Magic-angle-spinning nuclear magnetic resonance as a probe of nuclear materials

NUCL 117

Ian Farnan, ifarnan@esc.cam.ac.uk1, Herman Cho, hm.cho@pnl.gov2, William J. Weber, bill.weber@pnl.gov2, Joseph Somers, joseph.somers@ec.europa.eu3, Catherina Nastren3, and Lynn A. Boatner, boatnerla@ornl.gov4. (1) Department of Earth Sciences, University of Cambridge, CB2 3EQ Cambridge, United Kingdom, (2) Pacific Northwest National Laboratory, P.O. Box 999, Richland, WA 99352, (3) EC Joint Research Centre - Institute for Transuranic Elements, D-76125 Karlsruhe, Germany, (4) ORNL Center for Radiation Detection Materials and Systems, Oak Ridge National Laboratory, Materials Science and Technology Division, Oak Ridge, TN 37831
Nuclear magnetic resonance (NMR) spectroscopy is an attractive probe of local structure in solids because it is element specific and equally sensitive to crystalline and amorphous phases. A methodology for carrying out high-resolution magic-angle spinning (MAS) experiments on highly radioactive ceramics (>5 GBq) will be described. This will be illustrated by applications in the quantitative characterisation of radiation damage in zirconium ceramics. We have also investigated the vacancy distribution in yttria-stabilized zirconia and how it is affected by the substitution of lanthanide proxies for actinides. The detailed structural information obtainable is illustrated by studies on xenotime (YPO4) doped with a few percent cerium as a Pu proxy. The appearance of the 31P MASNMR spectrum is consistent with a random distribution of Ce3+ in the structure. There is also evidence of longer-range paramagnetic interactions that offer the possibility of constraining the local substitution to a high degree.