Generic Strategy to Synthesize High-Tap Density Anode and Cathode Structures with Stratified Graphene Pliable Pockets via Monomeric Polymerization and Evaporation, and Their Utilization to Enable Ultrahigh Performance in Hybrid Energy Storages.

Hybrid energy storage systems have shown great promise for many applications; however, achieving high energy and power densities with long cycle stability remains a major challenge. Here, a strategy to synthesize high-tap density anode and cathode structures that yield ultrahigh performance in hybrid energy storage is reported. First, vinyl acetate monomers are polymerized into molecular sizes via chain reactions controlled by the surface free radicals of graphene and metals. Subsequently, molecular-size polymers are thermally evaporated to construct battery-type anode structures with encapsulated tin metals for high-capacity and stratified graphene pliable pockets (GPPs) for fast charge transfer. Similarly, sulfur particles are attached to GPPs via monomeric polymerization, and capacitor-type hollow GPP (H@GPP) cathode structures are produced by evaporating sulfur, where sublimated S particles yield mesopores for rapid anion movement and micropores for high capacity. Moreover, hybrid full-cell devices with high-tap density anodes and cathodes show high gravimetric energy densities of up to 206.9 Wh kg-1 , exceeding those of capacitors by ≈16-fold, and excellent volumetric energy densities of up to 92.7 Wh L-1 . Additionally, they attain high power densities of up to 23 678 W kg-1 , outperforming conventional devices by a factor of ≈100, and long cycle stability over 10 000 cycles.

Inhibiting dissolution strategy achieving high-performance sodium titanium phosphate hybrid anode in seawater-based dual-ion battery.

Aqueous sodium-ion batteries (ASIBs) show great promise as candidates for large-scale energy storage. However, the potential of ASIB is impeded by the limited availability of suitable anode types and the occurrence of dissolution side reactions linked to hydrogen evolution. In this study, we addressed these challenges by developing a Bi-coating modified anode based on a sodium titanium phosphate (NTP)-carbon fibers (CFs) hybrid electrode (NTP-CFs/Bi). The Bi-coating effectively mitigates the localized enrichment of hydroxyl anion (OH-) near the NTP surface, thus addressing the dissolution issue. Notably, the Bi-coating not only restricts the local abundance of OH- to inhibit dissolution but also ensures a higher capacity compared with other NTP-based anodes. Consequently, the NTP-CFs/Bi anode demonstrates an impressive specific capacity of 216.8 mAh/g at 0.2 mV/s and maintains a 90.7 % capacity retention after 1000 cycles at 6.3 A/g. This achievement sets a new capacity record among NTP-based anodes for sodium storage. Furthermore, when paired with a cathode composed of hydroxy nickel oxide directly grown on Ni foam, we assembled a seawater-based cell exhibiting high energy and power densities, surpassing the most recently reported ASIBs. This groundbreaking work lays the foundation for a potential method to develop long-life NTP-based anodes.

Quasi-Solid-State Sodium-Ion Full Battery with High-Power/Energy Densities.

Developing a high-performance, low-cost, and safer rechargeable battery is a primary challenge in next-generation electrochemical energy storage. In this work, a quasi-solid-state (QSS) sodium-ion full battery (SIFB) is designed and fabricated. Hard carbon cloth derived from cotton cloth and Na3V2(PO4)2O2F (NVPOF) are employed as the anode and the cathode, respectively, and a sodium ion-conducting gel-polymer membrane is used as both the QSS electrolyte and separator, accomplishing the high energy and power densities in the QSS sodium-ion batteries. The energy density can reach 460 W h kg-1 according to the mass of the cathode materials. Moreover, the fabricated QSS SIFB also exhibits an excellent rate performance (e.g., about 78.1 mA h g-1 specific capacity at 10 C) and a superior cycle performance (e.g., ∼90% capacity retention after 500 cycles at 10 C). These results show that the developed QSS SIFB is a hopeful candidate for large-scale energy storage.