The International Atomic Energy Agency (IAEA) has established international safeguards standards for fissionable material at spent fuel reprocessing plants to ensure that significant quantities of weapons-grade nuclear material are not diverted over a specified time frame. Currently, methods to verify that the facilities are operating under adequate safeguard-declared conditions require time consuming sampling and expensive, destructive analysis. The time delay between sampling and subsequent analysis provides a potential opportunity to divert the material out of the appropriate chemical stream. One way to avoid this problem is to use process monitoring equipment that is capable of on-line and in near-real time monitoring of the flowsheet radiochemical streams to rapidly identify deviations from normal operating conditions. Three integrated systems for flowsheet monitoring are currently being developed at PNNL including: 1) Multi-Isotope Process Monitor (MIP), 2) a spectroscopy-based monitor utilizing UV-Vis-NIR (Ultra Violet-Visible-Near Infrared) and Raman spectrometers, and 3) Electrochemically Modulated Separations (EMS). MIP uses gamma spectroscopy and pattern recognition software to identify off-normal conditions in process streams. The UV-Vis-NIR and Raman spectroscopic monitoring continuously measures chemical compositions of the process streams including actinide metal ions (U, Pu, Np), selected fission products, and major cold flowsheet chemicals. EMS provides an on-line means formore » pre-separating and preconcentrating elements of interest out of complex matrices prior to detection via non-destructive assay by gamma spectroscopy or destructive analysis with mass spectrometry. PNNL previously reported some of its initial modeling work as proof of principle. Here we will provide a general overview of the technologies and the ongoing demonstrations that utilize actual spent fuel.« less