The speciation, stability, solubility and biodegradation of organic co-contaminant radionuclide complexes: a review.

The potential migration of radionuclides is of concern at contaminated land sites and, in the long term, waste repositories. Pathways of migration need to be characterised on a predictive level so that management decisions can be made with confidence. A pathway that is relatively poorly understood at present is radionuclide solubilisation due to complexation by organic complexing agents that are present in mixed radioactive wastes, and at radioactively contaminated land sites. Interactions of the complexing agents with radionuclides and the host environment, and the response to changes in the physicochemical conditions make their role far from simple to elucidate. In addition, chemical and biodegradation of the organic materials may be important. In this paper, key co-contaminant organics are reviewed with emphasis on their environmental fate and impact on radionuclide migration.

[1]  B. Gyurcsik,et al.  Coordination chemistry of polyhydroxy acids: role of the hydroxy groups , 1998 .

[2]  R. D. Orr,et al.  Radionuclide-Chelating Agent Complexes in Low-Level Radioactive Decontamination Waste; Stability, Adsorption and Transport Potential , 2002 .

[3]  S. Brooks,et al.  Sustained bacterial reduction of CoIIIEDTA- in the presence of competing geochemical oxidation during dynamic flow , 1999 .

[4]  D. Reed,et al.  Radiotoxicity of plutonium in NTA-degrading Chelatobacter heintzii cell suspensions , 2004, Biodegradation.

[5]  M. Glaus,et al.  Degradation of Cellulosic Materials Under the Alkaline Conditions of a Cementitious Repository for Low- and Intermediate-Level Radioactive Waste. II. Degradation Kinetics , 1999 .

[6]  E. Wieland,et al.  The effect of α-isosaccharinic acid on the stability of and Th(IV) uptake by hardened cement paste , 2002 .

[7]  M. Glaus,et al.  Review of the kinetics of alkaline degradation of cellulose in view of its relevance for safety assessment of radioactive waste repositories , 1997 .

[8]  P. Warwick,et al.  Studies on some divalent metal α-isosaccharinic acid complexes , 2006 .

[9]  T. Egli,et al.  Dynamics of Substrate Consumption and Enzyme Synthesis in Chelatobacter heintzii during Growth in Carbon-Limited Continuous Culture with Different Mixtures of Glucose and Nitrilotriacetate , 1996, Applied and environmental microbiology.

[10]  S. Canonica,et al.  Determination of the Reaction Quantum Yield for the Photochemical Degradation of Fe(III)-EDTA: Implications for the Environmental Fate of EDTA in Surface Waters. , 1995, Environmental science & technology.

[11]  S. D. Harvey,et al.  Degradation of Metal−Nitrilotriacetate Complexes by Chelatobacter heintzii , 1996 .

[12]  S. Brooks,et al.  Multispecies transport of metal-EDTA complexes and chromate through undisturbed columns of weathered fractured saprolite. , 2000 .

[13]  P. Worsfold,et al.  Effect of organic co-contaminants on technetium and rhenium speciation and solubility under reducing conditions. , 2006, Environmental science & technology.

[14]  P. Reiller,et al.  Effect of organics on selenite uptake by cementitious materials. , 2006, Waste management.

[15]  C. Oviedo,et al.  EDTA: the chelating agent under environmental scrutiny , 2003 .

[16]  P. Warwick,et al.  Complexation of Ni(II) by α-isosaccharinic acid and gluconic acid from pH 7 to pH 13 , 2003 .

[17]  J. McCarthy,et al.  Mobilization of transuranic radionuclides from disposal trenches by natural organic matter , 1998 .

[18]  P. Worsfold,et al.  Characterisation of thorium-ethylenediaminetetraacetic acid and thorium-nitrilotriacetic acid species by electrospray ionisation-mass spectrometry. , 2007, Analytica chimica acta.

[19]  L. Rao,et al.  The Influence of Isosaccharinic Acid on the Solubility of Np(IV) Hydrous Oxide , 1998 .

[20]  J. Vanbriesen,et al.  The rate-controlling substrate of nitrilotriacetate for biodegradation by chelatobacter heintzii , 2000 .

[21]  M. Erk,et al.  The interactions of 54Mn with aminopolycarboxylic acids in aquatic systems , 1996 .

[22]  L. V. Van Loon,et al.  Degradation of Cellulosic Materials under the Alkaline Conditions of a Cementitious Repository for Low- and Intermediate Level Radioactive Waste. Part III: Effect of Degradation Products on the Sorption of Radionuclides on Feldspar , 1999 .

[23]  B. Rittmann,et al.  Subsurface interactions of actinide species and microorganisms: Implications for the bioremediation of actinide-organic mixtures , 1999 .

[24]  Wayne H. Smith,et al.  EDTA and mixed-ligand complexes of tetravalent and trivalent plutonium. , 2004, Inorganic chemistry.

[25]  G. Choppin,et al.  Thermodynamic model for the solubility of PuO2(am) in the aqueous Na+-H+-OH--Cl--H2O-ethylenediaminetetraacetate system , 2001 .

[26]  R. Butcher,et al.  Study on some metal(III) complexes with pyrazine-2-carboxylic and pyridine-2-carboxylic acids , 2001 .

[27]  E. Wieland,et al.  The effect of isosaccharinic acid and gluconic acid on the retention of Eu(III), Am(III) and Th(IV) by calcite , 2005 .

[28]  F. Livens,et al.  Uranyl monopicolinate complexes , 1998 .

[29]  G. Choppin,et al.  Coordination modes in the formation of the ternary Am(III), Cm(III), and Eu(III) complexes with EDTA and NTA: TRLFS, 13C NMR, EXAFS, and thermodynamics of the complexation. , 2006, Inorganic chemistry.

[30]  G. M. Escandar,et al.  Interaction of divalent metal ions withd-gluconic acid in the solid phase and aqueous solution , 1996 .

[31]  S. Williams,et al.  The Effect of Cement Additives on Radionuclide Solubilities , 1998 .

[32]  Bert Allard,et al.  Alkaline Degradation of Cellulose: Mechanisms and Kinetics , 2003 .

[33]  J. Vanbriesen,et al.  Mathematical Modelling of the Effects of Aerobic and Anaerobic Chelate Biodegradation on Actinide Speciation , 1998 .

[34]  T. E. Ward Aerobic and anaerobic biodegradation of nitrilotriacetate in subsurface soils. , 1986, Ecotoxicology and Environmental Safety.

[35]  T. Egli,et al.  Biodegradation of metal-complexing aminopolycarboxylic acids. , 2001, Journal of bioscience and bioengineering.

[36]  P. Warwick,et al.  Modelling the effect of humic substances on the transport of europium through porous media : a comparison of equilibrium and equilibrium/kinetic models , 2000 .

[37]  D. Read,et al.  The migration of uranium through Clashach Sandstone: the role of low molecular weight organics in enhancing radionuclide transport , 1998 .

[38]  C. J. Knill,et al.  Degradation of cellulose under alkaline conditions , 2003 .

[39]  G. Choppin,et al.  Thermodynamics and the structural aspects of the ternary complexes of Am(III), Cm(III) and Eu(III) with Ox and EDTA + Ox. , 2006, Dalton transactions.

[40]  Environmental fate and microbial degradation of aminopolycarboxylic acids. , 2001, FEMS microbiology reviews.

[41]  N. Hess,et al.  Comprehensive Thermodynamic Model Applicable to Highly Acidic to Basic Conditions for Isosaccharinate Reactions with Ca(II) and Np(IV) , 2003 .

[42]  A. Martell,et al.  Mixed Ligand Chelates of Thorium(IV) , 1964 .

[43]  N. Hess,et al.  Thermodynamic model for the solubility of ThO2(am) in the aqueous Na+-H+-OH--NO3--H2O-EDTA system , 2003 .

[44]  S. Brooks,et al.  pH-Dependent fate and transport of NTA-complexed cobalt through undisturbed cores of fractured shale saprolite. , 2002, Journal of contaminant hydrology.

[45]  M. Glaus,et al.  EVIDENCE FOR THE EXISTENCE OF COMPLEXES BETWEEN TH(IV) AND ALPHA -ISOSACCHARINIC ACID UNDER ALKALINE CONDITIONS , 1999 .

[46]  D. Crerar,et al.  Migration of Radioactive Wastes: Radionuclide Mobilization by Complexing Agents , 1978, Science.

[47]  L. Rao,et al.  Protonation and complexation of isosaccharinic acid with U(VI) and Fe(III) in acidic solutions: potentiometric and calorimetric studies , 2004 .

[48]  T. Tuhkanen,et al.  Photodegradation of ethylenediaminetetraacetic acid (EDTA) and ethylenediamine disuccinic acid (EDDS) within natural UV radiation range. , 2001, Chemosphere.

[49]  A. Martell,et al.  Mixed Ligand Chelates of Uranium (IV)1,2 , 1967 .

[50]  I. Burke,et al.  The behaviour of technetium during microbial reduction in amended soils from Dounreay, UK. , 2007, The Science of the total environment.

[51]  S. Brooks,et al.  Geochemical reactions governing the fate of Co-NTA in contact with natural subsurface materials , 2003 .

[52]  D. Camaioni,et al.  Initial laboratory studies into the chemical and radiological aging of organic materials in underground storage tanks at the Hanford Complex , 1994 .

[53]  L. V. Van Loon,et al.  Complexation of Th(IV) and Eu(III) by α-isosaccharinic acid under alkaline conditions , 2001 .

[54]  S. W. Li,et al.  Biodegradation of Synthetic Chelates in Subsurface Sediments from the Southeast Coastal Plain , 1993 .

[55]  D. Crerar,et al.  Relative degradation rates of NTA, EDTA and DTPA and environmental implications , 1980 .

[56]  S. Achatz,et al.  Degradation of cellulosic materials under the alkaline conditions of a cementitious repository for low and intermediate level radioactive waste. Part I : Identification of degradation products , 1999 .