A-site compositional effects in Ga-doped hollandite materials of the form BaxCsyGa2x+yTi8-2x-yO16: implications for Cs immobilization in crystalline ceramic waste forms.
The hollandite structure is a promising crystalline host for Cs immobilization. A series of Ga-doped hollandite BaxCsyGa2x+yTi8-2x-yO16 (x = 0, 0.667, 1.04, 1.33; y = 1.33, 0.667, 0.24, 0) was synthesized through a solid oxide reaction method resulting in a tetragonal hollandite structure (space group I4/m). The lattice parameter associated with the tunnel dimension was found to increases as Cs substitution in the tunnel increased. A direct investigation of cation mobility in tunnels using electrochemical impedance spectroscopy was conducted to evaluate the ability of the hollandite structure to immobilize cations over a wide compositional range. Hollandite with the largest tunnel size and highest aspect ratio grain morphology resulting in rod-like microstructural features exhibited the highest ionic conductivity. The results indicate that grain size and optimized Cs stoichiometry control cation motion and by extension, the propensity for Cs release from hollandite.
Department of Materials Science and Engineering, Clemson, SC, USA.
Yun
Y
Xu
Department of Environmental Engineering and Earth Science, Clemson, SC, USA.
Yi
Y
Wen
Department of Materials Science and Engineering, Clemson, SC, USA.
Rob
R
Grote
Savannah River National Laboratory, Aiken, SC, USA.
Jake
J
Amoroso
Department of Environmental Engineering and Earth Science, Clemson, SC, USA.
Lindsay
L
Shuller Nickles
Department of Materials Science and Engineering, Clemson, SC, USA.
Kyle S
KS
Brinkman