Behavior of Technetium in Alkaline Solution: Identification of Non-Pertechnetate Species in High-Level Nuclear Waste Tanks at the Hanford Reservation

摘要

Technetium is a long-lived (99Tc: 213,000 year half-life) fission product found in nuclear waste and is one of the important isotopes of environmental concern. The known chemistry of technetium suggests that it should be found as pertechnetate, TcO4-, in the extremely basic environment of the nuclear waste tanks at the Hanford site. However, other chemical forms of technetium are present in significant amounts in certain tanks, and these non-pertechnetate species complicate the treatment of the waste. The only spectroscopic characterization of these non-pertechnetate species is a series of X-ray absorption near edge structure (XANES) spectra of actual tank waste. To better understand the behavior of technetium under these conditions, we have investigated the reduction of pertechnetate in highly alkaline solution in the presence of compounds found in high-level waste. These results and the X-ray absorption fine structure (XAFS) spectra of these species are compared to the chemical behavior and XANES spectra of the actual non-pertechnetate species. The identity of the nonpertechnetate species is surprising.