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PhD-FSTC-2013-03 The Faculty of Sciences, Technology and Communication DISSERTATION Defense held on 28/01/2013 in Luxembourg to obtain the degree of DOCTEUR DE L’UNIVERSITÉ DU LUXEMBOURG EN SCIENCES DE L’INGÉNIEUR by Lara ALELUIA DA SILVA REIS Born on 06 October 1984 in Agualva-Cacém Sintra (Portugal) ∗ Development and Application of an Asymptotic Level Transport Pollution Model for Luxembourg Energy Air Quality Project Dissertation defense committee Dr. Bernhard Peters, dissertation supervisor Professor, Université du Luxembourg Dr. Daniel Zachary R&D Manager, CRP Henri Tudor Dr. Geoffrey Caruso, Chairman Professor, Université du Luxembourg Dr. Dimitrios Melas Professor, Aristotle University of Thessaloniki Dr. Ulf Janicke Executive, Janicke Consulting Abstract The connections between air pollution and the increase of respiratory diseases, are well known. In Europe, many efforts have been carried out towards the mitigation of the pollutants’ emissions over the last decades. However the ambient levels of some air pollutants, is still worrisome and a large part of the European population is still exposed to high levels pollution. The European Union supports the implementation of structural planning measures to control air pollution. The assessment and evaluation of these air quality policies must be carried out with the help of dedicated integrated assessment models. The use of integrated assessment models, which combine models from different fields, raises the need for developing specific modelling concepts in order to provide results to support policy decisions within a practi- cal time frame. Integrated assessment models for air policy relate technologies, the emitting sources, with air quality levels. Existing photochemical air qual- ity models are not directly suitable for integrated approaches as they are time intensive in terms of input preparation and simulation speed. This work presents the methodology and the development of a dedicated air quality model for an integrated assessment model. This approach has been designed for the Luxembourg Energy and Air Quality, LEAQ, integrated as- sessment model. It combines an air quality model, AUSTAL2000-AYLTP, with a techno-economic model, ETEM, which computes ozone precursors emissions related to energy consumption. The models are coupled via an optimization engine, which minimizes the total energy cost for a given ozone level. AUSTAL2000, a Lagrangian transport model, has been adapted to receive a photochemical module, the AsYmptotic Level Transport Pollution, AYLTP. This module consists of a Look-Up Table of quasi-linear reaction rates. The AUSTAL2000 model inquires the look-up table for pre-calculated initial condi- tions, and it reads the correspondent rate that is then used by AUSTAL2000. The look-up table has been built using a box model by simulating a large set of possible combinations of meteorological variables and precursor concen- trations. A balance has been found that gives an acceptable level of accu- racy, given the reduction of computational time. The development of such methodologies is important when considering integrated assessment models. Furthermore, the results of the air quality model have been compared with measurements, and with the regional model LOTOS-EUROS. The results of the validation are considered satisfactory for this type of approach. Addition- ally, the air quality model has been used within the in LEAQ model. Two study cases have been simulated, one including only the national emissions 2 from Luxembourg country, and a second one for the Luxembourg region, in- cluding the neighbouring countries emissions. The use of quasi-linear reaction rates obtained with the help of the look-up table represents an innovative step towards the use of simplified air quality models that involve complex chemistry. Acknowledgements First, I would like to acknowledge that this work would have not been possible, without the guidance of my committee members and the support of my family and friends. I would like to express my gratitude and recognition to my scientific advi- sor, Dr. Daniel Zachary who has proposed this research topic and has patiently guided my work throughout these four years, also for having raised my inter- est in integrated assessment approaches, and for being always supportive. I would, equally, like to acknowledge the help of Professor Bernhard Peters, my principal supervisor, for his guidance and advice during my Ph.D. studies, and also for the thesis management support. I am grateful to Professor Geoffrey Caruso, for the help in shaping this thesis work and for his constructive com- ments and encouragement. To professor Dimitrios Melas for having kindly received me as a guest student in his research group, for always providing a good and constructive advice, I express my gratitude. This thesis would not have been possible without the promptly answers of Dr. Ulf Janicke, to whom I thank for his patience to help me with the theoretical and technical details of the AUSTAL2000 model. I acknowledge the FNR - Fonds National de la Recherche Luxembourg for the grant founding, AFR - Aide a la Formation-Recherche, under the grant identifier PHD-08-004. My gratitude goes, also, to all the colleagues who have participated in the Luxembourg Energy Air Quality (LEAQ) project. Namely to Oliver O’Nagy and Guy Kneip for their contribution to the energy database. To Christian Braun for having introduced me to GRASS GIS and the restless help when- ever some technical support was needed. To Ulrich Leopold, for being a nice company and for making me an open-source software fan, and to his wife, El- bia who always had good Brazilian food to comfort me. To Laurent Drouet, my colleague, my friend, my mentor and my life partner, for his work on the Energy-Technology-Environment Model (ETEM), without whom the LEAQ project and this thesis would have not been possible, and for his patience, ideas and suggestions my deep and sincere “Merci”. I thank all the people I have met in Resource Centre for Environmental Technologies (CRTE), especially Bianca Schmit for all the support and trust that she conceded me. A big thank you to all the people who have inhabited the “Robert’s” office, for the nice coffee breaks and lunches we had together. I am grateful to Dr. Anastasia Poupkou from the Aristotle University of Thessaloniki, for the help with the biogenic Volatile Organic Compounds (VOC) data, and the good modelling advices. To Kostas Markakis for his help 4 with the temporal emissions’ profiles for Luxembourg, to Eleni Katragkou and Zoi Hristodoulou for having welcomed me and taken care of me in Thessa- loniki, to Spiros Dimopoulos and Theodoros Giannaros my nice officemates and to all the people at the laboratory of Atmospheric Physics of the Aristotle University of Thessalonik I express my honest “euqarist¸ poλύ’΄. I wish to thank professor Sergio Corrêa from the University of the State of Rio de Janeiro, for his help with OZIPR model. I acknowledge the help of Dr. Renske Timmermans for providing the LOTOS-EUROS data results, and for the constructive comments and suggestions on chapter 7 and Dr. Kumar Kannan for the help with OpenFOAM. Obviously, friends could not be forgotten. I thank all my friends in Portu- gal, who always send nice e-mails from time to time asking “Have you finished yet?”, and always had a little time for me whenever I was back in town. To all the nice people I have met in Luxembourg, who have made my days brighter and my weekends funnier, I dedicate a huge “villmols merci” to you all. Finally, I express my profound gratitude, admiration and affection to my extraordinary family. To my mother Maria Teresa and my brother André Silva Reis a big thank you for your never-ending patience, support and for always finding the best words to comfort me. To my grandmother Natalia who I am sure has always sent me positive thoughts, I express my “muito obrigada”. To my father, António Heitor Reis who is my idol and my hero, for all the help, patience, support and for his hints and suggestions, I express my sincere gratitude. Contents 1 Introduction1 1.1 Motivation and Objectives . .1 1.2 Thesis Outline . .5 2 Background7 2.1 Air Quality — A Major Concern . .7 2.2 Air Quality Integrated Assessment Models . 13 2.3 Energy-Economic Models . 19 2.4 Air Quality Models . 22 2.4.1 Classification of Air Quality Models . 25 2.5 Emission Reduction Instruments . 32 3 The Energy - Air Quality Integrated Assessment Model 37 3.1 Objectives and Concept . 37 3.2 The LEAQ Structure . 39 3.2.1 The ETEM - Techno-Economic Model . 41 3.2.2 Emission Allocator Module . 47 3.2.3 Oracle Based Optimisation Engine . 51 3.2.4 The Air Quality Model - AUSTAL2000-AYLTP . 55 4 The Air Quality Model 65 4.1 Model Concept . 66 4.2 Lagrangian Representation . 66 4.3 Transport Algorithm . 68 4.4 Concentration and Dry Deposition . 71 4.4.1 Turbulence . 73 4.4.2 Diagnostic Wind Field . 81 5 Ozone Photochemistry 83 5.1 Quasi-Linear Production Rates . 86 5.2 OZIPR — Calculation of The Look-up Tables . 90 5.2.1 Chemical Mechanism: CB-IV . 91 5.2.2 The VOC’s Speciation for Luxembourg . 91 6 CONTENTS 5.2.3 Analysis of the OZIPR model results . 92 5.3 Characteristics of the Look-up table . 98 5.3.1 The Relations Between the Look-up Table (LUT) Vari- ables and the Production Rates . 100 5.3.2 Relations Between the LUT Meteorological Variables and the Production Rates . 102 6 Validation of the Air Quality Model 105 6.1 Modelling Application . 105 6.1.1 Modelling Domain . 109 6.1.2 Meteorology . 110 6.1.3 Emissions . 111 6.2 AUSTAL2000-AYLTP Results . 114 6.3 Model Evaluation . 120 6.3.1 Qualitative Evaluation .

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