Experimental hydrothermal alteration of crystalline and radiation-damaged pyrochlore

We have performed hydrothermal experiments with a crystalline microlite and a heavily self-irradiation-damaged (i.e., X-ray amorphous) betafite in a solution containing 1 mol/l HCl and 1 mol/l CaCl ₂ at 175 °C for 14 days. The well-crystalline microlite grains were partly (∼5-10 μm rim) replaced by a Ca and Na-poorer, defect pyrochlore phase with a larger unit-cell and a sharp chemical gradient at the interface (on a nm scale) to the unreacted core. The amorphous betafite grains (up to ∼2 mm in diameter), on the other hand, were completely transformed into an intergrowth of different crystalline phases (polycrystalline anatase and rutile, a yet unidentified Nb-Ta oxide, and a Y-REE phase), showing complex non-equilibrium structures. Our experimental observations bear a remarkable resemblance to those made on natural samples. They indicate that the processes of the fluid-pyrochlore interaction are influenced by self-irradiation structural damage and that thermodynamic equilibrium models can hardly be applied to adequately describe such systems.