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Title: Hydrothermal interactions between calcine, glass, spent fuel, and ceramic-waste forms with representative shale-repository rocks

Abstract

A prototype waste glass (PNL 76-68), a prototype ceramic (SPC-2), a raw PW-7a calcine, and a simulated spent fuel were reacted individually with six shales in the presence of water in sealed gold capsules. Conditions were (usually) 1:1:1 waste:shale:water by weight, P = 30 MPa, T = 100, 200, 300 and 400/sup 0/C. Reaction products were characterized by optical microscopic and SEM examination, EDX analysis, x-ray diffraction analysis, and Gandolfi X-ray analysis. The shales react with the waste forms presumably by dissolution in water followed by reaction between the solution and the shale minerals. Degree of reaction ranges from barely detectable at 100/sup 0/C to almost complete alteration of the waste forms and shales at 400/sup 0/C. Cesium extracted from the waste forms reacts with alumino-silicate minerals to form a pollucite-analcime solid solution at lower temperatures. It is shown that the observed gradual disappearance of pollucite in higher temperature runs can be explained by the decomposition of the pollucite-analcime solid solution into a cesium-rich pollucite plus feldspar. The seeming disappearance of pollucite from high temperature runs need not imply loss of cesium fixation. The uranium reacts with silicate minerals under oxidizing conditions to form alkali uranyl silicates (of which weeksitemore » is the most common example). Shales containing sulfide minerals or organic materials maintain a reducing environment which keeps uranium (and presumably transuranic elements) in the far less soluble tetravalent state. Powellite, CaMoO/sub 4/, appears frequently as the reaction product of molybdenum. 23 figures, 15 tables.« less

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
Pennsylvania State Univ., University Park (USA). Materials Research Lab.
OSTI Identifier:
6749070
Report Number(s):
ONWI-306
ON: DE83002640
DOE Contract Number:  
AC06-76RL01830
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; CALCINED WASTES; WASTE-ROCK INTERACTIONS; RADIOACTIVE WASTE STORAGE; SHALES; SPENT FUELS; CERAMICS; ELECTRON DIFFRACTION; GLASS; HIGH TEMPERATURE; HYDROTHERMAL ALTERATION; MICROSTRUCTURE; MINERALS; OPTICAL MICROSCOPY; SCANNING ELECTRON MICROSCOPY; TEMPERATURE DEPENDENCE; UNDERGROUND STORAGE; X-RAY DIFFRACTION; COHERENT SCATTERING; CRYSTAL STRUCTURE; DIFFRACTION; ELECTRON MICROSCOPY; ENERGY SOURCES; FUELS; MANAGEMENT; MATERIALS; MICROSCOPY; NUCLEAR FUELS; RADIOACTIVE MATERIALS; RADIOACTIVE WASTES; REACTOR MATERIALS; ROCKS; SCATTERING; SEDIMENTARY ROCKS; STORAGE; WASTE MANAGEMENT; WASTE STORAGE; WASTES; 052002* - Nuclear Fuels- Waste Disposal & Storage; 053000 - Nuclear Fuels- Environmental Aspects

Citation Formats

Freeborn, W P, Zolensky, M, Scheetz, B E, Komarneni, S, McCarthy, G J, and White, W B. Hydrothermal interactions between calcine, glass, spent fuel, and ceramic-waste forms with representative shale-repository rocks. United States: N. p., 1982. Web.
Freeborn, W P, Zolensky, M, Scheetz, B E, Komarneni, S, McCarthy, G J, & White, W B. Hydrothermal interactions between calcine, glass, spent fuel, and ceramic-waste forms with representative shale-repository rocks. United States.
Freeborn, W P, Zolensky, M, Scheetz, B E, Komarneni, S, McCarthy, G J, and White, W B. Fri . "Hydrothermal interactions between calcine, glass, spent fuel, and ceramic-waste forms with representative shale-repository rocks". United States.
@article{osti_6749070,
title = {Hydrothermal interactions between calcine, glass, spent fuel, and ceramic-waste forms with representative shale-repository rocks},
author = {Freeborn, W P and Zolensky, M and Scheetz, B E and Komarneni, S and McCarthy, G J and White, W B},
abstractNote = {A prototype waste glass (PNL 76-68), a prototype ceramic (SPC-2), a raw PW-7a calcine, and a simulated spent fuel were reacted individually with six shales in the presence of water in sealed gold capsules. Conditions were (usually) 1:1:1 waste:shale:water by weight, P = 30 MPa, T = 100, 200, 300 and 400/sup 0/C. Reaction products were characterized by optical microscopic and SEM examination, EDX analysis, x-ray diffraction analysis, and Gandolfi X-ray analysis. The shales react with the waste forms presumably by dissolution in water followed by reaction between the solution and the shale minerals. Degree of reaction ranges from barely detectable at 100/sup 0/C to almost complete alteration of the waste forms and shales at 400/sup 0/C. Cesium extracted from the waste forms reacts with alumino-silicate minerals to form a pollucite-analcime solid solution at lower temperatures. It is shown that the observed gradual disappearance of pollucite in higher temperature runs can be explained by the decomposition of the pollucite-analcime solid solution into a cesium-rich pollucite plus feldspar. The seeming disappearance of pollucite from high temperature runs need not imply loss of cesium fixation. The uranium reacts with silicate minerals under oxidizing conditions to form alkali uranyl silicates (of which weeksite is the most common example). Shales containing sulfide minerals or organic materials maintain a reducing environment which keeps uranium (and presumably transuranic elements) in the far less soluble tetravalent state. Powellite, CaMoO/sub 4/, appears frequently as the reaction product of molybdenum. 23 figures, 15 tables.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {1982},
month = {10}
}

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