Large-scale synthesis of centrifugally spun tantalum oxynitride fiber electrocatalysts for hydrogen evolution reaction

Tantalum oxynitride (TaO_xN_1−x) fibers were synthesized and evaluated for their electrocatalytic hydrogen activity using an in-house developed centrifugal spinning setup. By tailoring the composition of the spinning solution and optimizing collector distance and rotation speed of the spinneret, bead-free TaO_xN_1−x fibers with a diameter of 800 nm were obtained. The fibers were structurally characterized through phase and elemental analysis, confirming the formation of monoclinic TaO_xN_1−x with clear splitting of the X-ray photoelectron spectroscopy peaks indicating Ta was in +5 oxidation state. The resulting oxynitride fibers exhibited superior electrocatalytic performance with low overpotentials (250 mV) to generate 10 mA/cm² compared to Ta₂O₅ oxide fibers. Interestingly, the enhanced activity of oxynitride fibers was observed to be suppressed in basic medium due to the high oxophilicity of tantalum ions and a negative Gibbs adsorption-free energy, leading to poisoning of the active sites. This work demonstrates a facile pathway for the fabrication of high-performance electrocatalysts, based on TaO_xN_1−x fibers, from a cost-effective and energy-efficient centrifugal spinning technique.