Multiple‐dimensioned defect engineering for graphite felt electrode of vanadium redox flow battery

Abstract The scarcity of wettability, insufficient active sites, and low surface area of graphite felt (GF) have long been suppressing the performance of vanadium redox flow batteries (VRFBs). Herein, an ultra‐homogeneous multiple‐dimensioned defect, including nano‐scale etching and atomic‐scale N, O co‐doping, was used to modify GF by the molten salt system. NH₄Cl and KClO₃ were added simultaneously to the system to obtain porous N/O co‐doped electrode (GF/ON), where KClO₃ was used to ultra‐homogeneously etch, and O‐functionalize electrode, and NH₄Cl was used as N dopant, respectively. GF/ON presents better electrochemical catalysis for VO²⁺/VO₂⁺ and V³⁺/V²⁺ reactions than only O‐functionalized electrodes (GF/O) and GF. The enhanced electrochemical properties are attributed to an increase in active sites, surface area, and wettability, as well as the synergistic effect of N and O, which is also supported by the density functional theory calculations. Further, the cell using GF/ON shows higher discharge capacity, energy efficiency, and stability for cycling performance than the pristine cell at 140 mA cm⁻² for 200 cycles. Moreover, the energy efficiency of the modified cell is increased by 9.7% from 55.2% for the pristine cell at 260 mA cm⁻². Such an ultra‐homogeneous etching with N and O co‐doping through “boiling” molten salt medium provides an effective and practical application potential way to prepare superior electrodes for VRFB.