No abstract

Zinc-based redox flow batteries (ZRFBs) have been considered as ones of the most promising large-scale energy storage technologies owing to their low cost, high safety, and environmental friendliness. However, their commercial application is still hindered by a few key problems. First, the hydrogen evolution and zinc dendrite formation cause poor cycling life, of which needs to ameliorated or overcome by finding suitable anolytes. Second, the stability and energy density of catholytes are unsatisfactory due to oxidation, corrosion, and low electrolyte concentration. Meanwhile, highly catalytic electrode materials remain to be explored and the ion selectivity and cost efficiency of membrane materials demands further improvement. In this review, we summarize different types of ZRFBs according to their electrolyte environments including ZRFBs using neutral, acidic, and alkaline electrolytes, then highlight the advances of key materials including electrode and membrane materials for ZRFBs, and finally discuss the challenges and perspectives for the future development of high-performance ZRFBs.

Based on inexpensive, safe, and environmentally friendly active redox species, neutral polysulfide-ferrocyanide redox flow batteries (PFRFBs) have attracted much attention for large-scale energy storage. However, the development of PFRFBs is undermined by the expensive commercial membrane materials as well as the sluggish polysulfide redox reactions. This work attempts to solve these critical problems by combining the economical membrane with the highly catalytic electrode. In specific, K+-exchanged sulfonated polyether ether ketone (SPEEK-K) membranes have been investigated in PFRFBs to replace the costly Nafion membrane. SPEEK-K with optimized degree of sulfonation enables the PFRFB high average coulombic efficiency of 99.80% and superior energy efficiency of 90.42% at a current density of 20 mA cm-2. Meanwhile, to overcome the kinetic limitations of polysulfide redox reactions, a CuS-modified carbon felt electrode is demonstrated with excellent catalytic performance, enabling the PFRFB higher and more stable energy efficiency over cycling. The combination of the cost-effective membrane with the catalytic electrode in one cell leads to a capacity retention of 99.54% after 1180 cycles and an outstanding power density (up to 223 mW cm-2). The significant enhancements of electrochemical performance at reduced capital cost will make the PFRFB more promising for large-scale energy storage systems.