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A Thermodynamic Study of the Zeolite Stilbite

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A Thermodynamic Study of the Zeolite Stilbite Western Michigan University ScholarWorks at WMU Master's Theses Graduate College 8-1987 A Thermodynamic Study of the Zeolite Stilbite David Adams Howell Follow this and additional works at: https://scholarworks.wmich.edu/masters_theses Part of the Geology Commons Recommended Citation Howell, David Adams, "A Thermodynamic Study of the Zeolite Stilbite" (1987). Master's Theses. 1263. https://scholarworks.wmich.edu/masters_theses/1263 This Masters Thesis-Open Access is brought to you for free and open access by the Graduate College at ScholarWorks at WMU. It has been accepted for inclusion in Master's Theses by an authorized administrator of ScholarWorks at WMU. For more information, please contact [email protected]. A THERMODYNAMIC STUDY OF THE ZEOLITE STILBITE by David Adams Howell A Thesis Submitted to the Faculty of The Graduate College in partial fulfillment of the requirements for the Degree of Master of Science Department of Geology Western Michigan University Kalamazoo, Michigan August 1987 Reproduced with permission of the copyright owner. Further reproduction prohibited without permission. A THERMODYNAMIC STUDY OF THE ZEOLITE STILBITE David Adams Howell, M.S. Western Michigan University, 1987 Stilbite is a calcium-rich zeolite found in low-grade metamorphic and hy- drothermally altered environments. In this study, measurements of the en­ thalpy of formation at 298.15 K, heat capacity from 5 to 350 K, and enthalpy increments horn 350 to 500 K were performed on a specimen of stilbite char­ acterized by electron microprobe analysis. The actual formula of the stilbite is: Cai.oi9Nao.i36Ko.oo6Al2.i8oSi6.82oOis * 7.33HjO. Evaluation of the thermo­ dynamic properties for stilbite at T = 298.15 K produced the following val­ ues: AfH °(T) = —11034.6±6.6 kJ-mol"1, C ^ T ) = 808.73dbl.62 J.K - 1-mol-1, S ° (T )-S ° ( 0) = 805.54dbl.61 J-K -^m ol"1, AfS°(T) = -2990.44±1.86 J-K "1- mol-1, and AfG^(T) = —10143.0±6.6 kJ-mol-1. Comparison of the calorimet- rically derived value for the Gibbs fr ee energy of formation, AfG^,, of stilbite with that calculated from an estimation method (La Iglesia and Anzar, 1986) shows a difference of 49 kJ-mol-1. An attempt was made to retrieve a consistent Gibbs free energy value for laumontite using available phase equilbria and calorimetric data for heulandite and stilbite. Reproduced with permission of the copyright owner. Further reproduction prohibited without permission. ACKNOWLEDGEMENTS I owe many thanks to those who helped make this research successful. I am indebted to my advisor, John D. Grace, for introducing me to the op­ portunities that existed through the Department of Educational Programs at Argonne National Laboratory. Special thanks are directed to Argonne researchers Patrick A. G. O’Hare, Gerald K. Johnson, and Ian R. Tasker for their patient in­ struction, guidance and suggestions during the course of my thesis work. Recog­ nition of Professor William S. Wise from the University of California, Santa Barbara, for his preparation and analysis of the stilbite is also due. I am very grateful for the typing expertise of Kay Shields at Argonne. Most dearly, I wish to express my appreciation of the love and support given to me by my parents, Stephen and Ann Howell. David A. Howell ii Reproduced with permission of the copyright owner. Further reproduction prohibited without permission. INFORMATION TO USERS This reproduction was made from a copy of a document sent to us for microfilming. 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Zeeb Road Ann Arbor, Ml 48106 Reproduced with permission of the copyright owner. Further reproduction prohibited without permission. Reproduced with permission of the copyright owner. Further reproduction prohibited without permission. 1331678 A THERMODYNAMIC STUDY OF THE ZEOLITE STILBITE Howell, David Adams, M.S. Western Michigan University, 1987 U MI 300 N. Zeeb Rd. Ann Arbor, MI 48106 Reproduced with permission of the copyright owner. Further reproduction prohibited without permission. Reproduced with permission of the copyright owner. Further reproduction prohibited without permission. PLEASE NOTE: In all cases this material has been filmed in the best possible way from the available copy. Problems encountered with this document have been identified here with a check mark V . 1. Glossy photographs or pages 2. Colored illustrations, paper or print 3. Photographs with dark background _____ 4. Illustrations are poor copy_______ 5. Pages with black marks, not original copy______ 6. Print shows through as there is text on both sides of page 7. Indistinct, broken or small print on several pages S' 8. Print exceeds margin requirements______ 9. Tightly bound copy with print lost in spine_______ 10. Computer printout pages with indistinct print______ 11. Page(s) ___________lacking when material received, and not available from school or author. 12. Page(s) seem to be missing in numbering only as text follows. 13. Two pages numbered . Text follows. 14. Curling and wrinkled pages ______ 15. Dissertation contains pages with print at a slant, filmed as received 16. Other________________________________________________ Reproduced with permission of the copyright owner. Further reproduction prohibited without permission. Reproduced with permission of the copyright owner. Further reproduction prohibited without permission. TABLE OF CONTENTS ACKNOWLEDGEMENTS. ......................................................... ii TABLE OF CONTENTS.................... iii LIST OF TABLES............................................ v LIST OF FIGURES................................................. vi CHAPTER I. INTRODUCTION........................................................... 1 Stilbite Mineralogy...................................................... .... 3 Stilbite Occurrence and Experimental Phase Equilibria .... 4 II. ENTHALPY OF FORMATION OF STILBITE AT 298.15 K .................................... 8 A pparatus..................................... 8 Material Preparation ..........................................................................12 Sample Preparation ........................................................................... 15 Experimental Procedure .............................................. 16 Data Analysis and R esults ....................................................... 17 III. HEAT CAPACITIES OF STILBITE FROM 5 TO 350 K . 24 A pparatus................................. 24 Sample Preparation ........................ ................................................29 Experimental Procedure ........................ ........................................31 Data Analysis and R esults ................................................................32 IV. ENTHALPY INCREMENTS RELATIVE TO 298.15 K OF STILBITE FROM 350 TO 500 K .............................................. 42 Apparatus ......................................................................... 42 Sample Preparation .......................................... 45 m• •• Reproduced with permission of the copyright owner. Further reproduction prohibited without permission. Table of Contents— Continued CHAPTER Experimental Procedure ............................................. 47 Data Analysis and R esults ............................................................ 49 V. DISCUSSION OF RESULTS AND CONCLUSION................................ 53 Comparison With Estimation M ethod ................................................ 53 Retrieval of Gibbs Free Energy of Formation ofLaumontite ............................................ 54 Conclusion ........................................................ 57 APPENDICES A. Definition of Symbols .........................................................
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