This study achieved dendrite-free Zn metal anodes for Zn-ion batteries viaan in situgenerated gradient organic/inorganic hybrid solid–electrolyte interphase enabled by a eutectic electrolyte.
Turbulent interfacial evolution at the Zn anode/electrolyte, leading to rampant dendrites and parasitic reactions, is responsible for low Coulombic efficiency (CE) and premature failure in Zn metal batteries. To address this issue, an integrated eutectic electrolyte was introduced to construct a gradient organic/inorganic hybrid SEI (GHS) layer on the Zn anode through in situchemical reconstruction. The entanglement between the thermodynamic equilibrium of the species and the evolution of the GHS layer in a coordinated state was revealed. The GHS layer with a gradient structure and composition alleviates corrosion and passivation on the Zn anode, as well as the hydrogen evolution reaction. Additionally, the diffusion behavior of Zn 2+at the interface is optimized, allowing epitaxial deposition of Zn 2+along the (002) plane to eradicate dendrites. This results in an ultra-stable Zn anode with a substantially improved CE of 99.8% over 1200 cycles and a high cumulative plated capacity of 5.57 A h cm −2at 5 mA cm −2. The effectiveness of this approach is demonstrated by the extremely long lifespan of 22 000 cycles of a Zn//V 2O 5full cell.