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The vanadium redox flow battery (VRFB) is a large‐scale energy storage technique and has been regarded as a promising candidate to integrate intermittent renewable energy with the grid. Its long‐term stability has so far been limited by the core component, an ion exchange membrane with low ion selectivity. Here a hybrid membrane with superhydrophilic TiO2 nanotubes dispersed in a Nafion matrix is reported. The VRFB single cell with the hybrid membrane exhibits an impressive performance with high coulombic efficiency (CE, ≈98.3%) and outstanding energy efficiency (EE, ≈84.4%) at 120 mA cm−2, which is higher than that of the commercial Nafion 212 membrane (CE, ≈94.5%; EE, ≈79.2%). More importantly, the cell maintains a discharge capacity of ≈55.7% after 1400 cycles (over 518 h), in obvious contrast to that of ≈20% after only 410 cycles for the one using commercial Nafion 212. This is attributed to the high ion selectivity of the hybrid membrane, because of, 1) the blocked and elongated ion diffusion pathway induced by the dispersed nanotubes and 2) binding and alignment of the sulfonic acid groups on nanotube surface. The high‐performance membranes may also find important applications in other fields, such as fuel cells, dialytic batteries, and water treatment.

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The redox flow battery (RFB) is an electrochemical device for large-scale energy storage. The most attractive merit of the RFB is the decoupling of energy storage and power generation. It is one of the most promising energy storage technologies for renewable energy, such as solar and wind, and grid energy storage due to its flexible design, high storage capacity, long cycle life, and safety. The development of the different RFB systems is holistically reviewed here, classified by the redox couples and supporting electrolytes. Particularly, based on the redox targeting concept, redox targeting-based flow batteries are extensively discussed as a novel flow battery technology for high-density energy storage. The working principles, key materials, and some typical redox targeting-based flow battery chemistries are highlighted.

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The purpose of this study was to improve the repulsion ability of sulfonated poly(ether ether ketone) (SPEEK) membrane for the vanadium ions crossover. For this purpose graphene oxide (GO) nanosheet and titanium dioxide (TiO2) nanoparticles were employed into the polymer matrix to prepare SPEEK/GO/TiO2 hybrid membrane via solution-casting method for vanadium redox flow battery (VRFB). The morphology, permeability of vanadium ions and device performance of asprepared membrane were investigated and discussed. It was observed that with the barrier block effect by the filler, the VRFB single cell with the optimized SPEEK/GO/TiO2 hybrid membrane exhibited high coulombic efficiency (~99%), excellent energy efficiency (~85%) and vigorous cyclability (~97.2% capacity retention after 100 cycles). Moreover, the VRFB cell with this blend membrane showed lower vanadium ions permeability than Nafion 212 or pure SPEEK membranes. These results demonstrated that the comprehensive properties of hybrid membrane have been remarkably improved comparing to pristine SPEEK which suggested that the hybrid membrane was applicable for VRFB energy storage system.