IAEA-TECDOC-301 THE BEHAVIOUR OF RADIUM IN WATERWAYS AND AQUIFERS FINAL REPORT OF THE CO-ORDINATED RESEARCH PROGRAMME ON SOURCE, DISTRIBUTION, MOVEMENT AND DEPOSITION OF RADIUM IN INLAND WATERWAYS AND AQUIFERS SPONSORED BY THE INTERNATIONAL ATOMIC ENERGY AGENCY FROM 1976 TO 1980 A TECHNICAL DOCUMENT ISSUED BY THE INTERNATIONAL ATOMIC ENERGY AGENCY. VIENNA, 1984 THE BEHAVIOUR OF RADIUM IN WATERWAYS AND AQUIFERS IAEA, VIENNA, 1984 IAEA-TECDOC-301 Printed by the IAEA in Austria January 1984 PLEASE BE AWARE THAT ALL OF THE MISSING PAGES IN THIS DOCUMENT WERE ORIGINALLY BLANK The IAEA does not maintain stocks of reports in this series. However, microfiche copie f thesso e reportobtainee b n sca d from INIS Clearinghouse International Atomic Energy Agency Wagramerstrasse 5 P.O. Box 100 A-1400 Vienna, Austria Orders shoul accompaniee db prepaymeny db f Austriao t n Schillings 60.00 fore for e chequ th a f mth IAEm f o n i n o i r Aeo microfiche service coupons which may be ordered separately from the INIS Clearinghouse. FOREWORD In 1975, radiusignificana knows e b mwa o nt t contaminane th n ti liquid and solid wastes from uranium mining and milling and so the IAEA began a coordinated research programme on "The source, distribution, movemen depositiod tan radiuf no inlann mi d waterway aquifers"d san . The primary aim of this coordinated research programme was to produc erepora radiun o t m behaviou aquatie th n ri c environment froe mth point of view of health protection. It was no easy matter to draft this repor eacs a t h principal autho chaptea f ro s require rwa submio t d n ta integrated report on the work produced by the other laboratories participatin contexprogramme e f th thith placo o t n n f sl i i go t d eal ean the work publishe literaturee th n i d . All the authors set about doing this on the basis of the data available to them at the time, and the chapters thus forced together can in general, albeit with varying degree successf so consideree ,b o t d cove mose rth t important aspect e subjectth f so . Technical and administrative aspects are dealt with in the relevant chapter, so at this point we shall only mention that the Scientific Secretaries were, successively: P.A. Bonhote (1975-1976), L. Farges (1976-1979 Kirchman. R d )an n (1980). It is hoped that the data produced by the various laboratories participating in the programme will be of great value to those authorities responsibl assessinr fo e consquencee th g radiuf so m releases to inland waters and to those responsible for setting discharge limits. René KIRCHMANN 1982-10-01 TABLE OF CONTENTS PREFACE.......................................................................................................................... 9 HISTORY........................................................................................................................... 12 INTRODUCTION..............................................................................................................3 1 . 1. RADIUM HISTORICAA : L INTRODUCTIO OVERVIEW...........................D NAN 5 1 . 1.1. The discovery of radium ..................................................................................... 17 1.2. Using the properties of radium ........................................................................... 17 1.3. Awaking to the consciousness of dangers ........................................................ 18 1.3.1. Realizing health hazards of radium ......................................................... 18 1.3.2. Considering environmental effect radiuf o s m .........................................9 1 . References.......................................................................................................................... 20 2. ANALYTICAL METHOD . Kobal,S(I A.R. Williams) ...............................................3 2 . 2.1. Methods for measuring 226Ra .............................................................................. 25 2.1.1. Direct measurement of radium activity................................................... 25 2.1.2. Spectrometry of radium decay products .................................................. 25 2.1.3. Gross counting methods ........................................................................6 2 . 2.2. Methods for preparing and analysing samples...................................................... 30 2.2.1. Waters..................................................................................................... 30 2.2.2. Soil, sediment, ore, tailings ..................................................................... 33 2.2.3. Food .....................................................................................................4 3 . 2.2.4. Animal materials..................................................................................... 35 2.3. Interpretation of results ..................................................................................... 36 2.3.1. Components of the random precision error ............................................ 36 2.3.2. Inter-laboratory comparison ................................................................... 38 2.4. Conclusions and recommendations ..................................................................... 39 References.......................................................................................................................... 44 . 3 DISTRIBUTIO NATURN I E (M.A.R. lyengar)........................................................7 5 3.1. Introduction ......................................................................................................9 5 . 3.2. Groundwaters ....................................................................................................0 6 . 3.2.1R. a226 distribution in selected geographic regions .................................... 60 3.2.2. Discussion............................................................................................... 61 3.3. Surface waters ...................................................................................................2 6 . 3.3.1. BaselinRea226 levels in surface waters in mining areas ............................ 62 3.3.2. Discussion .............................................................................................. 63 3.4. Stream sediments ...............................................................................................4 6 . 3.4.1. 226Ra distribution and movement behaviour in stream sediments ........... 64 3.4.2. Discussion .............................................................................................. 65 3.5. Biota................................................................................................................... 65 3.5.1. Rshes ....................................................................................................5 6 . 3.5.2. Algae and plankton................................................................................. 67 3.5.3. Aquatic macrophytes.............................................................................. 68 3.5.4. Mollusca.................................................................................................. 69 3.6. Conclusions........................................................................................................0 7 . References.......................................................................................................................... 85 4. TECHNOLOGICAL ENHANCEMENT (A.S.M. de Jesus) .......................................... 87 4.1. Introduction ......................................................................................................9 8 . 4.2. Source term .......................................................................................................0 9 . 4.2.1. Uranium ................................................................................................ 90 4.2.2. Phosphates.............................................................................................0 9 . 4.2.3. Coal.......................................................................................................1 9 . 4.2.4. Others....................................................................................................1 9 . 4.3. Uranium minin milling...............................................................................d gan 1 9 . 4.3.1. Economic aspects ................................................................................... 91 4.3.2. Aci alkalin. dvs e leaching .......................................................................2 9 . 4.3.3. Underground vs. open-pit mining ............................................................ 92 4.3.4. Climatological considerations.................................................................2 9 . 4.3.5. Site-specific aspects ................................................................................ 93 4.3.6. Tailings and effluents.............................................................................. 93 4.4. Ra-226 distributio aqueoue th n i s environment...............................................3 9 . 4.4.1. Ground water .......................................................................................... 94 4.4.2. Surface water.........................................................................................8 9 . 4.4.3. Stream sediment..................................................................................... 102 4.4.4. Biota......................................................................................................5