Multi-Channel Engineering of 3D Printed Zincophilic Anodes for Ultrahigh-Capacity and Dendrite-Free Quasi-Solid-State Zinc-Ion Microbatteries.

Abstract

Zinc-ion microbatteries (ZIMBs) are regarded as one of most promising miniaturized energy storage candidates owing to their high safety, compatible device size, superior energy density, and cost efficiency. Nevertheless, the zinc dendrite growth during charging/discharging and the inflexible device manufacturing approach seriously restrict practical applications of ZIMBs. Herein, we report a unique material extrusion 3D printing approach with reinforced zincophilic anodes for ultrahigh-capacity and dendrite-free quasi-solid-state ZIMBs. A 3D printed N-doped hollow carbon nanotube (3DP-NHC) multichannel host is rationally designed for desirable dendrite-free zinc anodes. Favorable structural metrics of 3DP-NHC hosts with abundant porous channels and high zincophilic active sites enhance the ion diffusion rate and facilitate uniform zinc deposition behavior. Rapid zinc-ion migration is predicted through molecular dynamics, and zinc dendrite growth is significantly suppressed with homogeneous zinc-ion deposition, as observed by in situ optical microscopy. 3D printed symmetric zinc cells exhibit an ultralow polarization potential, a glorious rate performance, and a stable charging/discharging process. Accordingly, 3D printed quasi-solid-state ZIMBs achieve an outstanding device capacity of 11.9 mA h cm-2 at 0.3 mA cm-2 and superior cycling stability. These results reveal a feasible approach to effectively restrain zinc dendrite growth and achieve high performance for state-of-the-art miniaturized energy storage devices.