Metal Oxide Aerogels: A New Horizon for Stabilizing Anodes in Rechargeable Zinc Metal Batteries

Abstract Dendritic deposition and side reactions have been long‐standing interfacial challenges of Zn anode, which have prevented the development of practical aqueous zinc‐based batteries. Herein, an oxygen vacancy‐rich CeO₂ aerogel (VAG‐Ce) interface layer that simultaneously integrates Zn²⁺ selectivity, porosity, and is lightweight is reported as a new strategy to achieve dendrite‐free and corrosion‐free Zn anodes. The well‐defined and uniform nanochannels of VAG‐Ce can act as ion sieves that redistribute Zn²⁺ at the Zn anode surface by regulating Zn²⁺ flux, leading to uniform Zn deposition and significantly suppressing dendrite growth. Importantly, the abundant oxygen vacancies exposed on VAG‐Ce surface can strongly capture SO₄²⁻, forming a negatively charged layer that can attract Zn²⁺ and accelerate the Zn²⁺ migration kinetics, while the subsequent repulsion of additional anions can effectively suppress the generation of (Zn₄SO₄(OH)₆·xH₂O) byproducts, thereby realizing very stable Zn anodes. Consequently, VAG‐Ce modified Zn anode (VAG‐Ce@Zn) enables a long‐term lifespan over 4000 h at 4 mA cm⁻² and a record‐high cycle life of 1200 h is achieved under an ultrahigh 85% Zn utilization at 8 mA cm⁻², which enables excellent capacity retention and cycling performance of VAG@Zn/MnO₂ cells. This work contributes an innovative design concept by introducing oxygen vacancy‐rich aerogels and provides a new horizon for stabilizing Zn anode for large‐scale energy storage.