Radiochemical Separation of Nickel for 59Ni and 63Ni Activity Determination in Nuclear Waste Samples

Alulsio Sousa Reis, Jdnior, Eliane S. C. Temba, Geraldo F. Kastner and Roberto P. G. Monteiro

Centro de Desenvolvimento da Tecnologia Nuclear — (CDTN)

Brazil

1. Introduction

For legal and regulatory purposes, the International Atomic Energy Agency (IAEA, 1994) defines radioactive waste as "waste that contains or is contaminated with radionuclides at concentrations or radioactivity levels greater than clearance levels as established by the regulatory body". The radioactive wastes are residues that have been produced by human nuclear activity and for which no future use is foreseen. Besides the nuclear power plants, the nuclear weapons testing, medical uses and various research studies involve a large number of radionuclides. In particular the nuclear accidents such as Three Mile Island Nuclear Power Station, where some gas and water were vented to the environment around the reactor, Chernobyl Nuclear Power Plant, the effects of the disaster were very widespread and Fukushima II Nuclear Power Plant have also released a large amount of radionuclides to environment.

In the case of radioactive wastes each country has its own classification, in general we can identify three types of wastes, that are, Low Level Waste (LLW), the LLW wastes contain primarily short lived radionuclides which refer to half-lives shorter than or equal to 30-year half-life, Intermediate Level Waste (ILW), radioactive non-fuel waste, containing sufficient quantities of long-lived radionuclides which refer to half-lives greater than 30 years. And a third one that is High Level Waste (HLW), arise from the reprocessing of spent fuel from nuclear power reactors to recover uranium and plutonium, containing fission products that are high radioactive, heat generating and long-lived. We would like to call attention to the fact that the waste classification LLW, ILW, HLW used here is only one of several alternative schemes; we adopted the simplest one.

Identification and characterization of radioactive wastes is a technical challenge because of their importance in choosing the appropriate permanent storage mode or further processing. Characterization definition of nuclear waste by IAEA (IAEA, 2003) is "the determination of the physical, chemical and radiological properties of the waste to establish the need for further adjustment, treatment, conditioning, or its suitability for further handling, processing, storage or disposal. Thus, it involves a collection of data that pertains to specific waste properties as well as processing parameters and quality assurance, some of

which include the following: thermal, mechanical, physical, biological, chemical and radioactivity properties (IAEA, 2007).

Testing and analyzes to demonstrate the radioactive content and the quality of final waste forms and waste packages are key components of this knowledge and control and are essential to accurate characterization of the waste. Physical characterization involves inspection of the waste to determine its physical state (solid, liquid or gaseous), size and weight, compactability, volatility and solubility, including closed waste packages which can be done using a variety of techniques, such as radiography (X-ray). Chemical waste characterization involves the determination of the chemical components and properties of the waste that is, potential chemical hazard, corrosion resistance, organic content, reactivity. This is most often done by chemical analysis of a waste sample. The radioactive inventory of various materials needs to be assessed for the classification of the nuclear waste. Radiological waste characterization involves detecting the presence of individual radionuclides and its properties such as half-life, intensity of penetrating radiation, activity and concentration and quantifying their inventories in the waste. This can be done by a variety of techniques, such as radiometric methods, mass spectrometric methods depending on the waste form, radionuclides involved and level of detail/accuracy required.

Furthermore, for developing a scaling factor (IAEA, 2009) to be applicable to the assessment of the radioactive inventory of the wastes with various matrices, it is indispensable to prepare a database compiled with a large numbers of information related to the radioactive inventory of long lived alpha and beta emitting nuclides which are difficult to measure (DTM) and gamma emitting nuclides which are easy to measure (ETM). It is necessary to develop analytical techniques for the DTM nuclides.

The aim of this work was to develop a sensitive analytical procedure for simultaneous determination of radionuclides difficult to measure. Between them is the 59Ni and 63Ni determination in low and intermediate level wastes from Brazilian Nuclear Power Plants — Eletrobras Termonuclear according to an analytical protocol developed based on sequential separation of different radionuclides presents in the waste matrices (Reis et al, 2011). Sources for 59Ni are austenitic steel in the reactor and activation of nickel dissolved in the coolant and in corrosion particles deposited on the core. The content of nickel in stainless steel is around to 10% and in Inconel in the range of 50-75%. Furthermore, nickel is found as an impurity in Zircaloy, ~ 40 ppm, and in reactor fuel, ~ 20 ppm (Lingren et al, 2007).