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These De Doctorat De THESE DE DOCTORAT DE L’ECOLE NATIONALE SUPERIEURE DE CHIMIE RENNES COMUE UNIVERSITE BRETAGNE LOIRE ECOLE DOCTORALE N ° 596 Matière, Molécules, Matériaux Spécialité : « Chimie, Procédés, Environnement » Par Margaux LHUISSIER Éco-procédé de traitement de COV et de valorisation d’huiles de collecte Thèse présentée et soutenue à Rennes, le 3 juillet 2019 Unité de recherche : Équipe Chimie et Ingénierie des Procédés, UMR CNRS 6226 ISCR Thèse N° : ENSCR_0056 Rapporteurs avant soutenance : Sophie Fourmentin Professeur, Université du Littoral Côte d'Opale Eric Dumont Maître de conférences HDR, Université de Nantes Composition du Jury : Président : Nicolas Roche Professeur, Université d’Aix-Marseille Examinateurs : Abdeltif Amrane Professeur, Université de Rennes 1 / Co-encadrant de la thèse Abdoulaye Kane Enseignant-Chercheur, UniLaSalle-EME / Co-encadrant de la thèse Florent Mancini Directeur de site, Groupe Chimirec Dir. de thèse : Annabelle Couvert Professeur, Ecole Nationale Supérieure de Chimie de Rennes Co-dir. de thèse : Jean-Luc Audic Maître de conférences HDR, Université de Rennes 1 Invités Anthony Caillibot Technicien de laboratoire, Groupe Chimirec Jérôme Normand Directeur adjoint, Groupe Chimirec « C'est une véritable révolution, métamorphose, mutation, que nous devons engager. Les mesures isolées qui ne repenseraient pas l'organisation de nos sociétés en profondeur [...] n'ont pas de sens, nous devons désormais réfléchir de façon globale, tenant compte de l'interdépendance de tous les systèmes. Nous avons besoin de réinventer totalement nos modèles économiques, agricoles, énergétiques, éducatifs, notre organisation démocratique... » [Cyril Dion] Remerciements L’aventure d’une thèse demande beaucoup d’autonomie et d’investissement personnel de la part d’un doctorant mais n’est pas possible sans l’aide et la bienveillance de son entourage dans les cadres scientifique ou personnel. Tout d’abord, j’aimerais remercier mon co-directeur de thèse et mes encadrants : Jean-Luc Audic, Abdoulaye Kane et Abdeltif Amrane pour leur aide dans chacun de leurs domaines, leur bienveillance et leur pouvoir de dédramatisation dans les moments plus difficiles. Je voudrais tout particulièrement remercier ma directrice de thèse Annabelle Couvert pour sa présence, son immense soutien, sa disponibilité et sa sérénité. Nos discussions m’ont permis de prendre du recul sur mon travail et d’avancer plus sereinement et surtout de garder le cap et le moral. J’ai beaucoup appris, cette expérience enrichie de vos conseils a été très formatrice. Je souhaite également remercier le Groupe Chimirec de m’avoir fait confiance pour ce projet de recherche et particulièrement Florent Mancini, responsable scientifique du projet, Philippe Merleix, directeur et Jérôme Normand, directeur adjoint. Merci à Pierre-François Biard et Sylvain Giraudet pour leur aide dans la réalisation d’articles et d’essais au laboratoire et merci aux stagiaires ayant travaillé avec moi. Je remercie également Isabelle Soutrel, Pierre Largillière, Valérie Courousse, Christelle Gardin et Apolline Lalande qui me sont venus en aide de nombreuses fois et m’ont permis de réaliser mes manipulations au laboratoire. J’ai aussi passé de bons moments avec les personnes présentes au CIP lors de ma thèse dans une ambiance studieuse et conviviale : Lucie T, Nina, Kamagaté, Kheir-Eddine, Wala, Ni, Pacôme, Simon, Lucie L, Audrey. Mon expérience à Chimirec m’a permis d’apprendre beaucoup de choses aux niveaux technique et humain. Je tiens à remercier particulièrement les maintenanciers du site de Chimirec Javené et particulièrement Arnaud et Sylvain. Nous avons passé de longues heures sur l’installation pilote pour pouvoir la faire fonctionner avec de nombreuses embûches, ces moments ont été très enrichissants. Merci à mes collègues géniaux qui m’ont donné le sourire dès le matin et particulièrement Nathalie, Linda et Alan. Merci à mes merveilleux amis qui m’ont permis de m’évader pendant les week-ends et vacances et qui répondent toujours présent : mes amis de promo, de prépa et d’ingé et mes mayennais chéris. Certains moments ont pu être difficiles mais nous les avons surmontés avec optimisme, votre amitié est si précieuse. Je n’ai pas souvent l’occasion de le faire, merci à ma famille pour leur amour inconditionnel. Mes parents m’ont toujours encouragée et soutenue dans mes choix professionnels, je leur dois beaucoup. Merci à ma sœur Clara et à mon frère Mathieu. Merci à mon Anthony pour sa douceur, sa force et son intelligence. J’aimerais dédier ce travail mon amie Marielle. Sommaire Glossaire ________________________________________________________________________ I Nomenclature _______________________________________________________________________ I Lettres grecques ____________________________________________________________________ II Nombres adimensionnels _____________________________________________________________ II Indices et exposants _________________________________________________________________ III Abréviations _______________________________________________________________________ III Liste des figures __________________________________________________________________V Liste des tableaux _______________________________________________________________ VIII Introduction générale __________________________________________________ 1 Chapitre 1. Les Composés Organiques Volatils ______________________________ 3 1. Définition ___________________________________________________________________ 5 2. Sources d’émission ____________________________________________________________ 5 3. Effets sur l’Homme et l’environnement ____________________________________________ 6 3.1. Environnement________________________________________________________________ 6 3.1.1. Accumulation d’ozone troposphérique _________________________________________________ 6 3.2. Effets sur la santé humaine ______________________________________________________ 7 3.2.1. Indirects __________________________________________________________________________ 7 3.2.2. Directs ___________________________________________________________________________ 7 4. Réglementation_______________________________________________________________ 8 4.1. Environnement________________________________________________________________ 8 4.1.1. Au niveau mondial _________________________________________________________________ 8 4.1.2. Au niveau de l’Union Européenne _____________________________________________________ 8 4.1.3. Au niveau national _________________________________________________________________ 9 4.2. Santé au travail _______________________________________________________________ 9 5. Méthodes de traitement ______________________________________________________ 10 5.1. Procédés récupératifs _________________________________________________________ 10 5.1.1. Adsorption _______________________________________________________________________ 10 5.1.2. Absorption _______________________________________________________________________ 10 5.1.3. Condensation ____________________________________________________________________ 10 5.1.4. Procédés à membrane _____________________________________________________________ 10 5.2. Procédés destructifs ___________________________________________________________ 11 5.2.1. Procédés biologiques ______________________________________________________________ 11 5.2.2. Oxydation thermique ______________________________________________________________ 11 5.2.3. Oxydation catalytique ______________________________________________________________ 11 5.2.4. Photocatalyse ____________________________________________________________________ 11 5.2.5. Oxydation par plasma froid _________________________________________________________ 11 5.3. Couplage de procédés _________________________________________________________ 12 5.4. Choix d’un procédé de traitement ________________________________________________ 12 6. Problématique de l’étude ______________________________________________________ 14 6.1. Contexte industriel ____________________________________________________________ 14 6.1.1. Besoins __________________________________________________________________________ 14 6.1.2. COV cibles _______________________________________________________________________ 14 6.2. Solution proposée ____________________________________________________________ 15 6.2.1. Procédé étudié ___________________________________________________________________ 15 6.2.2. Objectifs de l’étude ________________________________________________________________ 16 Références bibliographiques _______________________________________________________ 18 Chapitre 2. Élimination des COV par absorption ___________________________ 19 1. Équilibre liquide-gaz __________________________________________________________ 21 1.1. Influence de la température ____________________________________________________ 21 1.2. Influence de la viscosité ________________________________________________________ 22 1.3. Influence de la présence de biomasse _____________________________________________ 22 1.4. Interactions régissant l’absorption _______________________________________________ 22 2. Transfert de matière __________________________________________________________ 22 2.1. Diffusion ____________________________________________________________________ 22 2.2. Coefficients locaux et globaux de transfert de matière ________________________________ 23 3. Contacteurs gaz/liquide _______________________________________________________ 25 3.1. Choix d’un
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