Date of Award

3-21-2013

Document Type

Thesis

Degree Name

Master of Science

Department

Department of Engineering Physics

First Advisor

Timothy Zens, PhD.

Abstract

Hydrothermal synthesis of ThO2 and UxTh1-xO2, and UOx at temperatures between 670°C and 700°C has been demonstrated. Synthesis at these temperatures is 50-80°C below prior crystal growths and represents a new lower bound of successful growth. Hydrothermal synthesis represents a cost effective, environmentally friendly way of growing bulk actinide materials of optical quality. These refractory oxide single crystals offer potential applications in thorium nuclear fuel technology, wide-band-gap uranium-based direct-conversion solid state neutron detectors, and understanding how actinide fuels age with time. ThO2 single crystals of dimensions 6.49mm x 4.89mm x 3.89 mm and weighing 0.633g have been synthesized at growth rates near 0.125mm/wk. Single crystal UxTh1-xO2 crystals with mole fractions up to x approx. equal 0.30 have also been grown. The largest alloyed crystal with mole fraction x approx. equal 0.23 has dimensions of 2.97mm x 3.23mm x 3mm and saw growth rates likely near 0.2mm/wk. Mineralizer molarity, temperature gradient, and synthesis temperature were gradually optimized to produce a faceted, cubic crystal approximately 3mm a side. X-ray diffraction of single crystal ThO2 determined the unit cell to be of the calcium fluorite structure with a lattice parameter of 5.596(4) Angstrom. Lattice parameters for UxTh1-xO2 varied linearly with thorium concentration suggesting homogenous uranium incorporation into the lattice.

AFIT Designator

AFIT-ENP-13-M-06

DTIC Accession Number

ADA583232

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