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High Themal Energy Storage Density Molten Salts for Parabolic HIGH THEMAL ENERGY STORAGE DENSITY MOLTEN SALTS FOR PARABOLIC TROUGH SOLAR POWER GENERATION by TAO WANG RAMANA G. REDDY, COMMITTEE CHAIR NITIN CHOPRA YANG-KI HONG A THESIS Submitted in partial fulfillment of the requirements for the degree of Master of Science in the Department of Metallurgical and Materials Engineering in the Graduate School of The University of Alabama TUSCALOOSA, ALABAMA 2011 Copyright Tao Wang 2011 ALL RIGHTS RESERVED ABSTRACT New alkali nitrate-nitrite systems were developed by using thermodynamic modeling and the eutectic points were predicted based on the change of Gibbs energy of fusion. Those systems with melting point lower than 130oC were selected for further analysis. The new compounds were synthesized and the melting point and heat capacity were determined using Differential Scanning Calorimetry (DSC). The experimentally determined melting points agree well with the predicted results of modeling. It was found that the lithium nitrate amount and heating rate have significant effects on the melting point value and the endothermic peaks. Heat capacity data as a function of temperature are fit to polynomial equation and thermodynamic properties like enthalpies, entropies and Gibbs energies of the systems as function of temperature are subsequently induced. The densities for the selected systems were experimentally determined and found in a very close range due to the similar composition. In liquid state, the density values decrease linearly as temperature increases with small slope. Moreover, addition of lithium nitrate generally decreases the density. On the basis of density, heat capacity and the melting point, thermal energy storage was calculated. Among all the new molten salt systems, LiNO3-NaNO3- KNO3-Mg(NO3)2-MgKN quinary system presents the largest thermal energy storage density as well as the gravimetric density values. Compared to the KNO3-NaNO3 binary solar salt, all the new molten salts present larger thermal energy storage as well as the gravimetric storage density values, which indicate the better thermal energy storage capacity for solar power generation systems. ii DEDICATION This thesis is dedicated to everyone who helped me and guided me through the trials and tribulations of creating this manuscript. In particular, my family and close friends who stood by me throughout the time taken to complete this masterpiece. iii ACKNOWLEDGEMENTS I am pleased to express my gratitude and appreciation to my advisor, Professor Ramana G. Reddy, for his patience and guidance during my graduate study and the entire research work. I am greatly benefited from his experience, knowledge and enthusiasm for scientific research. I would like to express my sincere thanks to Dr. Nitin Chopra and Dr. Yang-Ki Hong for serving on my committee. Their valuable suggestions and comments are very insightful for my research work. I would like to thank all the research colleagues of Dr. Reddy‟s research group, special thanks to Dr. Divakar Mantha for his valuable suggestions and comments. I would like to extend my gratitude to U.S Department of Energy for the financial support. Finally, I would like to thank my parents and my fiancée, whose invaluable understanding and loving support helped me through the difficult times. iv TABLE OF CONTENTS ABSTRACT ii DEDICATION iii ACKNOWLEDGEMENTS iv LIST OF TABLES viii LIST OF FIGURES x CHAPTER 1. INTRODUCTION 1 CHAPTER 2. LITERATURE REVIEW 11 2.1 Melting point 11 2.2 Density 15 2.3 Heat capacity 18 CHAPTER 3. OBJECTIVES 22 CHAPTER 4. THERMODYNAMIC MODELING OF SALT SYSTEMS 24 4.1 Thermodynamic modeling 24 4.2 Calculations 27 v CHAPTER 5. EXPERIMENTAL PROCEDURE 30 5.1 Melting point determination of molten salt mixtures 30 5.1.1 Materials 30 5.1.2 Apparatus and Procedure 30 5.2 Heat Capacity determination of molten salt mixtures 32 5.3 Density determination of molten salt mixtures 33 CHAPTER 6. RESULT AND DISCUSSION 34 6.1 Melting point determination 34 6.1.1 DSC equipment calibration 34 6.1.2 Results 35 6.1.3. Discussion 41 6.2 Heat capacity determination 51 6.2.1 Heat capacity calibration 51 6.2.2 Results 52 6.2.3 Thermodynamic properties 55 6.2.4 Discussion of Gibbs energy change for molten salts 84 6.3 Density determination 86 vi 6.3.1 Density calibration 86 6.3.2 Results and discussions 82 6.4 Thermal energy storage density of molten salts 90 CHAPTER 7. CONCLUSION 94 REFERENCES 96 APPENDIX 104 APPENDIX A 104 APPENDIX B 109 APPENDIX C 114 APPENDIX D 118 APPENDIX E 123 APPENDIX F 128 APPENDIX G 133 APPENDIX H 138 APPENDIX I 143 vii LIST OF TABLES 2.1. Melting point of various nitrate salt systems 12 2.2. Melting point of various carbonate salt systems 13 2.3 Melting point of various fluoride/chloride salt systems 14 2.4 Melting point of various hydroixde salt systems 15 2.5 Density coefficients A and B of nitrate salts 16 2.6 Density coefficients A and B of carbonate salts 17 2.7 Density coefficients A and B of chloride/fluoride salts 17 2.8 Density coefficients A and B of molten salt mixture with hydroxide salts 18 2.9 Heat capacity of alkali nitrate salt at 500oC 19 2.10 Heat capacity of alkali carbonate salt at 500oC 19 2.11 Heat capacity of fluoride/chloride salt at 500oC 20 2.12 Heat capacity of hydroxide salt at 500oC 21 4.1 Calculated composition and melting point for multi-component systems 29 6.1 Calibration data of melting points with different samples 35 6.2 DSC results of melting point, transition point and change of enthalpy 41 viii 6.3 Fusion and solid phase transition temperature for individual salts 42 6.4. Melting points of candidate systems as function of temperatures 51 6.5 Calibration data of heat capacities with different samples 52 6.6 Heat capacity of selected new TES molten salt mixtures 54 6.7 Change of Gibbs energy values at 623.15K for molten salt systems 85 6.8 Calibration of density measurements with different pure nitrate salts 86 6.9 Coefficient of A and B for density determination of salt #1 to salt # 9 87 6.10 Extrapolated value of density and heat capacity at 500oC of salt #1 to salt #9 91 6.11 Energy density of salt #1 to salt #9 compare to solar salt 92 6.12 Gravimetric storage densities for solar salt and new molten salts 93 ix LIST OF FIGURES 1.1 Theoretical and engineering energy conversion efficiency as function of temperature 6 1.2 Gravimetric storage density for different energy storage systems as function of temperature 8 5.1 Photography of set-up for DSC equipment 31 6.1 Melting point calibration with indium sample 34 6.2 Melting point calibration with KNO3 sample 35 6.3 DSC endothermic peaks of LiNO3-NaNO3-KNO3 salt. 36 6.4 DSC endothermic peaks of NaNO3-NaNO2-KNO3 salt. 37 6.5 DSC endothermic peaks of LiNO3-NaNO3-KNO3-MgK salt. 37 6.6 DSC endothermic peaks of LiNO3-NaNO3-KNO3-NaNO2 salt. 38 6.7 DSC endothermic peaks of LiNO3-NaNO3-NaNO2-KNO3-KNO2 salt. 38 6.8 DSC endothermic peaks of LiNO3-NaNO3-KNO3-KNO2 salt. 39 6.9 DSC endothermic peaks of LiNO3-KNO3-NaNO2-KNO2 salt. 39 6.10 DSC endothermic peaks of LiNO3-KNO3-NaNO2-Mg(NO3)2 salt. 40 6.11 DSC endothermic peaks of LiNO3-NaNO3-KNO3-Mg(NO3)2-MgKN Salt. 40 6.12 DSC plot of 69.8wt% KNO3 -30.2wt% NaNO2 binary system 43 x 6.13 DSC plot of 27.0wt% NaNO3-73.0wt% KNO3 binary system 45 6.14 DSC plot of 45.8wt%LiNO3-54.2wt%KNO3 binary system 45 6.15 DSC plot of 46.0wt% NaNO3-54.0wt% KNO3 binary system 46 6.16(a) DSC endothermic peaks of LiNO3-NaNO3-KNO3-KNO2 salt o for 20 C/min heating rate. 47 6.16(b) DSC endothermic peaks of LiNO3-NaNO3-KNO3-KNO2 salt o for 5 C/min heating rate. 48 6.17(a) DSC endothermic peaks of LiNO3-KNO3-NaNO2-KNO2 salt o for 5 C/min heating rate. 49 6.17(b) DSC endothermic peaks of LiNO3-KNO3-NaNO2-KNO2 salt o for 20 C/min heating rate. 49 6.18 Heat capacity data plot of LiNO3-NaNO3-KNO3 ternary system as function of temperature 53 6.19 Heat capacity of LiNO3-NaNO3-KNO3 in liquid state from 403.15-623.15K 54 6.20 Change of Gibbs energy as function of temperature for molten salt systems 85 6.21 The densities of the salt #1 to salt #5 as function of temperature 87 6.22 The densities of the salt #6 to salt #9 as function of temperature 89 6.23 Densities of the salt #1, salt #2 as function of temperature compared to the equimolar NaNO3-KNO3 binary system and pure KNO3. 90 6.24 Gravimetric storage density comparison of different energy storage xi systems as function of temperature 93 xii CHAPTER 1 INTRODUCTION Renewable energy sources such as wind, solar, water power, geothermal and biomass are playing more and more significant role in our energy supply. Because the cheap cost and infinite amount of energy storage inside the resource, solar energy is emphasized since 20th century and viewed as promising alternative method to satisfy the large energy consumption every day in the world, reduce the emission of carbon and strengthen the economy. The wind energy was used as a clean energy to generate electricity back to late 19th century. However, this renewable energy source was not emphasized due to the cheap price of fossil fuel.
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