Partial Sulfidation of the Electrochemically Exfoliated Layered Double Hydroxides toward Advanced Aqueous Zinc Batteries

Abstract Aqueous zinc‐based batteries are a promising alternative to lithium batteries. These batteries, however, persistently suffer from uncontrollable dendrite growth and sustained water consumption at the Zn anodes, along with low and often fading capacity at the cathodes. Herein, Zn metal is simply encapsulated into a chitosan‐containing polymer gel that not only suppresses hydrogen evolution but also enables dendrite‐free Zn plating/stripping. A binder‐free cathode based on the electrochemically exfoliated and partially sulfidated Ni–Co–Fe layered double hydroxide‐reduced graphene oxide (SNS‐rGO) nanocomposite is also reported. The fabricated devices (based on either Zn or chitosan‐coated Zn) deliver near record‐high values of specific capacity (756 mA h g⁻¹_cathode at 1 A g⁻¹) and specific energy (1284 W h kg⁻¹_cathode), along with an outstanding specific power (108 kW kg⁻¹_cathode), an excellent output voltage (up to 1.9 V), and prolonged cycling stability at 100% depth‐of‐discharge. This interface engineering strategy, supported by the density functional theory calculations, provides a solid basis for further practical applications of aqueous Zn batteries.