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Chemistry, materials, & energy publications April 1, 2008

Inor 121-Adventures in actinide coordination chemistry with Raymond ligands

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DKShuh@lbl.gov1, Géza Szigethy2, Anne E. V. Gorden, gordeae@auburn.edu3, Jide Xu2, Tolek Tyliszczak1, Liam Bradshaw1, Patricia W. Durbin1, Polly Chang4, Eleanor A. Blakely, EABlakely@lbl.gov5, and Kenneth N. Raymond, raymond@socrates.berkeley.edu2. (1) Chemical Sciences Division, Lawrence Berkeley National Laboratory, MS 70A-1150, Berkeley, CA 94720, (2) Chemical Sciences Division and Department of Chemistry, Lawrence Berkeley National Laboratory and University of California, Berkeley, CA 94720, (3) Department of Chemistry and Biochemistry, Auburn University, Auburn, AL 36849, (4) Biosciences Division, SRI International, 333 Ravenswood Ave, Mail stop: PN175, Menlo Park, CA 94025, (5) Life Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720

The coordination chemistry of several specific Raymond ligands, a few among a wide range of multi-purpose siderophore-inspired ligands that have been developed, has been explored with cerium and plutonium. Recent investigations have determined the structures of [Pu(IV){5LIO(Me-3,2-HOPO)}2] which was the first structurally characterized Pu hydroxipyridonate; a mixed salt of 1-hydroxy-pyridin-2-one Pu(IV); and most recently, Pu(IV) maltol and bromomaltol complexes that provide intriguing comparisons to their Ce(IV) analogues. These Pu coordination chemistry investigations rely on and were the first to employ small-molecule single crystal x-ray diffraction using synchrotron radiation at the Advanced Light Source (ALS) to obtain information from crystals with dimensions less than 20 microns. The electronic structure of selected Pu and Ce complexes has also been probed using soft x-ray spectromicroscopy at the ALS Molecular Environmental Science Beamline. There is a renewed effort to develop Raymond ligands as therapeutic agents for actinide decorporation that will be discussed.

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