Hydrophobic and zincophilic organic hierarchical nano-membranes with ordered molecular packing for stable zinc metal anodes

Abstract

Rechargeable aqueous Zn metal batteries hold significant potentials as one of the next-generation energy-storage devices due to their low cost and high safety. However, the uncontrollable dendrite growth and low efficiency in plating/stripping of Zn anodes hinder the commercial application of aqueous Zn-ion batteries (AZIBs). Herein, inspired by hydrophobic lotus, a multifunctional organic hierarchical nano-membrane serving as an artificial protective layer is constructed through the gas-liquid interface method, using self-assembled organic nanosheets (NOS). The organic nano-membrane exhibits ordered molecular packing, accompanied by uniform distribution of zincophilic carbonyl (CO) groups on the Zn metal surface. These groups function as active sites, homogenizing Zn2+ flux and accelerating Zn2+ deposition. Simultaneously, the hydrophobic membrane isolates active water, thereby restraining side reactions, effectively suppressing corrosion and extremely inhibiting dendrite growth. Consequently, NOS@Zn anode exhibits stable cycling over 2400 h and an average coulombic efficiency (CE) of 99.69 % (600 cycles) at 1 mA cm−2. Furthermore, NOS@Zn||CNT-MnO2 full cell presents remarkable capacity retention, approximately 5 times higher than that of Zn||CNT-MnO2 after 3000 cycles at 2 A g−1. This work develops an innovative organic interface modification material paving the way for dendrite-free Zn metal anodes and advancing the practical application of large-scale Zn-based energy storage systems.