Additive Manufacturing of Grid Reservoir‐Integrated Anodes for Dendrite‐Free, Safe, and Ultra‐Low Voltage Zinc‐Ion Batteries

Abstract This work reports a novel 3D printed grid reservoir‐integrated mesoporous carbon coordinated silicon oxycarbide hybrid composite (3DP‐MPC‐SiOC) to establish the zincophile interphase for controlling the dendrite formation. The customized 3D printed grid patterned structure inhibits Zn dendrite growth and achieves long‐term stability with reduced voltage polarization due to homogeneous electric field distribution. The hybrid composite consisting of SiOC interpenetrated within carbon constructs a high zinc nucleation interphase, hence promoting uniform Zn 2+ deposition and enhancing ionic diffusion with dendrite‐free growth and a reduced nucleation energy barrier. As a result, the 3DP‐MPC‐SiOC@Zn symmetrical cell affords a highly reversible Zn plating/stripping and dendrite‐free structure over 198 h with an ultra‐low voltage polarization. These inspiring performances endow the 3DP anode with a 3DP‐VO cathode as a full battery, which shows a retention capacity of 78.8 mAh g −1 (Coulombic efficiency: 94.04%) at 0.1 A g −1 and a large energy density of 41 Wh kg −1 at a power density of 1.2 W kg −1 (based on the total mass of electrode) after 120 cycles. This newly developed 3D printing of hybrid composite as an electrode is straightforward and scalable and provides a novel concept for realizing dendrite‐free and stable rechargeable Zn‐ion batteries.