MicroRaman Measurements for Nuclear Fuel Reprocessing Applications

Abstract

Treatment and reuse of used nuclear fuel is a key component in closing the nuclear fuel cycle. Solvent extraction reprocessing methods that have been developed contain various steps tailored to the separation of specific radionuclides, which are highly dependent upon solution properties. The instrumentation used to monitor these processes must be robust, require little or no maintenance, and be able to withstand harsh environments such as high radiation fields and aggressive chemical matrices.

Our group has been investigating the use of optical spectroscopy for the on-line monitoring of actinides, lanthanides, and acid strength within fuel reprocessing streams. This paper will focus on the development and application of a new MicroRaman probe for on-line real-time monitoring of the U(VI)/nitrate ion/nitric acid in solutions relevant to used nuclear fuel reprocessing. Previous research has successfully demonstrated the applicability on the macroscopic scale, using sample probes requiring larger solution volumes. In an effort to minimize waste and reduce dose to personnel, we have modified this technique to allow measurement at the microfluidic scale using a Raman microprobe. Under the current sampling environment, Raman samples typically require upwards of 10 mL and larger. Using the new sampling system, we can sample volumes at 10 μL or less, which is a scale reduction of over 1,000 fold in sample size.

This paper will summarize our current work in this area including: comparisons between the macroscopic and microscopic probes for detection limits, optimized channel focusing, and application in a flow cell with varying levels of HNO₃, and UO₂(NO₃)₂.