Modeling of the Atmospheric Dispersion of Heavy Metals Over Poland Janusz Zysk
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Modeling of the atmospheric dispersion of heavy metals over Poland Janusz Zysk To cite this version: Janusz Zysk. Modeling of the atmospheric dispersion of heavy metals over Poland. Ocean, Atmo- sphere. Université Paris-Est, 2016. English. NNT : 2016PESC1169. tel-01539576 HAL Id: tel-01539576 https://pastel.archives-ouvertes.fr/tel-01539576 Submitted on 15 Jun 2017 HAL is a multi-disciplinary open access L’archive ouverte pluridisciplinaire HAL, est archive for the deposit and dissemination of sci- destinée au dépôt et à la diffusion de documents entific research documents, whether they are pub- scientifiques de niveau recherche, publiés ou non, lished or not. The documents may come from émanant des établissements d’enseignement et de teaching and research institutions in France or recherche français ou étrangers, des laboratoires abroad, or from public or private research centers. publics ou privés. AGH University of Science and Technology University Paris-Est Faculty of Energy and Fuels Ecole des Ponts ParisTech Department of Sustainable Energy Centre d'Enseignement et de Development Recherche en Environnement Atmosphérique DOCTORAL THESIS Mgr inż. Janusz Zyśk Fields of study: Chemical Technology at Faculty of Energy and Fuels, Science and technology of the environment at École des Ponts ParisTech Modelling of atmospheric transport of heavy metals emitted from Polish power sector Date of defence 30-06-2016 Supervisors: Prof. dr hab. Janusz Gołaś Professor Christian Seigneur Ph.D., hab. Auxiliary supervisor: Yelva Roustan Ph.D. Kraków, 2016 Oświadczam, świadomy (-a) odpowiedzialności karnej za poświadczenie nieprawdy, że niniejszą pracę doktorską wykonałem (-am) osobiście i samodzielnie i że nie korzystałem (-am) ze źródeł innych niż wymienione w pracy. …………………………………………………… podpis autora pracy 2 Content 1 Introduction ........................................................................................................................ 6 PART I Review of the literature of the cycle of heavy metals in the environment ................. 11 2 Heavy metals in the environment ..................................................................................... 12 2.1 Global cycle of heavy metals..................................................................................... 12 2.2 Heavy metals emissions into the atmosphere ............................................................ 14 2.2.1 Natural emissions of heavy metals ..................................................................... 14 2.2.2 Anthropogenic emission of mercury into the air ................................................ 17 2.2.3 Emissions of mercury from coal combustion in the power sector ..................... 26 2.2.4 Anthropogenic emission of lead and cadmium into the air ................................ 30 2.3 Reactions of mercury in the atmospheric gas phase .................................................. 33 2.4 Reactions of mercury in the aqueous phase of the atmosphere ................................. 44 2.5 Mercury transformation in presence of aerosol particles .......................................... 49 2.6 Measurements of deposition and concentration of heavy metals .............................. 50 3 Overview of existing mercury chemical transport models ............................................... 57 4 Polyphemus air quality system ......................................................................................... 67 4.1 Below-cloud scavenging model implemented in the Polyphemus system ................ 69 4.2 Dry deposition models implemented in the Polyphemus system .............................. 73 4.2.1 Dry deposition for gaseous species .................................................................... 73 4.2.2 Dry deposition velocity for aerosols................................................................... 79 PART II Development and application of a new chemical transport model for mercury, modelling of atmospheric transport of lead and cadmium ....................................................... 81 5 Distribution of the emissions of heavy metals into the air by the Polish power sector with the use of the bottom-up approach ........................................................................................... 82 5.1 Methodology .............................................................................................................. 82 5.2 Results........................................................................................................................ 84 5.3 Implemented chemical scheme of atmospheric mercury........................................... 86 5.3.1 In-cloud scavenging............................................................................................ 96 6 Simulation setting ............................................................................................................. 98 6.1 Domains of simulation............................................................................................... 98 6.2 Input data ................................................................................................................... 99 6.2.1 Land use data ...................................................................................................... 99 6.2.2 Meteorological data ............................................................................................ 99 6.2.3 Boundary and initial concentrations ................................................................... 99 6.2.4 Concentrations of species that react with mercury ........................................... 100 6.2.5 Natural emissions ............................................................................................. 101 6.2.6 Anthropogenic emissions, simulations over Europe ........................................ 103 3 6.2.7 Anthropogenic emissions, simulation over Poland .......................................... 106 7 Results ............................................................................................................................ 109 7.1 Evaluation of intensity of precipitation ................................................................... 111 7.2 Dry deposition velocity for mercury species ........................................................... 112 7.3 Results and evaluation of concentrations of species that react with mercury ......... 114 7.4 Evaluation of mercury concentrations and deposition............................................. 124 7.5 Evaluation of cadmium and lead ambient concentrations and deposition............... 132 7.6 Results of ambient concentrations and deposition of mercury ................................ 135 7.7 Results of ambient concentrations and deposition of cadmium and lead ................ 142 7.8 Sensitivity analysis of the mercury model ............................................................... 144 7.9 Contribution of different sources to mercury deposition in Poland ........................ 156 7.10 The impact of the Polish power sector ................................................................. 157 8 Conclusions .................................................................................................................... 162 References .......................................................................................................................... 167 List of Tables ...................................................................................................................... 183 List of Figures..................................................................................................................... 187 Appendix 1 ......................................................................................................................... 194 4 Acknowledgements I would like to express my gratitude to Professors Janusz Gołaś and Christan Seignerur for their guidance as the supervisors of my Thesis. Thank you for helpful discussions and professional advice during my work on this Thesis. I would like to express my special appreciation and thanks to Dr. Yelva Roustan, you have been a tremendous mentor for me. I would like to thank you for encouraging my research and for allowing me to grow as a research scientist. I am greatly indebted to Dr. Artur Wyrwa for introducing me into the fascinating world of science. Your advice on both research as well as on my career has been priceless. I would also like to thank Professors Louis Jestin, Bruno Sporitsse, Luc Musson-Genon, Wojciech Suwała, Denis Quelo, Mariusz Filipowicz for their kindness, helpful and professional advice. I would like express my appreciation to the late professors Piotr Tomczyk and Adam Guła, who always surrounded me with unusual kindness. 5 1 Introduction During the last decades many studies have been conducted to investigate the atmospheric heavy metals contamination and its deposition to ecosystems. The increasing attention to mercury pollution has been mainly driven by the growing evidence of its negative impacts on wildlife, ecosystems and particularly human health. It should be noted, that after mercury moves through the water chain it can be transformed by aquatic microorganisms into methylmercury (MeHg), which is much more toxic than the other forms. Subsequently, MeHg is bioaccumulated in fish and seafood [1]. The predator fish can contain almost 100% of mercury in methylmercury form. Eventually, it enters the human body with consumed food. It is then transported by blood and can easily pass