Radiolytic effects on the redox behaviour of Np, Pu and Am in concentrated salt solutions
- 1. Technische Univ. Muenchen, Garching (Germany, F.R.). Inst. fuer Radiochemie
Description
In the course of solubility studies with Am(III) and Pu(IV) hydroxide in the presence of high chloride concentrations, a radiolytically induced oxidation of Am(V) and Pu(VI) has been observed by spectrophotometrical measurements. This oxidation process has been seen to be dependent on the specific α-activity in the solution, as well as on the pH-value and the chloride concentration. During the experiments, a considerable increase in the redox potential to values of over +1000 mV could be measured. The results are interpreted to reveal a radiolytic formation of oxidizing chlorine species, and their reaction with the actinide ions present in the solution. A reaction pattern is presented for the radiolysis of concentrated chloride solutions which describes all the phenomena observed. This pattern and the Eh-pH-diagrams of Np, Pu and Am are used as a basis for discussing the redox behaviour of actinides in salt solution. (orig.)
Abstract (German)
Im Rahmen von Loeslichkeitsuntersuchungen mit Am(III)- und Pu(IV)-Hydroxid in Gegenwart hoher Chlorid-Konzentrationen wurde durch spektrophotometrische Messungen eine radiolytisch induzierte Oxidation zu Am(V) bzw. Pu(VI) beobachtet. Diese Oxidation war abhaengig von der spezifischen α-Aktivitaet in der Loesung sowie vom pH-Wert und der Chlorid-Konzentration. Im Verlauf der Loeslichkeitsexperimente konnte gleichzeitig ein betraechtlicher Anstieg des Redoxpotentials auf Werte von ueber +1000 mV gemessen werden. Diese Ergebnisse werden interpretiert als radiolytische Bildung von oxidierenden Chlor-Spezies und deren Reaktion mit den in der Loesung vorhandenen Aktinoid-Ionen. Ein Reaktionsschema fuer die Radiolyse von konzentrierten Chlorid-Loesungen, welches alle beobachteten Phaenomene befriedigend beschreibt, wird vorgestellt. Anhand dieses Schemas und der Eh-pH-Diagramme von Np, Pu und Am wird das Redoxverhalten der Aktinoide in Salzloesungen diskutiert. (orig.)Additional details
Additional titles
- Original title (German)
- Radiolyse-Einfluss auf das Redoxverhalten von Np, Pu und Am in konzentrierten Salzloesungen
Publishing Information
- ISBN
- 3-88314-578-5
- Imprint Title
- Chemistry and migration behaviour of the actinides and fission products in natural aquatic systems
- Imprint Pagination
- 341 p.
- Journal Page Range
- p. 64-76.
- Report number
- PTB-SE--14
Conference
- Title
- 66. PTB-seminar 'Chemistry and migration behaviour of the actinides and fission products in natural aquatic systems'.
- Dates
- 24-25 Apr 1986.
- Place
- Garching (Germany, F.R.).
INIS
- Country of Publication
- Germany
- Country of Input or Organization
- Germany
- INIS RN
- 18098018
- Subject category
- S38: RADIATION CHEMISTRY, RADIOCHEMISTRY AND NUCLEAR CHEMISTRY;
- Resource subtype / Literary indicator
- Conference
- Descriptors DEI
- ALPHA PARTICLES; AMERICIUM HYDROXIDES; AQUEOUS SOLUTIONS; BRINES; CHEMICAL REACTION KINETICS; GEOCHEMISTRY; NEPTUNIUM; OXIDATION; PH VALUE; PLUTONIUM HYDROXIDES; RADIOLYSIS; REDOX POTENTIAL; SODIUM CHLORIDES; SOLUBILITY
- Descriptors DEC
- ACTINIDE COMPOUNDS; ACTINIDES; ALKALI METAL COMPOUNDS; AMERICIUM COMPOUNDS; CHARGED PARTICLES; CHEMICAL RADIATION EFFECTS; CHEMICAL REACTIONS; CHLORIDES; CHLORINE COMPOUNDS; DECOMPOSITION; DISPERSIONS; ELEMENTS; HALIDES; HALOGEN COMPOUNDS; HELIUM IONS; HOMOGENEOUS MIXTURES; HYDROGEN COMPOUNDS; HYDROXIDES; IONIZING RADIATIONS; IONS; KINETICS; METALS; MIXTURES; OXYGEN COMPOUNDS; PLUTONIUM COMPOUNDS; RADIATION EFFECTS; RADIATIONS; REACTION KINETICS; SODIUM COMPOUNDS; SOLUTIONS; TRANSPLUTONIUM COMPOUNDS; TRANSURANIUM COMPOUNDS; TRANSURANIUM ELEMENTS
Optional Information
- Notes
- Imprint:Chemie und Migrationsverhalten der Aktinoide und Spaltprodukte in natuerlichen aquatischen Systemen.;Vortraege.