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Microfilms International 300 N /6EB ROAD INFORMATION TO USERS This was produced from a copy of a document sent to us for microfilming. While the most advanced technological means to photograph and reproduce this document have been used, the quality is heavily dependent upon the quality of the material submitted. The following explanation of techniques is provided to help you understand markings or notations which may appear on this reproduction. 1.The sign or “target” for pages apparently tacking from the document photographed is “Missing Page(s)”. If it was possible to obtain the missing page(s) or section, they are spliced into the film along with adjacent pages. This may have necessitated cutting through an image and duplicating adjacent pages to assure you of complete continuity. 2. When an image on the film is obliterated with a round black mark it is an indication that the film inspector noticed either blurred copy because of movement during exposure, or duplicate copy. Unless we meant to delete copyrighted materials that shoutd not have been filmed, you will find a good image of the page in the adjacent frame. 3. When a map, drawing or chart, etc., is part of the material being photo­ graphed the photographer has followed a definite method in “sectioning” the material. It is customary to begin filming at the upper left hand comer of a large sheet and to continue from left to right in equal sections with small overlaps. If necessary, sectioning is continued again—beginning below the first row and continuing on until complete. 4. For any illustrations that cannot be reproduced satisfactorily by xerography, photographic prints can be purchased at additional cost and tipped into your xerographic copy. Requests can be made to our Dissertations Customer Services Department. 5. Some pages in any document may have indistinct print. In all cases we have filmed the best available copy. University Microfilms International 300 N /6EB ROAD. ANN ARBOR. Ml 48106 18 BEDFORD ROW, LONDON WC1R 4EJ, ENGLAND 7916045 VAU * TE-LIN THE PASSIVITY OF IRON—CHROMIUM ALLOYS. THE OHIO STATE UNIVERSITY* PH.D.* 1979 Uni\wsitv Microfilms International joon ^“ droao . ann arsoh .mi4bio6 PLEASE NOTE: In all cases this material has been filmed 1n the best possible way from the available copy. Problems encountered with this document have been Identified here with a check mark . 1. Glossy photographs_ 2. Colored Illustrations 3. Photographs with dark background 4. Illustrations are poor copy 5. Print shows through as there Is text on both sides of page 6. Indistinct, broken or small print on several paqes throughout ____ 7. Tightly bound copy with print lost 1n spine _ 8. Computer printout pages with Indistinct print _______ 9. Page(s) _ lacking when material received, and not available from school or author_______ 10. Paae(s) seem to be missing in numbering only as text follows 11. Poor carbon copy_______ 12. Not original copy, several pages with blurred type ________ 13. Appendix pages are poor copy 14. Original copy with light type _______ 15. Curling and wrinkled pages 16. O ther______ ___ ___________ Irtveraty Micrrinlms tiemational 10 N ZEES RD.. ANN ARBOR VII aSTOB <3131 761-4700 THE PASSIVITY OF IFfON-CHROMIUM ALLOYS DISAEHTATT OH Presented in Partial Fulfillment of the Requirements for the Degree Doctor of Philosophy in the Graduate School of The Ohio State University * By Te-Lin Yau, B.S., M.S. The Ohio State University 1979 Reading Committee: Approved By Professor R. W. Staehle Professor R. A. Rapp Professor J. A. Begley /Ad vi ser Department of Metallurgical DEDICATION To my mother, Mra. Yang Chih Yau, whose wisdom and guidance gave me the patience and perseverance to pursue the doctoral program* To my late father, Mr. Chiu Ho Yau, whose total commitment to the education of his children and the underprivileged made this dissertation possible. ii ACKNOWLEDGMENTS I would like to thank my adviser, Professor R. W. Staehle, for his guidance and counsel during the course of this investigation. Thanks are also due Professors R. A, Rapp and J. A. Begley for their interest. I also wish to thank Dr. S. Smialowska for her interest, suggestions, and stimulation. Financial support by the National Science Foundation is gratefully recognized. Finally, the author extend a special vote of thanks to Miss D. M, Essock for the polish of this dissertation, and to his sister, Shiow Yun, and to Miss Jue Hua Tsai for all the varied tasks they have helped him to complete. VITA April 9, 19ij-5>.... Born - Hunan, Republic of China 1969.............. B.S.E.S., Cheng Kung University, Tainan, Taiwan 1970-197 1......... Mechanical Engineer, Taiwan Shipbuild­ ing Corporation, Keelung, ^aiwan 1971-197 2......... Research Assistant, Department of Engineering Science, Tennessee Technological University, Cookeville, Tennessee 1973.............. M.Sc., Tennessee Technological University, Cookeville, Tennessee 1972-197 9......... Research Associate, Department of Metallurgical Engineering, The Ohio Stat'e University, Columbus, Ohio FIELDS OF STUDY Major Field: Metallurgical Engineering Studies in Metallic Corrosion. Professor M. G. Fontana, Professor F. H. Beck and Professor R. W. Staehle Studies in Physical Metallurgy. Professor J. P. Hirth and Professor G. W. Powell Studies in Mechanical Metallurgy. Professor J. W. Spretnak Studies in Thermodynamics. Professor G. R. St. Pierre TABLE OF CONTENTS i'age ACKNOWLEDGEMENT...................................... 1 ii VITA................................................... iv LIST OF TABLES....................................... viii LIST OF FIGURES...................................... INTRODUCTION........................................... 1.1 Scope of Investigation............ ............ 4 PASSIVITY............ ................................ 2.0 Introduction.................................... 6 2.1 Definition.......................... ............ 2.2 A General Description of Passive Metals and Alloys............ *............................. 2.3 Cathodic Reactions............................. 11 2.4 Anodic Passivation............................. 12 2.5 Theories of Passivity.......................... 16 2.5-1 The Film Theory.......................... 16 2.5-2 The Adsorption Theory................... 20 2-5-3 Combined Film-Adsorption Theory........ 23 2.5-4 Other Theories........................... 24 2.6 The Passivity of Alloys........................ 26 2.6.1 Theories of Passivity in Alloys........ 29 2.6.2 The Passivity of Fe-Cr Alloys.......... 30 2.6.2.1 Iron............................. 30 2.6.2.2 Chromium......................... 32 2.6.2. 3 Iron-Chromivim Alloys.......... 34 2.7 Processes of Film Formation................ 67 2.7-1 Initial Fast Oxidation.................. 67 2.7.2 Kinetics of Film Growth................. 66 2.7.3 The Transition Period................... 71 2.8 Solubility, Dissolution and Passivity........ 73 2.8.1 Solubility of Iron Oxides and Chromium Oxides.................................... 74 2.8.2 Formation and Dissolution of Anodic Oxide Films.............................. 75 2.8.3 Mechanisms of Oxide Dissolution........ 77 v TABLE OP CONTENTS (Continued) AUGER ELECTRON SPECTROSCOPY.................. 83 3.0 Introduction........................................ 83 3.1 Historical Note................................ ' 81; 3.2 The Detected Volume and Auger Electron Mean Escape Depth.................. 86 3.3 Quantitative Analysis......................... 87 3.3*1 Absolute Caloul ations ................. 89 3.3*2 Quantitative Analysis with Standards.. 90 3.3*3 Quantitative Analysis without Standard 3*4 Chemical Effects in AES...................... 9:V 3.5 Composition-vs-depth Profiles................ 101 3.6 Conclusion...,................................. 10o EXPERIMENTAL PROCEDURES.................................. 109 ij.,0 Introduction................................... 109 i|_.l Electrochemical Measurements .......... 110 4.2 Electrolyte Solutions......................... IIP I4..3 Electrochemical Test Cell.................... Ilf Auger Unit..................................... 117 ij-.5 Procedure........................................... 123 I;.5.1 Specimen Preparation...................... 123 4.5*2 Experimental Procedure...................... 12 9' 4.5.3 APPH and NAPH................................ 126 ^Auger Spectrum............................... 128 i;.5*5 Preliminary Alignment....................... 130 i;.5*6 Depth-Concentration Profile................ 132 EXPERIMENTAL RESULTS..................................... 133 5.1 Polarization Behavior of Alloys.................. 133 5*2 Current Decay Curves............................... 133 5.3 Auger Analysis..................................... lij-3 DISCUSSION................................................. 207 6.1 Polarization Behavior of Alloys............. ' 207 6.1.1 Rest Potential.............................. 210 6.1.2 Critical Current Density and Passivation Potential....................... 21^ 6.1.3 Passive Current Density..................... 221; 6.1.1; Transpassive Potential...................... 227 6.1.5 Summary...................................... 728 6.1.6 Conclusions.................................. 230 vi TABLE OP CONTENTS (Contuiued) 6.2 Current Decay Curves ............... 2 32 6.2.1 Determination of Passive Properties of Pe-Cr Alloys.................... 232 6.2.2 The Kinetics of Film Formation......... 239 6.2.3 Summary................................... 2^6 6 . 2 . [|. Conclusion........................ ....... 2ipti 6.3 Auger Analysis....................
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