Aqueous zinc ion batteries have been considered as the prominent candidate in the next-generation batteries for its low cost, safety and high theoretical capacity. Nonetheless, formation of zinc dendrites and side reactions at the electrode/electrolyte interface during the zinc plating/stripping process affect the cycling reversibility of the zinc anode. Regulation of the zinc plating/ stripping process and realizing a highly reversible zinc anode is a great challenge. Herein, we applied a simple and effective approach of controlled-current zinc pre-deposition at copper mesh. At the current density of 40 mA cm⁻², where the electron/ion transfers are both continuous and balanced, the Zn@CM-40 electrode with the (002) crystal plane orientation and the compactly aligned platelet morphology was successfully obtained. Compared with the zinc foil, the Zn@CM-40 exhibits greatly enhanced reversibility in the repeated plating/stripping (850 h at 1 mA cm⁻²) for the symmetric battery test. A series of characterization techniques including electrochemical analyses, XRD, SEM and optical microscopy observation, were used to demonstrate the correlation between the structure of pre-deposited zinc layer and the cycling stability. The COSMOL Multiphysics modeling demonstrates a more uniform electric field distribution in the Zn@CM than the zinc foil due to the aligned platelet morphology. Furthermore, the significant improvement is also achieved in a Zn||MnO₂ full battery with a high capacity-retention (87% vs 47.8%). This study demonstrates that controlled-current electrodeposition represents an important strategy to regulate the crystal plane orientation and the morphology of the pre-deposited zinc layer, hence leading to the highly reversible and dendrite-free zinc anode for high-performance zinc ion batteries.

Transition-metal oxides (TMOs) have gradually attracted attention from researchers as anode materials for lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs) because of their high theoretical capacity. However, their poor cycling stability and inferior rate capability resulting from the large volume variation during the lithiation/sodiation process and their low intrinsic electronic conductivity limit their applications. To solve the problems of TMOs, carbon-based metal-oxide composites with complex structures derived from metal-organic frameworks (MOFs) have emerged as promising electrode materials for LIBs and SIBs. In this study, we adopted a facile interface-modulated method to synthesize yolk-shell carbon-based Co₃O₄ dodecahedrons derived from ZIF-67 zeolitic imidazolate frameworks. This strategy is based on the interface separation between the ZIF-67 core and the carbon-based shell during the pyrolysis process. The unique yolk-shell structure effectively accommodates the volume expansion during lithiation or sodiation, and the carbon matrix improves the electrical conductivity of the electrode. As an anode for LIBs, the yolk-shell Co₃O₄/C dodecahedrons exhibit a high specific capacity and excellent cycling stability (1, 100 mAh·g^-1 after 120 cycles at 200 mA·g^-1). As an anode for SIBs, the composites exhibit an outstanding rate capability (307 mAh·g^-1 at 1, 000 mA·g^-1 and 269 mAh·g^-1 at 2, 000 mA·g^-1). Detailed electrochemical kinetic analysis indicates that the energy storage for Li⁺ and Na⁺ in yolk-shell Co₃O₄/C dodecahedrons shows a dominant capacitive behavior. This work introduces an effective approach for fabricating carbon- based metal-oxide composites by using MOFs as ideal precursors and as electrode materials to enhance the electrochemical performance of LIBs and SIBs.