Hierarchical Pore Structure Composite Electrode by Electrospinning for Dendrite‐free Zinc‐Based Flow Battery

Abstract In the pursuit of sustainable energy solutions, zinc‐based flow batteries stand out for their potential in large‐scale energy storage, offering a blend of cost efficiency and safety. Although the porous electrode provides an increased specific surface area for reaction, the non‐uniform deposition of zinc, attributed to uneven concentration distribution within the porous electrode, has been a pivotal issue in accelerating the formation of zinc dendrites, which hinders the enhancement of energy density. A composite electrode with a strategic hierarchical pore structure has been developed with aligned nitrogen‐doped carbon fibers and traditional carbon felt. This structure takes advantage of the large pores of the carbon felt for efficient through‐flow paths, ensuring higher flow rates, while the dual‐scale pores within the electrospun film enhance mass transfer and increase the specific surface area. At 320 mA cm⁻², it achieved an ≈11.4% improvement in the battery's energy efficiency. Moreover, the nitrogen doping and the optimized reaction uniformity within the composite electrode have been instrumental in reducing the generation of zinc dendrites. The battery, integrated with the innovative composite electrode, maintained an energy efficiency of 59.2% at 320 mA cm⁻² after 300 cycles, which is a substantial improvement in operational longevity.