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Profundización En Los Mecanismos De Corrosión De Las Aleaciones De Magnesio

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Profundización En Los Mecanismos De Corrosión De Las Aleaciones De Magnesio UNIVERSIDAD COMPLUTENSE DE MADRID FACULTAD DE CIENCIAS QUÍMICAS DEPT. CIENCIA DE LOS MATERIALES E INGENIERÍA METALÚRGICA Profundización en los Mecanismos de Corrosión de las Aleaciones de Magnesio. Estrategias para Mejorar la Resistencia a la Corrosión. Tesis Doctoral ALEJANDRO SAMANIEGO MIRACLE DIRECTOR DR. SEBASTIÁN FELIU BATLLE (CENIM-CSIC) TUTOR DR. RAÚL ARRABAL DURÁN (UCM) MADRID 2014 A mis padres que día a día hacen todo lo posible para que pueda lograr mis sueños. Gracias por haberme apoyado en todo momento, por vuestros consejos, valores y por la motivación constante que me aportáis en todo lo que hago. A mi hermano, por ser un ejemplo del cual aprendo cada día. A mi novia María, gracias por tu paciencia y comprensión. Gracias por sacrificar tu tiempo para que yo pueda cumplir con el mío. Esta tesis lleva mucho de ti, gracias por estar a mi lado. Agradecimientos En primer lugar, me gustaría dar las gracias a todas las personas que trabajan en el CENIM por su acogida y apoyo. Con vosotros estos últimos cuatro años han pasado volando, y eso solo ha sido posible gracias a vuestro trato. Me gustaría extender este agradecimiento de forma especial a los miembros del departamento de Ingeniería de Superficies, Corrosión, y Durabilidad con los que he tenido la posibilidad de compartir mí día a día durante la realización de esta tesis. Asimismo, quisiera expresar mi enorme gratitud a mi director de tesis, el Dr. Sebastián Feliu Batlle, por su paciencia, enseñanzas y apoyo constante en el desarrollo de la tesis, así como por anteponer mi desarrollo y aprendizaje frente a su propio beneficio personal. ¡Gracias Sebastián por sacar lo mejor de mí, tanto en el ámbito profesional como en el personal! No quisiera olvidarme de su padre, el Dr. Sebastián Feliu Matas, quien con su experiencia y paciencia, ha sabido transmitirme muchos conocimientos y más ilusión. También, me gustaría dar las gracias al Dr. Raúl Arrabal, por su ayuda durante la tesis y por hacerme saber que siempre podía acudir a él cuando lo necesitara. No podría haberlo hecho sin la financiación aportada por el Ministerio de Economía y Competitividad a través del proyecto MAT 2009-13530 y la gestión realizada por el CSIC durante mi tesis y mis estancias en el extranjero. En especial, me gustaría agradecer la gestión realizada por Isabel Ocaña. Quisiera hacer una mención especial a mis compañeros del CENIM; Amir, Violeta, Juan Carlos, Blanca, Rodrigo, Emilio, Santi, Belén, Cristina, Lucía, María Lorenza, María, Laura, Dani, Irene, Oscar, Iván, Heydis, Diana, Blanca, Joaquín, Teresa, Ana, David, Manuel, Fede y Mónica. ¡¡Gracias!! ¡¡Compartir este tiempo con vosotros ha sido sensacional!! A mis compañeros de máster y del CENIM, Alberto y Sara, y a Chus, Víctor, Nacho, Miliki, Antonio, Iñaki y Alfonso por su ayuda y apoyo durante la experimentación. Toda mi gratitud por el tiempo y el buen trato recibido durante mis estancias en el extranjero al Dr. Nick Birbilis (Monash University) y al Dr. Gerald Frankel (Fontana Corrosion Center, OSU), así como a todos aquellos que han amenizado mi experiencia en esos países. Kateryna, Xiao-Bo, Rajeev, Nazatul, Jermain, Nico, Ben, Will, Sara y Dan. Thanks to all folks!! Was great sharing some time with you!! Finalmente, quiero expresar mi agradecimiento de forma muy especial a mis padres, a mi hermano, a mi novia María y a mis abuelos; los que están y los que se han ido. Gracias por vuestro cariño, comprensión y apoyo incondicional en todo momento. Sin vosotros, no lo hubiera conseguido. ‐ 5 ‐ ‐ 6 ‐ Índice Contenido Summary ....................................................................................................................................... 9 Resumen ...................................................................................................................................... 13 Introducción ................................................................................................................................ 17 Propiedades mecánicas ........................................................................................................... 21 Utilización del magnesio. ........................................................................................................ 23 Comportamiento a la corrosión del magnesio y sus aleaciones ............................................. 24 Aleaciones de Magnesio .......................................................................................................... 32 Protección contra la corrosión ................................................................................................ 36 Materiales y Técnicas Experimentales ........................................................................................ 37 Objetivos y plan de trabajo ......................................................................................................... 49 Resultados y Discusión ................................................................................................................ 53 Capítulo I: Profundización en los Mecanismos de Corrosión del Magnesio y el Efecto Diferencial Negativo (NDE) ...................................................................................................... 55 Introducción ........................................................................................................................ 57 Resultados ........................................................................................................................... 59 Discusión ........................................................................................................................... 109 Capítulo II: Caracterización de las películas de óxidos superficiales y de las capas de productos de corrosión de las aleaciones AZ31 y AZ61 ........................................................ 115 Introducción ...................................................................................................................... 117 Resultados ......................................................................................................................... 119 Discusión ........................................................................................................................... 209 Capítulo III: Estrategias para mejorar la resistencia a la corrosión del magnesio y aleaciones del sistema Mg‐Al‐Zn ............................................................................................................. 213 Introducción ...................................................................................................................... 215 Resultados ......................................................................................................................... 217 Discusión ........................................................................................................................... 333 Conclusiones ............................................................................................................................. 339 Bibliografía ................................................................................................................................ 341 ‐ 7 ‐ Esta Memoria se ha editado siguiendo el formato de compilación de artículos científicos ya publicados, según la reglamentación de la Universidad Complutense de Madrid (www.ucm.es). Los artículos científicos se han insertado en la memoria en formato Word, manteniendo el texto, organización, numeraciones y bibliografía en el idioma original de las publicaciones. Junto con estos artículos ya publicados se han insertado como trabajo adicional tres artículos que actualmente se encuentran en revisión y todavía no han sido publicados. El resto de la memoria se ha redactado en castellano de acuerdo a la normativa oficial. Asimismo, se ha optado por enumerar de forma independiente la bibliografía general de esta memoria de aquella incluida en los artículos publicados, a fin de poder facilitar la lectura. ‐ 8 ‐ Summary Summary Magnesium (Mg) alloys posses a combination of low density, high specific strength and good castability, which makes them promising lightweight structural materials. However, since magnesium is one of the most chemically active metals, its corrosion resistance is one of the key points that limit its use in real conditions. This thesis is divided into three chapters. The first focuses on the corrosion mechanism of pure magnesium and the negative difference effect (NDE). The second is formed by an in-depth study of the native oxide surface films and the corrosion products layers formed on the AZ31 and AZ61 magnesium alloys, along with their influence on corrosion. The third chapter comprises several studies where different strategies to reduce the corrosion rate of magnesium and its alloys were analyzed. Chapter I: Corrosion Mechanisms of Magnesium and the Negative Difference Effect (NDE). Despite the large number of papers published on the corrosion mechanisms of magnesium and its alloys, there are still some issues that have not been sufficiently clarified. Magnesium experiences what in literature is called negative difference effect (NDE). This effect is characterized by an increase in the amount of hydrogen generated at anodic polarization; which is contradictory to the expected behaviour based on the classic electrochemical theory. The NDE phenomenon should be totally understood in order to fully assess the utilities of Mg as an electrode or as a structural material, the latter related to corrosion. Several mechanisms
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