Flexible/Rechargeable Zn-Air Batteries Based on Multifunctional Heteronanomat Architecture

The increasing demand for advanced rechargeable batteries spurs development of new power sources beyond currently most widespread lithium-ion batteries. Here, we demonstrate a new class of flexible/rechargeable zinc (Zn)-air batteries based on multifunctional heteronanomat architecture as a scalable/versatile strategy to address this issue. In contrast to conventional electrodes that are mostly prepared by slurry-casting techniques, heteronanomat (denoted as "HM") framework-supported electrodes are fabricated through one-pot concurrent electrospraying (for electrode powders/single-walled carbon nanotubes (SWCNTs)) and electrospinning (for polyetherimide (PEI) nanofibers) process. Zn powders (in anodes) and rambutan-shaped cobalt oxide (Co₃O₄)/multiwalled carbon nanotube (MWCNT) composite powders (in cathodes) are used as electrode active materials for proof of concept. The Zn (or Co₃O₄/MWCNT) powders are densely packed and spatially bound by the all-fibrous HM frameworks that consist of PEI nanofibers (for structural stability)/SWCNTs (for electrical conduction) networks, leading to the formation of three-dimensional bicontinuous ion/electron transport channels in the electrodes. The HM electrodes are assembled with cross-linked polyvinyl alcohol/polyvinyl acrylic acid gel polymer electrolytes (acting as zincate ion crossover-suppressing, permselective separator membranes). Benefiting from its unique structure and chemical functionalities, the HM-structured Zn-air cell significantly improves mechanical flexibility and electrochemical rechargeability, which are difficult to achieve with conventional Zn-air battery technologies.