Comparative Analysis of Thermal Activation on Felts and Continuous Carbon Filament Electrodes for Vanadium Redox Flow Batteries

Abstract

Thermal treatments are commonly used to improve electrode kinetics in vanadium redox flow batteries (VRFB). The impact of the widely adopted thermal treatment—400 °C for least 24 hours—was investigated on polyacrylonitrile (PAN)-based continuous carbon filaments (tows) and compared to PAN-based graphite felts. Surface properties were assessed with scanning electron microscopy (SEM), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS) and wettability measurements. The electrode activity was investigated via electrochemical impedance spectroscopy (EIS). Charge-transfer resistances and the constant phase element parameters related to the electric double layer were determined, revealing a correlation between enhanced electrode activity and increased double layer across all electrodes. An 8-hour 400 °C thermal treatment was sufficient to improve electrode activity for tows, whereas felts required longer durations, up to 24 hours, attributed to differences in the carbonization process employed for each material, with the tows undergoing continuous processing and the felts following a batch process. Three-electrode half-cell EIS measurements were conducted to elucidate positive and negative electrode contributions. Activated continuous carbon filament electrodes exhibited consistent electrode activities in both the catholyte (VO₂⁺/VO²⁺) and anolyte (V³⁺/V²⁺), whereas the electrochemical activity of felts was limited by the electrode deactivation in the anolyte.