Design and Synthesis of the Next Generation of Crown Ethers for Waste Separations: An Interlaboratory Comprehensive Proposal. 1997 Annual Progress Report Page: 2 of 6
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Research Objective
The purpose of this task is to undertake the design, synthesis, and characterization of the next
generation of crown ethers for metal-ion separations applicable to the U.S. Department of
Energy's (DOE's) environmental needs. The general target problem is the removal of alkali and
alkaline-earth metal contaminants from certain environmental and waste streams. Although not a
radioactivity hazard, Li'ions leaching from burial sites containing more than 12 metric tons of
lithium compounds contaminate the groundwater at the Oak Ridge Y-12 Plant and have raised
noncompliance concerns because of the resultant toxicity to aquatic biota.
A more highly visible problem has been treatment of high-level wastes stored in underground
tanks at Oak Ridge National Laboratory (ORNL), Idaho National Engineering and Environmental
Laboratory, and especially the Hanford Site. The fission products "Sr and I"Cs have been
explicitly targeted for removal by the following DOE programs: the Office of Environmental
Management, the Office of Science and Technology, the Tank Waste Remediation System, the
Tanks Focus Area, and the Efficient Separations and Processing Cross-Cutting Program. These
seemingly ubiquitous fission products also appear in soil and groundwater at numerous DOE
sites. In addition, radium has recently been named as a target contaminant at the Niagara Falls
Storage Site.
Unfortunately, the separations technologies needed to address these problems either do not
exist or exhibit substantial deficiencies. Established techniques such as solvent extraction and ion
exchange certainly have a strong role to play, especially as enhanced with the use of the new
highly selective metal-ion hosts such as crown ethers and calixarenes. Recently applied results in
the United States, France, Russia, and elsewhere have demonstrated the effective performance of
crown ethers under realistic or actual process conditions for the removal of alkali and
alkaline-earth metal ions from waste, including high-levelnuclear waste.
From these results, one can readily appreciate how improvements in selectivity and extraction
strength can immediately translate to improvements and cost savings in existing technologies.
One can also envision extending crown-ether-based chemistry to solve other problems, such as
groundwater remediation. Achieving these ends will require the design and synthesis of new
crown compounds with "next-generation" capabilities, which will in turn require efforts to build
upon the current base of fundamental knowledge pertaining to host-guest chemistry, solvent
extraction, and ion exchange.
Research Statement
In view of the needs and aims outlined above, this task combines three interdependent
projects dealing with (1) molecular mechanics and ligand design, (2) solvent extraction of
univalent and divalent metal ions, and (3) polymer-immobilized crown ethers. The partner
laboratories at ORNL, Pacific Northwest National Laboratory, Argonne National Laboratory, and
the University of Tennessee, Knoxville (UTK), have world-recognized programs in the area of
crown ethers, solvent extraction, and ion exchange. Their cooperation under this task represents
an unusual and effective combination of unique resources.
The general approach entails the use of computational methods to predict properties and
strategies for testing the resulting predictions. State-of-the-art molecular-mechanics calculations
are being used as a tool in the design of new crown ethers for the selective extraction of alkali16
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Moyer, B. A.; Dietz, M. L.; Alexandratos, S. D. & Hay, B. P. Design and Synthesis of the Next Generation of Crown Ethers for Waste Separations: An Interlaboratory Comprehensive Proposal. 1997 Annual Progress Report, report, September 1, 1997; Tennessee. (https://digital.library.unt.edu/ark:/67531/metadc620658/m1/2/: accessed April 19, 2024), University of North Texas Libraries, UNT Digital Library, https://digital.library.unt.edu; crediting UNT Libraries Government Documents Department.