A Generalized Method for High-Speed Fluorination of Metal Oxides by Spark Plasma Sintering Yields Ta₃ O₇ F and TaO₂ F with High Photocatalytic Activity for Oxygen Evolution from Water.

Abstract

A general method to carry out the fluorination of metal oxides with poly(tetrafluoroethylene) (PTFE, Teflon) waste by spark plasma sintering (SPS) on a minute scale with Teflon is reported. The potential of this new approach is highlighted by the following results. i) The tantalum oxyfluorides Ta₃ O₇ F and TaO₂ F are obtained from plastic scrap without using toxic or caustic chemicals for fluorination. ii) Short reaction times (minutes rather than days) reduce the process time the energy costs by almost three orders of magnitude. iii) The oxyfluorides Ta₃ O₇ F and TaO₂ F are produced in gram amounts of nanoparticles. Their synthesis can be upscaled to the kg range with industrial sintering equipment. iv) SPS processing changes the catalytic properties: while conventionally prepared Ta₃ O₇ F and TaO₂ F show little catalytic activity, SPS-prepared Ta₃ O₇ F and TaO₂ F exhibit high activity for photocatalytic oxygen evolution, reaching photoconversion efficiencies up to 24.7% and applied bias to photoconversion values of 0.86%. This study shows that the materials properties are dictated by the processing which poses new challenges to understand and predict the underlying factors.