Mass Transfer and Reaction Kinetic Enhanced Electrode for High‐Performance Aqueous Flow Batteries

Abstract A scalable and efficient process to modify electrodes with enhanced mass transfer and reaction kinetics is critical for redox flow batteries (RFBs). For the first time, this work introduces electrochemical exfoliation as a surface modification method of graphite felt (GF) to enhance the mass transfer and reaction kinetics in RFBs. Anion intercalation and subsequent gas evolutions at room temperature for one minute expand the graphite layers that increase the electrode surface area. Meanwhile, sufficient oxygen functional groups are introduced to the electrode, resulting in enhanced reaction kinetics and improved hydrophilicity. Further, spin‐polarized density functional theory is employed to reveal the role of oxygen functional groups in accelerating the vanadium redox reaction. Benefitting from sufficient oxygen groups, larger surface area, and superior wettability, the as‐prepared exfoliated GF (E‐GF) shows exceptional electrocatalytic activity with minimized overpotential, higher volumetric capacity, and improved energy efficiency. The redox flow battery assembled with the E‐GF electrode delivers voltage and energy efficiencies of 89.72% and 86.41% at the current density of 100 mA cm −2 , respectively. Remarkably, compared to the traditional GF treatment method, the elimination of the high temperature and long‐time treatment processes make this approach much more energy and time efficient, scalable, and affordable for large‐scale manufacturing.