chem. Phys., 17, 2817–2838, 2017

Research article 23 Feb 2017

Research article | 23 Feb 2017

Phenomenology of high-ozone episodes in NE Spain

Xavier Querol1, Gotzon Gangoiti2, Enrique Mantilla3, Andrés Alastuey1, Maria Cruz Minguillón1, Fulvio Amato1, Cristina Reche1, Mar Viana1, Teresa Moreno1, Angeliki Karanasiou1, Ioar Rivas1, Noemí Pérez1, Anna Ripoll1, Mariola Brines1, Marina Ealo1, Marco Pandolfi1, Hong-Ku Lee4, Hee-Ram Eun4, Yong-Hee Park4, Miguel Escudero5, David Beddows6, Roy M. Harrison6,a, Amelie Bertrand7, Nicolas Marchand7, Andrei Lyasota8,†, Bernat Codina8, Miriam Olid8, Mireia Udina8, Bernat Jiménez-Esteve8, María R. Soler8, Lucio Alonso2, Millán Millán3, and Kang-Ho Ahn4 Xavier Querol et al.
  • 1Institute of Environmental Assessment and Water Research, IDAEA-CSIC, C/Jordi Girona 18–26, 08034 Barcelona, Spain
  • 2Escuela Técnica Superior Ingeniería de Bilbao, Departamento Ingeniería Química y del Medio Ambiente, Universidad del País Vasco UPV/EHU, Urkixo Zumarkalea, S/N, 48013 Bilbao, Spain
  • 3Centro de Estudios Ambientales del Mediterráneo, CEAM, Unidad Asociada al CSIC, Parque Tecnológico C/Charles R. Darwin, 14 46980 Paterna, Valencia, Spain
  • 4Department of Mechanical Engineering, Hanyang University, Ansan 425-791, Republic of Korea
  • 5Centro Universitario de la Defensa de Zaragoza, Academia General Militar, Ctra. de Huesca s/n, 50090 Zaragoza, Spain
  • 6Division of Environmental Health & Risk Management, School of Geography, Earth & Environmental Sciences, University of Birmingham, Edgbaston, Birmingham B15 2TT, UK
  • 7Aix Marseille Univ, CNRS, LCE, 13331 Marseille, France
  • 8Department of Astronomy and Meteorology, Faculty of Physics, University of Barcelona, Martí I Franquès 1, 08028 Barcelona, Spain
  • aalso at: Department of Environmental Sciences/Centre for Excellence in Environmental Studies, King Abdulaziz University, Jeddah, Saudi Arabia
  • deceased

Abstract. Ground-level and vertical measurements (performed using tethered and non-tethered balloons), coupled with modelling, of ozone (O3), other gaseous pollutants (NO, NO2, CO, SO2) and aerosols were carried out in the plains (Vic Plain) and valleys of the northern region of the Barcelona metropolitan area (BMA) in July 2015, an area typically recording the highest O3 episodes in Spain. Our results suggest that these very high O3 episodes were originated by three main contributions: (i) the surface fumigation from high O3 reservoir layers located at 1500–3000 m a.g.l. (according to modelling and non-tethered balloon measurements), and originated during the previous day(s) injections of polluted air masses at high altitude; (ii) local/regional photochemical production and transport (at lower heights) from the BMA and the surrounding coastal settlements, into the inland valleys; and (iii) external (to the study area) contributions of both O3 and precursors. These processes gave rise to maximal O3 levels in the inland plains and valleys northwards from the BMA when compared to the higher mountain sites. Thus, a maximum O3 concentration was observed within the lower tropospheric layer, characterised by an upward increase of O3 and black carbon (BC) up to around 100–200 m a.g.l. (reaching up to 300 µg m−3 of O3 as a 10 s average), followed by a decrease of both pollutants at higher altitudes, where BC and O3 concentrations alternate in layers with parallel variations, probably as a consequence of the atmospheric transport from the BMA and the return flows (to the sea) of strata injected at certain heights the previous day(s). At the highest altitudes reached in this study with the tethered balloons (900–1000 m a.g.l.) during the campaign, BC and O3 were often anti-correlated or unrelated, possibly due to a prevailing regional or even hemispheric contribution of O3 at those altitudes. In the central hours of the days a homogeneous O3 distribution was evidenced for the lowest 1 km of the atmosphere, although probably important variations could be expected at higher levels, where the high O3 return strata are injected according to the modelling results and non-tethered balloon data.

Relatively low concentrations of ultrafine particles (UFPs) were found during the study, and nucleation episodes were only detected in the boundary layer.

Two types of O3 episodes were identified: type A with major exceedances of the O3 information threshold (180 µg m−3 on an hourly basis) caused by a clear daily concatenation of local/regional production with accumulation (at upper levels), fumigation and direct transport from the BMA (closed circulation); and type B with regional O3 production without major recirculation (or fumigation) of the polluted BMA/regional air masses (open circulation), and relatively lower O3 levels, but still exceeding the 8 h averaged health target.

To implement potential O3 control and abatement strategies two major key tasks are proposed: (i) meteorological forecasting, from June to August, to predict recirculation episodes so that NOx and VOC abatement measures can be applied before these episodes start; (ii) sensitivity analysis with high-resolution modelling to evaluate the effectiveness of these potential abatement measures of precursors for O3 reduction.

Short summary
High summer O3 episodes in NE Spain were analysed. We evidence the relevance of local emission of precursors in meteorological scenarios of vertical air mass recirculations, when transboundary contributions are also significant. Forecasting these scenarios and sensitivity analysis of possible O3 precursors drop are key for potential abatement strategies. However, this is a very difficult task due to the complexity of scenarios, the external contributions, and the complex O3 production reactions.
Final-revised paper