Self-assembled supramolecular pillared arrays as bionic interface to stabilize zinc metal anodes

Aqueous zinc-ion batteries (AZIBs) are appealing devices for cost-effective and environmentally sustainable energy storage. However, irreversible issues such as dendrites, corrosion and hydrogen evolution reaction at the anode threaten to hamper their widespread deployment. Herein, we propose synergic self-assembly and arraying to form ordered bionic supramolecular pillar-like architectures (BSPAs) on the Zn anode through physical vapor deposition (PVD). With the combination of physicochemical and electrochemical characterizations, we demonstrate that the BSPAs exhibit a superhydrophobic feature with an ultrahigh contact angle up to 160.4°, and provide ordered zincophilic channels with a low activation energy of 34.91 kJ mol⁻¹ due to the presence of well-organized electronegative N entities in the assemblies. This allows desolvation of Zn²⁺ and promotes fast transportation and uniform deposition of Zn without dendrites. Consequently, the BSPAs@Zn-based symmetric cells achieve a long cycling stability of over 1000 h at 1 mA cm⁻² and 1 mAh cm⁻², and the BSPAs@Zn||MnO₂ full cells exhibit an improved rechargeability up to 600 cycles with 50.0 % capacity retention at a high current density of 5.0 A g⁻¹. This work paves the avenue of developing large-scale molecular self-assembly in reducing water adsorption and regulating the Zn deposition, potentially providing an efficient approach to stabilize the AZIB anode.