Soft glass interphase engineering for ultra-stable aluminum metal batteries†

Aluminum metal batteries (AMBs), as a next-generation green energy system, have garnered significant attention due to their inherent safety, low cost, and environmental benignity. However, non-uniform aluminum deposition and dendrite growth during cycling lead to rapid battery failure, resulting in resource waste and environmental pollution. To enhance resource utilization and achieve aluminum metal batteries with high efficiency and long cycle life, this study proposes an eco-friendly soft ZnP-H₂Im glass film fabricated via a melt-quenching process as a protective layer for the aluminum anode, which minimizes the use of hazardous substances and improves process sustainability. This material combines excellent mechanical flexibility, chemical stability, and ion transport regulation (via its sub-nanochannels), enabling homogeneous AlCl₄⁻ and Al₂Cl₇⁻ migration and promoting uniform aluminum nucleation and deposition. As a result, Al//Al symmetric cells based on soft ZnP-H₂Im-protected Al achieve record-breaking cycle lives of more than 10 000 hours at various areal capacities and current densities, far surpassing those of unmodified systems. In addition, after coupling the soft ZnP-H₂Im-protected Al with two organic cathodes, tetrachlorobenzoquinone (TCQ) and 2,3-dichloro-5,6-dicyano-1,4-benzoquinone (DDQ), the AMBs demonstrate high capacity, high reversibility, and high stability, with a capacity retention of 95% after 200 cycles and 80% after 220 cycles, respectively. This study not only advances interfacial engineering for AMBs but also provides a potential reference for extending this eco-friendly coordination polymer vitrification strategy to other metal anode systems, providing a transformative approach for developing high-performance secondary batteries with enhanced resource efficiency.