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Title: Technetium Chemistry in HLW: Role of Organic Complexants

Technical Report ·
DOI:https://doi.org/10.2172/839063· OSTI ID:839063

Tc contamination is found within the DOE complex at those sites whose mission involved extraction of plutonium from irradiated uranium fuel or isotopic enrichment of uranium. At the Hanford Site, chemical separations and extraction processes generated large amounts of high level and transuranic wastes that are currently stored in underground tanks. Technetium is thought to have followed U in bismuth phosphate, REDOX and PUREX extraction campaigns and the Cs and Sr isotope recovery efforts. The waste from these extraction processes is currently stored in underground High Level Waste (HLW) tanks. However, the chemistry of the HLW in any given tank is greatly complicated by repeated efforts to reduce volume and recover isotopes. These processes ultimately resulted in mixing of waste streams from different processes. As a result, the chemistry and the fate of Tc in HLW tanks are not well understood. This lack of understanding has been made evident in the failed efforts to leach Tc from sludge and to remove Tc from supernatants prior to immobilization. Although recent interest in Tc chemistry has shifted from pretreatment chemistry to waste residuals, both needs are served by a fundamental understanding of Tc chemistry. The fate of Tc in the insoluble salts that constitute tank residuals is of paramount importance due to the long half-life and environmental mobility of Tc. Knowledge gaps include determination of the Tc oxidation state, the stability of reduced Tc solution species, and interactions with possible organic complexants in HLW. The objective of this renewal proposal is to continue to pursue fundamental understanding of Tc solution chemistry that provides the basis to make knowledgeable decisions and predictions of Tc behavior during retrieval operations and in tank residuals.

Research Organization:
Pacific Northwest National Lab., Richland, WA; Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
USDOE Office of Science (SC) (US)
OSTI ID:
839063
Report Number(s):
EMSP-81921-2004; R&D Project: EMSP 81921; TRN: US200509%%182
Resource Relation:
Other Information: PBD: 1 Jun 2004
Country of Publication:
United States
Language:
English