De Micco, Georgina (2007) Fisicoquímica de las reacciones de cloración de metales y aleaciones. Tesis Doctoral en Ciencias de la Ingeniería, Universidad Nacional de Cuyo, Instituto Balseiro.
![[img]](/style/images/fileicons/application_pdf.png)
| PDF (Tesis) Español 4Mb | |
| PDF (Cap. 2) Restringido a Usuario depositante solamente Español 486Kb | |
| PDF (Cap.5) Restringido a Usuario depositante solamente Español 4Mb | |
| PDF (Cap.8) Restringido a Usuario depositante solamente Español 2679Kb |
Resumen en español
En esta tesis se avanzó en el conocimiento fisicoquímico de sistemas complejos. Las reacciones de cloración son reacciones heterogéneas sólido-gas no catalíticas, que no sólo presentan las dificultades propias del estudio de la reacción produciéndose en una interfase, sino que se suman las características particulares de los cloruros y sus interacciones. Los interrogantes que surgen de este tipo de estudio no pueden resolverse aplicando una sola técnica de análisis; por ello también resulta desde el punto de vista experimental una tarea complicada y deben conocerse varias técnicas instrumentales tanto para obtener los resultados como para la interpretación de los mismos. Se eligió estudiar la cloración de las aleaciones ternarias y binarias que contengan Al, Cu y Zn y los metales puros, ya que estos elementos se encuentran en las vainas de los combustibles nucleares gastados. El objetivo de la investigación es lograr un proceso que elimine la mayor parte del Al el cual es el componente mayoritario. De esta manera se reduce la cantidad de residuos para acondicionar a través de la vitrificación. Los resultados obtenidos permiten no sólo lograr los objetivos propuestos para cada sistema, sino que además pueden ser aplicados a otros sistemas similares para el reciclado de metales.
Resumen en inglés
This thesis has contributed towards the knowledge of complex systems. The chlorination reactions are non-catalytic solid-gas heterogeneous reactions which, in addition to the difficulties associated with the reactions occurring in an interface, have the particular features of chlorides compounds and their interactions. The questions arising from this type of study can not be solved by the application of an individual analysis technique. From the experimental point of view it is complicated, and many instrumental techniques need to be applied in order to obtain significant results as well as meaningful interpretations. The system under study is the chlorination of ternary and binary alloys containing Al, Cu and Zn and the pure metals, as these elements belong to the spent nuclear fuel cladding. The aim of the research has been to develop a process that eliminates most of the aluminium, which is the more abundant specie. In this way, the amount of material to be conditioned (vitrified) is reduced. The objectives proposed for each system have been achieved, and the results obtained can also be applied to similar systems for metal recycling.
| Tipo de objeto: | Tesis (Tesis Doctoral en Ciencias de la Ingeniería) |
|---|---|
| Palabras Clave: | Chlorination; Cloruración; Alloys; Aleaciones; Chlorides; Cloruros; Metals; Metales; Ternary alloy systems; Sistemas de aleaciones ternarias ; Binary alloy systems; Sistemas de aleación binarios. |
| Referencias: | Allain E., Djona M., Gaballah I., “Kinetics of chlorination and carbochlorination of pure tantalum and niobium pentoxides”, Metall. Mater. Trans. B, 1997, vol. 28B, p. 223-233. Alvarez F. J., De Micco G., Bohé A. E., Pasquevich D. M., “Options for spent fuels conditioning”, Final Report Technical Cooperation Regional Project, RLA/4/018, IAEA, March, 2005 Alvarez F. J., De Micco G., Bohé A.E., Pasquevich D.M. “Physicochemical Interactions in the volatilization of chlorides, applied to the Spent Fuel Conditioning”, , Proceedings of the Global Symposium on Recycling Waste Treatment and Clean Technology Rewas 2004, vol. III, p. 2707-16. Avrami M. J. Chem. Phys. 1939, vol. 7, p. 1103. Avrami M. J. Chem. Phys. 1940, vol. 8, p. 212 Avrami M. J. Chem. Phys. 1941, vol. 9, p.177 Baetzold R. C., Somorjai G. A., “Preexponential Factors in Surface Reactions”, Journal of Catalysis, 1976, vol. 45, p. 94-105. Barrett E. P., Soguer L. G., Halenda P. P., “The determination of pore volume and area distributions in porous substances. I. Computations from nitrogen isotherms”, J. Am. Soc., 1951, vol. 73, p. 373- 380. Basan, S., O. Güven, “A comparison of various isothermal thermogravimetric methods applied to the degradation of PVC”. Thermochimica Acta. 1986, vol. 106, p. 169-178. Belknap, L. S., Aluminum trichloride production, US Pat. 3721731, Cabot Corporation, Boston, Massachusetts, USA, 1973. Bevilacqua, A.M., Bohé A.E., Nassini H.E., Pasquevich D.M.. “Radioactive waste reduction from LEU Al-U spent fuel management by a dry chlorination process.” REWAS’99 GLOBAL SYMPOSIUM ON RECYCLING WASTE TREATMENT AND CLEAN TECHNOLOGIES. Septiembre 5-9, 1999, San Sebastián, España. Bohé A. E., Andrade Gamboa J. J., Pasquevich D. M., “Chlorination process applied to zirconium recovery from Zircaloy shavings”, Materials Science and Technology. 1997, vol. 13, p. 865-871. Bohé A.E., Andrade Gamboa, J.J., Lopasso E.M., Pasquevich D.M., “Zirconium recovery from zircaloy shavings”, J. of Materials Science. 1996, vol. 31, p.3469-3474. Bohé, A E, Nassini H E, Bevilacqua A M, Pasquevich D M, Proceedings of the 21th int. symposium on the scie. basis for nuclear waste management XXI; 1997, Switzerland vol. 506, p. 535-542. Bourhila N., Thomas N., Palleau J., Torres J., Bernard C, Madar R.. Applied Surface Science. 1995, vol. 91, p.175-181. Brunaver S., Grumete P. H., Teller E., “Adsorption of Gases in Multimolecular Layers”,: J. Am. Chem. Soc., 1938, vol. 60, p. 309-19 Cahn R. W., Haasen P., Kramer E. J., Materials Science and Technology, VCH, Federal Republic of Germany, 1996 Castrillejo Y., García M.A., Barrado E., Pasquier P., Picard G., Electrochim. Acta. 1995, vol. 40, p. 2731 Castrillejo Y., Martinez A.M., Vega M., Barrado E., Picard G., J. Electroanal. Chem. 1995, vol. 397, p. 139. Castro M.L., Tesis Doctoral, Universidad Nacional del Centro de la Provincia de Buenos Aires, Argentina, 1999 Chang Y. N., Wei F. I., Journal of Materials Science. 1991, vol. 26, p. 3693-3698 Chaudhary A.J., Donaldson J.D., Grimes S.M., J. Chem. Tech. Biotechnol. 1994, vol. 61, p. 293-297 . Chaudhary J.A., Donaldson J. D., Grimes S. M., “Heavy-Metals in the Environment .5. The Use of High Copper-Zinc Residues in the Zinc-Chloride Process and the Recovery of Copper as Anhydrous Copper(II) Chloride”, J. Chem. Tech. Biotechnol, 1994, vol. 61, p. 293-97. Christian J. W., The Theory of transformations in metals and alloys. Pergamon Press, Oxford, 1965 De Beauchamp R. L., Preparation of Anhydrous Aluminium Chloride, Inf. Circ. U.S. Bur. Mines, n° 8412, 1969. De Micco G., Bohé A. E., Pasquevich D. M., Journal of Alloys and Compounds, 2007, vol. 437, nro. 1-2, p. 351-359 Dell’Anna A., Emmenegger F.P., Helv. Chim. Acta. 1975, vol. 58, p. 1145 Djona M., Allain E., Gaballah I., “Kinetics of chlorination and carbochlorination of molybdenum trioxide”, Metall. Mater. Trans. B, 1995, vol. 26B, p. 703-710 Emmenegger F. P., Rohrbasser C., Schläpfer W., Inorg. Nucl. Chem. Letters. 1976, vol. 12, p. 127-131. Ferry D., Castrillejo Y., Picard G., Electrochim. Acta. 1988., vol. 33, p. 1661 Ferry D., Castrillejo Y., Picard G., Electrochim. Acta. 1989, vol. 34, p. 313 Fletcher A. J., Lloyd T. D., J. of Inst. of Met. 1970, vol. 98, p. 188. Flynn J.H., J. of Thermal Anal., 1988, vol. 34, p. 367-381 . Furnas C. ed., Roger`s Industrial Chemistry, Van Nostrand, New York, vol. 1, 1942, ch. 2, p. 460. Gaballah I., Djona M., Allain E., “Kinetics of chlorination and carbochlorination of vanadium pentoxide”, Metall. Mater. Trans. B, 1995, vol. 26B, p. 711-718. Gaballah I., Djona M., Mugica J. C., Solozabal R., Resources, Conservation and Recycling. 1994, vol. 10, nro. 1-2, p. 87-96. Galvele J. R., Duffó G. S., “Degradación de materiales corrosión”, Monografía tecnológica nro. 3., UNSAM, CNEA, Instituto Sabato, Buenos Aires, 2006. Garcia M., Castrillejo Y., Pasquier P., Picard G., Molten Salt Forum. 1993/1994, vol. 1-2, p. 47. Geiger G.H:, Poirier D.R., Transport Phenomena in Metallurgy, Addison-Wesley Publishing Company, Inc., MA, 1973, p. 468. Gennari, F.C., Pasquevich D.M., “Kinetics of chlorination of hematite”. Thermochimica Acta. 1996, vol. 284, p. 325-339. Goldstein JI, Newbury DE, Echlin P; Scanning electron microcopy and X-ray microanalysis. Plenum Press, New York, 1992. González J. A., Gennari F. C., Ruiz M. C., Bohé A. E., Pasquevich D. M., Trans. of the Inst. of Min. and Met. Section C, 1998, vol. 107, p. 130-138 Helmboldt O., Hudson L. K., Misra C., Wefers K, Stark H., Danner M., Ullman`s Encyclopedia of Industrial Chemistry, 6th edn, 2002, Electronic Release. Aluminium Compounds, Inorganic – Aluminium Chloride Hildenbranda D. L., Lau, K. H., Thermochemistry of ZnCl(g), Journal of Chemical Physics, vol. 111, nro. 3, 15 july 1999. Hills, A.W. “The importance of convective mass transfer in the reduction of hematite”. Metallurgical Transactions B. 1978, vol 9B, p.121-128. IAEA (1996) “Clearance levels for radionuclides in solid materials. Applications of exemption principles” Interim report for comment (TECDOC-855-IAEA, 1996) Ishida M., Wen C. Y., “Effectiveness factors and instability in solid-gas reactions”, Chemical Engineering Science, 1968, vol. 23, p. 125-137. Johnson W. A., Mehl R. F. Trans. Am. Inst. Min. (Metall.) Engs. 1939, vol.135, p. 416 (JCPDS) Joint Committee for Powder Diffraction Standards, International Center for Diffraction Data. Powder Diffraction File, 2001. Kanari N., Gaballah I., Allain E., Menad N., Metallurgical and Material Transactions B. 1999, vol 30B, p. 567-576 Kanari N., Gaballah I., Allain E., Thermochimica Acta. 2001, vol. 373, p 75-93. Kempen A. T. W., Sommer F., Mittemeijer E. J. Acta Mater. 2002a, vol. 50, p. 1319 Kempen, A. T. W., Sommer F., Mittemeijer E. J. J. Mater. Sci. 2002, vol. 37, p. 13 Kennon N. F., Dunne D. P., Middleton. L., Met. Trans. A, 1982, vol. 13, p. 551 Kim S.K.,“The determination of the kinetics of gas-solid reactions by the nonisothermal technique”, Ph.D. Thesis, University of Utah, 1981. Kumar M. L., Warren Kun Li, Garry W., Canadian Metallurgical Quarterly. 1987, vol. 26, nro1, p. 29-36. Laidler, K.J.; Meiser, J.H., Physical Chemistry, Boston , Houghton Mifflin , 2da edición, 1995. Landsbrg A., Journal of Less-Common Metals. 1990, vol. 159, p. 163-172 Lee E.-S., Kim Y. G., Met. Trans. A, 1990, vol 21, p.1681 Lee E.-S., Kim Y.G., Scripta Met. et Mater.1990a, vol. 24, p. 745. Lide D. R. ed., CRC Handbook of Chemistry and Physics, , 85th ed. 2004-2005, CRC Press. p. 4-95 Mannan S. K., Vaidehi G., Vijayalakdhmi M., Seetharaman V. J. Mater. Sci. 1984, vol.19, p. 2465. Massalski, T. B., King, H. W. Progr. Mater. Sci. 1961, vol. 10, p. 43. Matsumaru K., Susa M., Nagata K., Tetsu-To-Hagane/Journal of the Iron and Steel Institute of Japan. 1996, vol. 82, nro.10, p. 1-6. Matsuura H., Tsukihashi F., “Chlorination kinetics of ZnO with Ar-Cl2-O2 gas and the effect of oxychloride formation”, Metall. Mater. Trans. B, 2006, vol. 37B, p. 413-20. Mittemeijer E. J. J. Mater. Sci. 1992, vol. 27, p. 3977. Nonaka R., Sugawara K., Sugawara T., “Heavy metal recovery from molten fly ashes by chlorination”, AIChE Annual Meeting Conference Proceedings, 2005, p. 5709 Norvell N. J., Process for etching an aluminium-copper alloy, U.S. Patent 4468284, http://www.freepatentsonline.com/4468284.html , 1984 Nuffield, E. W, "X ray diffraction methods", New York , Wiley ,1966 Paige, R E, Gibson G W, Rhode K L, “The effect of Silicon on fabrication and Reprocessing of aluminium Alloys Reactor Fuels”. USDOE Report IN-1194, Idaho Nuclear Corporation, National Reactor Testing Station. Idaho Falls, 1968 Pasquevich D. M. Thermochimica Acta, 1990, vol. 167, p. 91 Pasquevich D. M., Caneiro A. M.. “A Thermogravimetric Analyzer for Corrosive Atmospheres and its applications to the Chlorination of ZrO2-C Mixture”. Thermochimica Acta, 1989, vol. 156, nro. 2, p. 275-283. Pasquevich D. M., Gaviría J. P., Esquivel M., Bohé A. E., “Intrinsic kinetic of the chlorination of hematite powder between 898 and 1023 K”, Metall. Mater. Trans. B, 2006, vol. 37B, nro. 4, p. 589-597. Pasquevich D.M., “Estudio de la Reacción de Cloración de la Circonia en presencia de Carbono. Desarrollo de un sistema termogravimétrico especialmente adecuado para el estudio cinético de reacciones de cloración de óxidos”. Tesis doctoral, Universidad Nacional de La Plata, 1990. Petzow, G., Effenberg, G. “Ternary Alloys A Comprehensive Compendium of Evaluated Constitutional Data and Phase Diagrams”, Weinhein; Basel, Switzerland/ Cambridge/New York , NY: VCH, Vol. V, 1992. Piccolo L., Ghirga M., Calcagno B., Process for preparing aluminium trichloride, US Pat. 3812241, Societa Italiana Resine S. I. R. S. P. A., Milan, Italy, 1974. Pilling N. B., Bedworth R. E., J. Instit. Metals, 1923, vol. 29, p. 539. Porter D.A., Easterling K.E., “Phase transformation in metals and alloys”, Chapman and Hall, 1981. Rapacioli, R., Ahlers, M. Scripta Met., 1977, vol. 11, p. 1147 Remeika J. P., Batlogg B., Mat. Res. Bull.1980, vol. 15, p.1179-1182. Richardson H. W., Ullman`s Encyclopedia of Industrial Chemistry, 6th edn, 2002, Electronic Release. Copper Compounds – Salts and Basic Salts Roine A. Roine, Outokumpu HSC chemistry for Windows, 93001-ORGT version 2.0 Outokumpu Research Oy Information Service, 1994. Romero R.,. Pelegrina J. L. Mater. Sci. and Eng. 2003, vol. A354, p. 243 Sesselmann W., Chuang T. J., Surface Science. 1986, vol. 176, nro. 1-2, p. 32-66. Sesselmann W., Chuang T. J., Surface Science. 1986a, vol. 176, nro. 1-2, p. 67-90 Siemens R. E., Jong B. W., Russell J. H., “Potential of spent catalysts as a source of critical metals”, Conservation & Recycling, 1986, vol. 9, nro. 2, p.189-96. Son S. H., Tsukihashi F. “Vapor pressure measurements of zinc oxychloride”, ISIJ International, 2003, vol. 9, p. 1356-1361. Son S. H., Tsukihashi F., “Vapor pressure measurements of zinc oxychloride”, Journal of Physics and Chemistry of Solids, 2005, vol. 66, p.392-395. Szekely, J., Evans J.W., Sohn, H.Y.“Gas Solid Reactions”, Academic Press, New York, 1965. Tamagawa T., Fu N. X., Kobayashi M., Iwasaki I. Minerals and Metallurgical Processing. 2001, vol. 18, nro. 4, p. 209-214. Tee J.K.S., Fray D.J.,“Recycling of galvanised steel scrap using chlorination”,: Ironmaking and Steelmaking, 2005, vol. 32, nro. 6, p. 509-14 Thomas B. K., Fray D. J. “Leaching of oxidic zinc materials with chlorine and chlorine hydrate,”, Metall. Trans. B, 1981, vol. 12B, p. 281-5 Thomas B. K., Fray D. J., “Leaching of zinc and zinc alloys with chlorine and chlorine hydrate,” Metall. Trans. B, 1981a, vol. 12B, p. 559-63. Tití-Manyaka R., Iwasaki I., SME Transactions, 1972, vol. 252, pp. 307-313. Tití-Manyaka R., Iwasaki I., Society of Mining Engineers, AIME. 1976, vol. 260, p. 282-288 Ullman`s Encyclopedia of Industrial Chemistry, 6th edition, 2002, electronic release. Villars P., Pearson’s Handbook of Crystallographica Data for Intermetallic Phases, Materials Park , ASM ,1991, p. 3027. Virčíková E., Molnár L, Resources, Conservation and Recycling. 1992, vol. 6, nro. 2, p. 133 - 138. Wheeler A., Advances in Catalysis, Academic Press Inc., New York, N. Y., 1951, vol. 3, p. 249-327 Yang F., Hlavacek V., “Kinetic study of chlorination of niobium(V) oxide with chlorine and carbon monoxide”, Powder Technology, 1999, vol. 102, p. 177-183. Yon S., Han Y., J. Mater. Sci. 1986, vol.21, p. 2711 Zhang B., Yan X., Shibata K., Tada M., Hirasawa M., “Novel process for recycling metallic elements from mixtures of metal oxide wastes and waste polyvinyl chloride”, High Temperature Materials and Processes, 1999, vol. 18, nro. 4, p 197-211. |
| Materias: | Química > Química analítica Física > Física de materiales Metalurgia > Aleaciones |
| Divisiones: | Presidencia > Gcia. Complejo Tecnológico Pilcaniyeu |
| Código ID: | 304 |
| Depositado Por: | Marisa G. Velazco Aldao |
| Depositado En: | 01 Feb 2012 10:38 |
| Última Modificación: | 19 Dic 2012 10:08 |
Personal del repositorio solamente: página de control del documento
