Scalable fabrication of free-standing and integrated electrodes with commercial level of areal capacity for aqueous zinc-ion batteries

Aqueous zinc-ion batteries (AZIBs) present a highly promising avenue for the deployment of grid-scale energy storage systems. However, the electrodes fabricated through conventional methodologies not only suffer from insufficient mass loadings, but also are susceptible to exfoliation under deformations. Herein, a scalable and cost-effective freezing-thawing method is developed to construct free-standing and integrated electrode, comprising H11Al2V6O23.2, carboxymethyl cellulose, and carbon nanotubes. Benefiting from the synergistic effect of these components, the resultant electrode exhibits superior flexibility and robustness, large tensile strength, exceptional electrical conductivity, and favorable electrolyte wettability. Under a large mass loading of 8 mg cm−2 (corresponding to a negative/positive electrode capacity ratio of 2.09), the electrode achieves remarkable capacity of 345.2 mAh/g (2.76 mAh cm−2) at 0.2 A/g and maintains 235.2 mAh/g (1.88 mAh cm−2) at 4 A/g, while sustaining an impressive capacity retention of 97.7 % over 5000 cycles. These considerably outperform conventional electrodes employing traditional binders. Even at an elevated mass loading of 14 mg cm−2 or when operated at a low temperature of − 30 °C, the electrode continues to deliver excellent electrochemical performance (e.g., extraordinary areal capacity of 4.32 mAh cm−2). In addition, the electrode owns outstanding tolerance to external forces. This research contributes to our understanding of the pivotal challenges within the realm of AZIB technology.