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Experimental measurement and thermodynamic modelling of clathrate hydrate equilibria and salt solubility in aqueous ethylene glycol and electrolyte solutions
Institution:1. Chemical and Biological Engineering Department, Colorado School of Mines, 1500 Illinois St., Golden, CO 80401, USA;2. Kangwon National University, Department of Energy and Resources Engineering, 1 Kangwondaehak-gil, Chuncheon-si, Gangwon-do 200-701, Republic of Korea;1. Key Laboratory of Gas Hydrate, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, PR China;2. Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development, Chinese Academy of Sciences, Guangzhou 510640, PR China;3. Guangzhou Center for Gas Hydrate Research, Chinese Academy of Sciences, Guangzhou 510640, PR China;4. Nano Science and Technology Institute, University of Science and Technology of China, Suzhou 215123, PR China;1. College of Power and Energy Engineering, Harbin Engineering University, Harbin 150001, China;2. CNOOC Research Institute Co. Ltd., Beijing 100027, China
Abstract:We present the extension of a recently developed method for modelling saline water to the thermodynamic prediction of phase behaviour for mixed salt–organic clathrate hydrate inhibitor aqueous solutions. Novel freezing point, boiling point and salt solubility data have been generated for NaCl–ethylene glycol (EG) and KCl–EG aqueous solutions. These data have been used in the optimisation of binary interaction parameters between salts and ethylene glycol. The extended thermodynamic model is capable of predicting complex vapour–liquid–solid (VLSE) equilibria for aqueous electrolytes and/or organic inhibitor solutions over a wide range of pressures, temperatures and inhibitor concentrations. Reliable hydrate dissociation data for two mixed salt–organic inhibitor quaternary systems (CH4–H2O–NaCl–EG and CH4–H2O–KCl–EG) have been measured at pressures up to 50 MPa. These data are used to validate the predictive capabilities of the model for hydrate equilibria. Good agreement between experimental data and predictions is observed, demonstrating the reliability of the developed model.
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