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Phase Behaviour in Water/Hydrocarbon Mixtures Involved in Gas Production Systems Antonin Chapoy

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Phase Behaviour in Water/Hydrocarbon Mixtures Involved in Gas Production Systems Antonin Chapoy Phase behaviour in water/hydrocarbon mixtures involved in gas production systems Antonin Chapoy To cite this version: Antonin Chapoy. Phase behaviour in water/hydrocarbon mixtures involved in gas production systems. Engineering Sciences [physics]. École Nationale Supérieure des Mines de Paris, 2004. English. pastel- 00001202 HAL Id: pastel-00001202 https://pastel.archives-ouvertes.fr/pastel-00001202 Submitted on 15 Apr 2005 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. Collège doctoral N° attribué par la bibliothèque |__|__|__|__|__|__|__|__|__|__| T H E S E pour obtenir le grade de Docteur de l’Ecole des Mines de Paris Spécialité “Génie des Procédés” présentée et soutenue publiquement par Antonin CHAPOY Le 26 Novembre 2004 PHASE BEHAVIOUR IN WATER/HYDROCARBON MIXTURES INVOLVED IN GAS PRODUCTION SYSTEMS ETUDE DES EQUILIBRES DES SYSTEMES : EAU-HYDROCARBURES-GAZ ACIDES DANS LE CADRE DE LA PRODUCTION DE GAZ Directeur de thèse : Dominique RICHON Jury : M. Jürgen GMEHLING ................................................................... President M. Jean-Michel HERRI.................................................................Rapporteur M. Gerhard LAUERMANN........................................................Examinateur M. Francois MONTEL................................................................Examinateur M. Dominique RICHON .............................................................Examinateur M. Bahman TOHIDI .....................................................................Rapporteur 2 A ma Misstinguette, 3 4 Remerciements Dans un premier temps, je voudrais exprimer ma sincère gratitude au Professeur Dominique Richon d’avoir été mon Directeur de Thèse durant ces trois années passées au sein du laboratoire TEP et qui m’a fait confiance pour réaliser ce travail. Ich bin Herrn Jürgen Gmehling außerordentlich dankbar, den Vorsitz des Prüfungsausschusses für diese Dissertation angenommen zu haben. Je remercie très sincèrement M. Jean-Michel Herri et M. Bahman Tohidi d’avoir accepté d’être rapporteurs de cette thèse et de participer au jury chargé de son examen. Je tiens également à remercier M. Gerhard Lauermann et M. Francois Montel d’avoir eu la gentillesse de s’intéresser à ce travail et pour leur participation au jury d’examen. Ce travail est, pour une grande partie un travail expérimental et il matérialise les efforts et la participation de toute l’équipe du laboratoire. Pour cela je tiens à remercier Alain Valtz, Albert Chareton et Pascal Théveneau pour leurs conseils sur le plan expérimental ainsi que David Marques et Hervé Legendre pour leurs aides techniques. Sans aucun doute, les résultats de ce travail tiennent la marque d’une série de discussions très fructueuses avec l’ensemble des doctorants et post- doctorants. Je garderai également un très bon souvenir des différents membres du laboratoire que j’ai pu côtoyer au cours de ces trois années: Christophe, Fabien, Cathy, Jeannine, Armelle, Vania, Samira, Salim, Wael, Duc. I also would like to thank Professor Bahman Tohidi from the Centre of Gas Hydrate, for welcoming me in his team. It has been very helpful time to discuss problems with him, during my stay at the Heriot Watt Petroleum Institute. A big thank you goes to his Ph. D. students, A. H. Mohammadi and Zahidah Md Zain for all the help they provided me during my stay, for 5 welcoming me in their office and for very fruitful discussions. I wish also to thank Rod Burgass, Ross Anderson, Alastair Reid, Colin Flockhart and Jim Pantling for their experimental expertise and the maintenance of the experimental set up. I wish also to acknowledge the European Infrastructure for Energy Reserve Optimization (EIERO) for their financial support providing me the opportunity to work with the hydrate team. Further I am grateful to Professor Adrian Todd for helping me to get through the EIERO application process. 6 Table of Contents 1. INTRODUCTION AND INDUSTRIAL CONTEXT.......................................... 17 2. STATE OF THE ART, BIBLIOGRAPHY REVIEW ........................................ 25 2.1. Properties and Characteristics of Water................................................................... 25 2.2. Gas Hydrates............................................................................................................ 31 2.3. Experimental Data.................................................................................................... 33 2.3.1. Water Content in the Gas Phase....................................................................... 34 2.3.1.1. Water Content in the Gas Phase of Binary Systems ................................ 34 2.3.1.2. Water Content in Natural Gas Systems.................................................... 37 2.3.2. Hydrocarbon Solubility in Water ..................................................................... 38 2.3.3. Hydrate Forming Conditions............................................................................ 45 3. THERMODYNAMIC MODELS FOR FLUID PHASE EQUILIBRIUM CALCULATION ............................................................................................ 53 3.1. Approaches for VLE Modelling............................................................................... 53 3.1.1. Virial Equations................................................................................................ 54 3.1.2. Cubic Equations of State.................................................................................. 55 3.1.2.1. van der Waals Equation of State .............................................................. 56 3.1.2.2. RK and RKS Equation of State................................................................ 57 3.1.2.3. Peng-Robinson Equation of State ............................................................ 58 3.1.2.4. Three-Parameter Equation of State .......................................................... 59 3.1.2.5. Temperature Dependence of Parameters.................................................. 63 3.1.2.6. EoS Extension for Mixture Application................................................... 66 3.1.3. The γ – Φ approach .......................................................................................... 67 3.1.4. Activity Coefficient.......................................................................................... 70 3.1.4.1. NRTL Model............................................................................................ 71 3.1.4.2. UNIQUAC Model.................................................................................... 72 3.1.4.3. UNIFAC and Modified UNIFAC ............................................................ 73 3.2. Hydrate Phase Equilibria.......................................................................................... 75 3.2.1. Empirical Determination........................................................................................ 75 3.2.2. van der Waals-Platteeuw Model (Parrish and Prausnitz Development) ................ 77 3.2.3. Modifications of the vdW-P Model ....................................................................... 80 3.2.3.1. Classical Modifications................................................................................... 80 3.2.3.2. Chen and Guo Approach................................................................................. 81 4 EXPERIMENTAL STUDY ................................................................................................... 87 4.1 Literature Survey of Experimental Techniques and Apparatus ............................... 87 4.1.1 Synthetic Methods............................................................................................ 88 4.1.2 Analytical Methods.......................................................................................... 90 7 4.1.3 Stripping Methods, Measurement of Activity Coefficient and Henry’s Constant at Infinite Dilution............................................................................................................ 91 4.1.4 Review of the Experimental Set-Ups for Determination of the Water Contents . .......................................................................................................................... 93 4.1.4.1 Direct Methods............................................................................................. 93 4.1.4.2 Indirect Methods ......................................................................................... 95 4.1.5 Review of the Experimental Set-ups for Determination of Gas Solubilities . 100 4.2 Description of the Apparati for Measurement of the Water Content and Gas Solubilities.......................................................................................................................... 100 4.2.1 The Experimental Set-ups for Determination of the Water Content and Gas Solubilities...................................................................................................................... 101 4.2.1.1 Chromatograph..........................................................................................
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