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Title: APPLICATION OF FORMOHYDROXAMIC ACID IN NUCLEAR PROCESSING: SYNTHESIS AND COMPLEXATION WITH TECHNETIUM-99

Abstract

Acetohydroxamic acid (AHA) is an organic ligand planned for use in the Uranium Extraction (UREX) process. It reduces neptunium and plutonium, and the resultant hydrophilic complexes are separated from uranium by extraction with tributyl phosphate (TBP) in a hydrocarbon diluent. AHA undergoes hydrolysis to acetic acid which will impede the recycling of nitric acid. During recent discussions of the UREX process, it has been proposed to replace AHA by formohydroxamic acid (FHA). FHA will undergo hydrolysis to formic acid which is volatile, thus allowing the recycling of nitric acid. The reported reduction potentials of AHA and pertechnetate (TcO{sub 4}{sup -}) indicated that it may be possible for AHA to reduce technetium, altering its fate in the fuel cycle. At UNLV, it has been demonstrated that TcO{sub 4}{sup -} undergoes reductive nitrosylation by AHA under a variety of conditions. The resulting divalent technetium is complexed by AHA to form the pseudo-octahedral trans-aquonitrosyl (diacetohydroxamic)-technetium(II) complex ([Tc{sup II}(NO)(AHA){sub 2}H{sub 2}O]{sup +}). In this paper, we are reporting the synthesis of FHA and its complex formation with technetium along with the characterization of FHA crystals achieved by NMR and IR spectroscopy. Two experiments were conducted to investigate the complexation of FHA with Tc andmore » the results were compared with previous data on AHA. The first experiment involved the elution of Tc from a Reillex HP anion exchange resin, and the second one monitored the complexation of technetium with FHA by UV-visible spectrophotometry.« less

Authors:
; ; ; ;
Publication Date:
Research Org.:
Idaho National Lab. (INL), Idaho Falls, ID (United States)
Sponsoring Org.:
DOE - NE
OSTI Identifier:
1034439
Report Number(s):
INL/JOU-11-20847
TRN: US1200822
DOE Contract Number:  
DE-AC07-05ID14517
Resource Type:
Journal Article
Journal Name:
ASME Conference Proceedings
Additional Journal Information:
Journal Volume: 1
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; 21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS; ACETIC ACID; ANIONS; FORMIC ACID; FUEL CYCLE; HYDROCARBONS; HYDROLYSIS; NEPTUNIUM; NITRIC ACID; NUCLEAR ENGINEERING; PERTECHNETATES; PLUTONIUM; PROCESSING; RECYCLING; SPECTROPHOTOMETRY; SPECTROSCOPY; SYNTHESIS; TBP; TECHNETIUM; TECHNETIUM 99; URANIUM; extraction; formohydroxamic acid; recycling; technetium

Citation Formats

Wright, Amber, Mausolf, Edward, Campbell, Keri, Poineau, Frederic, and Paviet-Hartmann, P. APPLICATION OF FORMOHYDROXAMIC ACID IN NUCLEAR PROCESSING: SYNTHESIS AND COMPLEXATION WITH TECHNETIUM-99. United States: N. p., 2010. Web.
Wright, Amber, Mausolf, Edward, Campbell, Keri, Poineau, Frederic, & Paviet-Hartmann, P. APPLICATION OF FORMOHYDROXAMIC ACID IN NUCLEAR PROCESSING: SYNTHESIS AND COMPLEXATION WITH TECHNETIUM-99. United States.
Wright, Amber, Mausolf, Edward, Campbell, Keri, Poineau, Frederic, and Paviet-Hartmann, P. 2010. "APPLICATION OF FORMOHYDROXAMIC ACID IN NUCLEAR PROCESSING: SYNTHESIS AND COMPLEXATION WITH TECHNETIUM-99". United States.
@article{osti_1034439,
title = {APPLICATION OF FORMOHYDROXAMIC ACID IN NUCLEAR PROCESSING: SYNTHESIS AND COMPLEXATION WITH TECHNETIUM-99},
author = {Wright, Amber and Mausolf, Edward and Campbell, Keri and Poineau, Frederic and Paviet-Hartmann, P},
abstractNote = {Acetohydroxamic acid (AHA) is an organic ligand planned for use in the Uranium Extraction (UREX) process. It reduces neptunium and plutonium, and the resultant hydrophilic complexes are separated from uranium by extraction with tributyl phosphate (TBP) in a hydrocarbon diluent. AHA undergoes hydrolysis to acetic acid which will impede the recycling of nitric acid. During recent discussions of the UREX process, it has been proposed to replace AHA by formohydroxamic acid (FHA). FHA will undergo hydrolysis to formic acid which is volatile, thus allowing the recycling of nitric acid. The reported reduction potentials of AHA and pertechnetate (TcO{sub 4}{sup -}) indicated that it may be possible for AHA to reduce technetium, altering its fate in the fuel cycle. At UNLV, it has been demonstrated that TcO{sub 4}{sup -} undergoes reductive nitrosylation by AHA under a variety of conditions. The resulting divalent technetium is complexed by AHA to form the pseudo-octahedral trans-aquonitrosyl (diacetohydroxamic)-technetium(II) complex ([Tc{sup II}(NO)(AHA){sub 2}H{sub 2}O]{sup +}). In this paper, we are reporting the synthesis of FHA and its complex formation with technetium along with the characterization of FHA crystals achieved by NMR and IR spectroscopy. Two experiments were conducted to investigate the complexation of FHA with Tc and the results were compared with previous data on AHA. The first experiment involved the elution of Tc from a Reillex HP anion exchange resin, and the second one monitored the complexation of technetium with FHA by UV-visible spectrophotometry.},
doi = {},
url = {https://www.osti.gov/biblio/1034439}, journal = {ASME Conference Proceedings},
number = ,
volume = 1,
place = {United States},
year = {Sat May 01 00:00:00 EDT 2010},
month = {Sat May 01 00:00:00 EDT 2010}
}