Current and emerging technologies for the remediation of difficult-to-measure radionuclides at nuclear sites.

Difficult-to-measure radionuclides (DTMRs), defined by an absence of high energy gamma emissions during decay, are problematic in groundwaters at nuclear sites. DTMRs are common contaminants at many nuclear facilities, with (often) long half-lives and high radiotoxicities within the human body. Effective remediation is, therefore, essential if nuclear site end-state targets are to be met. However, due to a lack of techniques for in situ DTMR detection, technologies designed to remediate these nuclides are underdeveloped and tend to be environmentally invasive. With a growing agenda for sustainable remediation and reduction in nuclear decommissioning costs, there is renewed international focus on the development of less invasive technologies for DTMR clean-up. Here, we review recent developments for remediation of selected problem DTMRs (129I, 99Tc, 90Sr and 3H), with a focus on industrial and site-scale applications. We find that pump and treat (P&T) is the most used technique despite efficacy issues for 129I and 3H. Permeable reactive barriers (PRBs) are a less invasive alternative but have only been demonstrated for removal of 99Tc and 90Sr at scale. Phytoremediation shows promise for site-scale removal of 3H but is unsuitable for 129I and 99Tc due to biotoxicity and bioavailability hazards, respectively. No single technique can remediate all DTMRs of focus. Likewise, there has been no successful site-applied technology with high removal efficiencies for iodine species typically present in groundwaters (iodide/I-, iodate/IO3- and organoiodine). Further work is needed to adapt and improve current techniques to field scales, as well as further research into targeted application of emerging technologies.