Designing High-Performance Composite Electrodes for Vanadium Redox Flow Batteries: Experimental and Computational Investigation.

Highly catalytic electrodes play a vital role in exploiting the capability of vanadium redox flow batteries (VRFBs), but they suffer from a tedious synthesis process and ambiguous interaction mechanisms for catalytic sites. Herein, a facile urea pyrolysis process was applied to prepare graphitic carbon nitride-modified graphite felt (GF@CN), and by the virtue of a density functional theory-assisted calculation, the electron-rich pyridinic nitrogen atom of CN granules is demonstrated as the adsorption center for redox species and plays the key role in improving the performance of VRFBs, with 800 cycles and an energy efficiency of 75% at 150 mA cm-2. Such experimental and computational collaborative investigations guide a realizable and cost-effective solution for other high-power flow batteries.