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AECL EACL AECL Research EACL Recherche AECL EACL AECL Research EACL Recherche AECL-10851, COG-93-147, SKB TR 94-04 Final Report of the AECL/SKB Cigar Lake Analog Study Rapport definitif d'etude de 1'analogue de Cigar Lake effectuee par EACL et SKB JJ. Cramer, J.A.T Smellie MEr Uranium Deposit Waterbury Lake _ "'-'••• i-'v:-vi;.:,'...-,:,/,J:.™ Weathered Sandstone • i / ' Bleached ' 7 /' Sandstone ' / ' / /, Sandstone /'. / ' .-../ / - Main Groundwater Flow 100 m VOL 27 Ns 17 July 1994juillet AECL Research FINAL REPORT OF THE AECL/SKB CIGAR LAKE ANALOG STUDY Edited by J.J. Cramer (AECL) and J.A.T. Smellie (SKB) Whiteshell Laboratories Pinawa, Manitoba, Canada ROE 1L0 1994 AECL-10851 COG-93-147 SKB TR 94-04 RAPPORT DEFINITIF D'ETUDE DE L'ANALOGUE DE CIGAR LAKE EFFECTUÉE PAR EACL ET SKB Révisé par J. Cramer (EACL) et J. Smellie (SKB) RÉSUMÉ Le gisement d'uranium de Cigar Lake est situé dans le nord de la Saskatchewan au Canada. Ce gisement de 1,3 milliard d'années se trouve à une profondeur d'environ 450 m, sous la surface, dans un grès saturé d'eau au contact de la discordance avec les roches métamorphi- ques Précambriennes du Bouclier canadien. Le minerai d'uranium, qui contient principale- ment de l'uraninite (UO2), est entouré d'un halo riche en argile aussi bien dans le grès que dans le socle, reste très bien conservé et intact. La teneur moyenne du minerai est d'environ 8 % en poids d'U; localement, la teneur peut atteindre d'environ 55 % en poids d'U. Le gisement de Cigar Lake comporte de nombreux éléments qui sont équivalents à ceux en cours d'examen dans le contexte du concept canadien de stockage permanent des déchets de combustible nucléaire. L'étude de ces structures et processus naturels donne un aperçu précieux de la conception et de la sélection d'un site de dépôt de déchets de combustible nucléaire qui s'ensuivraient. La principale caractéristique de cet analogue est l'absence de tout indice sur la surface du minerai riche en uranium situé à 450 m de profondeur. Ceci indique que la combinaison des barrières naturelles a isolé efficacement le minerai d'uranium de l'environnement de surface. De façon plus particulière, cet analogue apporte des renseignements quant à la stabilité des déchets de combustible d'UO2, aux performan-ces des barrières à base d'argile, à la géochimie des produits de fission et aux aspects de l'interaction eau-roche. Les principales études géochimiques de ce gisement portent sur l'évolution de la composition des eaux souterraines et sur la chimie des phénomènes d'oxydo-réduction dans celles-ci en fonction de l'uranium, du fer et du sulfure. Des études de cet analogue sont menées, depuis 1984, par la coopération des propriétaires du gisement de Cigar Lake. EACL, avec le soutien d'Ontario Hydro sous les auspices du Groupe des propriétaires de réacteurs CANDU, a lancé la participation internationale en 1989 par la collaboration avec la Société suédoise de gestion du combustible et des déchets nucléaires (SKB) et, tout récemment, avec le Los Alamos National Laboratory (LANL). Le présent rapport donne les résultats des diverses études effectuées au cours des 3 ans de collaboration entre EACL et SKB ainsi qu'un résumé de l'étude effectuée par LANL. Il donne des renseignements précis sur les bases de données et modèles produits et intégre ces renseignements sous forme de conclusions à utiliser pour l'évaluation, quant à la sûreté, des concepts canadiens, suédois et américains (E-U) de stockage permanent. EACL Recherche Laboratoires de Whiteshell Pinawa, Manitoba, Canada ROE 1L0 1994 AECL-10851 COG-93-147 SKB TR 94-04 FINAL REPORT OF THE AECL/SKB CIGAR LAKE ANALOG STUDY Edited by J. Cramer (AECL) and J. Smellie (SKB) ABSTRACT The Cigar Lake uranium deposit is located in northern Saskatchewan, Canada. The 1.3- billion-year-old deposit is located at a depth of about 450 m below surface in a water- saturated sandstone at the unconformity contact with the high-grade metamorphic rocks of the Canadian Shield. The uranium mineralization, consisting primarily of uraninite (UO2), is surrounded by a clay-rich halo in both sandstone and basement rocks, and remains extremely well preserved and intact. The average grade of the mineralization is — 8 wt. % U; locally grades are as high as ~55 wt.% U. The Cigar Lake deposit has many features that parallel those being considered within the Canadian concept for disposal of nuclear fuel waste. The study of these natural structures and processes provides valuable insight toward the eventual design and site selection of a nuclear fuel waste repository. The main feature of this analog is the absence of any indication on the surface of the rich uranium ore 450 m below. This indicates that the combination of natural barriers has been effective in isolating the uranium ore from the surface environment. More specifically, the deposit provides analog information relevant to the stability of UO2 fuel waste, the performance of clay-based barriers, radionuclide migration, colloid formation, radiolysis, fission-product geochemistry and general aspects of water-rock interaction. The main geochemical studies on this deposit focus on the evolution of groundwater compositions in the deposit and on their redox chemistry with respect to the uranium, iron and sulphide systems. Since 1984, through cooperation from the owners of the Cigar Lake deposit, analog studies have been conducted. AECL, with support from Ontario Hydro under the auspices of the CANDU Owners Group, initiated international participation in 1989 through collaboration with the Swedish Nuclear Fuel and Waste Management Company (SKB) and, more recently, with the Los Alamos National Laboratory (LANL). This report gives the results of the various studies carried out during the 3-year collaboration between AECL and SKB, as well as a summary of the LANL study. It provides detailed information on the generated databases and models, and integrates this information into conclusions for use in safety assessment of the Canadian, Swedish and United States disposal concepts. AECL Research Whiteshell Laboratories Pinawa, Manitoba, Canada ROE 1L0 1994 AECL-10851 COG-93-147 SKB TR 94-04 PREFACE This report summarizes the results of the Cigar Lake Analog Study, a 3-year collaborative program (1989-1992) between Atomic Energy of Canada Limited (AECL), with support from Ontario Hydro under the auspices of the Candu Owners Group, and the Swedish Nuclear Fuel and Waste Management Company (SKB). It also includes a contribution from the Los Alamos National Laboratory, which started collaboration with AECL in 1991 with funding from the United States Department of Energy. The report represents a summary of the effort of a large group of writers from different countries and organizations, and covers a variety of technical disciplines. No attempt has been made to harmonize the style, format, spelling or technical terminology. Editorial changes were made to ensure clarity, and introductions were written for each major section. CONTENTS Page 1. EXECUTIVE SUMMARY 1 1.1 INTRODUCTION 1 1.2 OBJECTIVES 1 1.3 THE CIGAR LAKE URANIUM DEPOSIT 2 1.4 ANALOG FEATURES OF THE DEPOSIT 4 1.5 STUDY APPROACH 4 1.6 GENERAL CONCLUSIONS 5 2. INTRODUCTION 7 2.1 BACKGROUND AND OBJECTIVES 7 2.2 STUDY APPROACH AND ACTIVITIES 8 2.3 STRUCTURE AND MANAGEMENT 11 3. TASKS 14 3.1 GEOLOGY 14 3.2 MINERALOGY AND LITHOGEOCHEMISTRY 26 3.2.1 Introduction 26 3.2.2 Geochemical and isotcpic features of the host sandstone 28 and clay halo 3.2.3 Clay mineralogy and geochemistry 51 3.2.4 The Fe-O-C-S-H system 65 3.3 ORE MINERALOGY AND GEOCHEMISTRY 74 3.3.1 Introduction 74 3.3.2 Characterization of ore samples 75 3.3.3 XPS studies on uranium ore from Cigar Lake 84 3.3.4 Uraninite from Cigar Lake: Drill Cores 220 and FH-18 93 3.4 HYDROGEOLOGICAL MODELLING 104 3.4.1 Introduction 104 3.4.2 Hydrogeological data 105 3.4.3 Conceptual models 109 3.4.4 Hydraulic modelling 118 3.4.5 Discussion 133 3.4.6 Summary and conclusions 138 3.5 HYDROGEOCHEMISTRY 143 3.5.1 Introduction 143 3.5.2 Water sampling and analysis 144 3.5.3 Hydrologic and isotopic constraints 161 3.5.4 Groundwater evolution and redox geochemistry 191 3.5.5 36CI at Cigar Lake 208 CONTENTS (concl.) Page 3.6 COLLOIDS 219 3.6.1 Introduction 219 3.6.2 Colloid characterization 220 3.6.3 Behaviour during sampling 228 3.6.4 Element distributions between particles and groundwater 236 3.6.5 Colloid migration: status 238 3.7 ORGANICS AND MICROBIOLOGY 242 3.7.1 Introduction 242 3.7.2 Humic substances in groundwaters from the Cigar Lake area 243 3.7.3 Total organic carbon and other organics 255 3.7.4 Microbial research 261 3.8 NUCLEAR REACTION PRODUCT GEOCHEMISTRY 267 3.8.1 Introduction 267 3.8.2 Natural nuclear products in the Cigar Lake deposit 268 3.8.3 Oxidation by water radiolysis products 292 3.9 PERFORMANCE-ASSESSMENT-RELATED MODELLING 309 3.9.1 Introduction 309 3.9.2 Testing of solubility and speciation codes 310 3.9.3 Spent fuel dissolution modelling 326 3.9.4 Mass transport modelling 342 3.9.5 Conclusions 375 4. SUMMARY OF RESULTS AND CONCLUSIONS 380 4.1 DATABASES AND CONCEPTUAL MODELS 380 4.2 PERFORMANCE-ASSESSMENT-RELATED MODELLING 383 4.3 CONCLUSIONS 389 5. ACKNOWLEDGEMENTS 392 6. LIST OF CONTRIBUTORS 393 1. EXECUTIVE SUMMARY (J. Cramer and J. Smellie) 1.1 INTRODUCTION AECL has conducted natural analog studies on the Cigar Lake uranium deposit in northern Saskatchewan since 1984, as part of the Canadian Nuclear Fuel Waste Management Program.
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