Removal of radionuclides by ferrocyanide sorbents for the treatment of liquid radioactive wastes of nuclear power plants

A.Toropov., toropov@nnc.kz

 

Radioactive waste management, being an integral part of the nuclear fuel cycle, is one of the key areas in the development of nuclear energy in general. [1].

Currently, the reactor BN-350 in Aktau, Kazakhstan is being decommissioned. The nuclear power complex in Mangistau stores about 5,000 m3 of liquid radioactive waste (LRW). This LRW has a total volume activity of 107-108 Bq L-1. The status  of storage tanks is close to the emergency. However, the LRW with its high salt content can in the long term corrode the structural materials of these tanks, and this poses serious environmental risks in its vicinity.

In international practice, selecting the most appropriate method for managing LRW is determined by technical and non-technical factors. The most frequently used techniques include micro-ultrafiltration using ceramic filters, reverse osmosis and selective sorption on organic and inorganic materials.  Is known successful method employed in the LRW cooling pool at the Taiwan Research Reactor uses a cascade of ceramic filters with diatomite [2]..  However, this technology cannot be applied on highly mineralized LRW, which is the LRW in BN-350.

Also is not effective to apply the processing technologies which use of reverse osmosis membranes due to the limitations on the chemical composition and salinity of liquid wastes. For the processing of concentrated of LRW with a high content of nitrates and borates in the Loviisa NPP (Finland) and the Paks NPP (Hungary) use a deposition technology borates as crystalline precipitation and further purification of the cesium ions with sorbents based on cobalt ferrocyanide. Also as sorption materials used ferrocyanides other metals as well as their composite materials, such as copper and nickel ferrocyanides [3].

This article have been studied composite materials based on ferrocyanides of metals applied on natural sorbent - mineral matrix to make the benefits of the sorbent in the chemical and radiation resistance, which achieved by the combination of qualities each of them.

The purpose of research was the choice of the most suitable composite material based on metal's ferrocyanide and natural sorbent for the extraction of cesium from highly mineralized LRW.

For the study of sorption properties of the composites have been synthesized 15 composites ferrocyanides copper, nickel, cobalt were applied to five types of mineral sorbents of East Kazakhstan region.

Sorption of microquantities of cesium on composite ferrocyanide sorbents were carried out in static conditions by continuously stirring sample of air-dry sorbent with an aliquot of the liquid phase during 1 hour, then to stand for 2 hours to an additional capture of cesium ions sorbent particles. The ratio of the solid and liquid phases was 1:400. After standing the liquid and solid phases were separated by filtration through cellulose filter paper.

Contents of the main components of salinity and cesium were determined by atomic emission spectrometry (ICP-AES) on the instrument iCAP 6300 and mass spectrometry (ICP-MS) instrumentation by ELAN 9000. Activity radioactive tracers - cesium isotopes was determined by gamma- spectrometers with semiconductor detector CANBERRA. pH was monitored by potentiometric pH meter Mettler Toledo. Repeated experiments are three-time.

This article studied a series of sorbents for their ability to absorption of cesium - main dose radionuclide of LRW. Revealed that the most effective composite materials are ferrocyanides copper applied on mineral sorbent. The distribution coefficients of unmodified natural sorbents determined by the values Kd = 102, ferrocyanide composite sorbents copper and nickel Kd = 103-104. The optimum time of sorption purification - 1 hour. Among the factors affecting the extraction of cesium from solutions, the most significant effect is the concentration of organic matter.

The results of the research can be seen that at pH values above 10, as the adsorption capacity of composite sorbents and pure ferrocyanides directionally begins to decline, and for pure ferrocyanide reduction is more noticeable. With additional studies, the most effective composite sorbents can be tested on real LRW which the similar comrosition.

1.The Principles of Radioactive Waste Management. – Vienna: IAEA, Safety series, ¹ 111-F, STI/PUB/989, 1995

2.  Chung-Ping Huang, Tzung-Yi Lin, Ling-Huan Chiao, Hong-Bin Chen. Characterisation of radioactive contaminants and water treatment trials for the Taiwan Research Reactor’s spent fuel pool // Journal of Hazardous Materials – 233-234 (2012) P. 140-147

3. Milyutin V., Kononenko O., Mikheev S., GelisV. Sorption of cesium on finely dispersed composite ferrocyanide sorbents / / Radiochemistry. - 2010. - T.52. - ¹ 3. - P.238-240.