Coherent and Compact Zinc Electrodeposition Enabled by Compressing the Electric Double Layer of the Deposits

The porous hexagonal-platelet Zinc (Zn) deposits exacerbate the chemical corrosion and deteriorate the reversibility of the Zn electrodes in aqueous electrolytes. Based on the Derjaguin-Landau-Verwey-Overbeek (DLVO) theory, to turn the messy Zn deposits into agglomerate ones, the challenge is to weaken the electric double layer repulsive force, which is the main reason preventing the dense Zn deposits, between the electrodeposited Zn particles. Here, we proposed a strategy to compress the electric double layer and regulate the forces between the electrodeposited Zn particles by introducing inert charges to the surface of the Zn deposits. The results of the electron microscopies revealed dense and coherent electrodeposition of Zn, indicating that the van der Waals attraction between the deposits becomes governing during electrodeposition. Such results could be attributed to the adsorbed inert charges on Zn deposits decrease the net charges and weaken the electric double layer repulsive force. This design enables the Zn||Zn cells a long-term plating/stripping stability for > 1200 h, a high average Coulombic Efficiency of 99.9% for > 2100 h, and steady charge/discharge responses even under a draconian deep-discharge condition of 80% depth of discharge of Zn (DODZn). In addition, the Zn||VS2 full cells demonstrate significantly improved electrochemical reversibility and capacity retention.