Microfluidic‐Assisted 3D Printing Zinc Powder Anode with 2D Conductive MOF/MXene Heterostructures for High‐Stable Zinc−Organic Battery

Zinc powder (Zn‐P) anodes have significant advantages in terms of universality and machinability compared with Zn foil anodes. However, their rough surface, which has a high surface area, intensifies the uncontrollable growth of Zn dendrites and parasitic side reactions. In this study, an anti‐corrosive Zn‐P‐based anode with a functional layer formed from a MXene and Cu‐THBQ (MXene/Cu‐THBQ) heterostructure is successfully fabricated via microfluidic‐assisted 3D printing. The unusual anti‐corrosive and strong adsorption of Zn ions using the MXene/Cu‐THBQ functional layer can effectively homogenize the Zn ion flux and inhibit the hydrogen evolution reaction (HER) during the repeated process of Zn plating/stripping, thus achieving stable Zn cycling. Consequently, a symmetric cell based on Zn‐P with the MXene/Cu‐THBQ anode exhibits a highly reversible cycling of 1800 h at 2 mA cm−2/1 mAh cm−2. Furthermore, a Zn‐organic full battery matched with a 4‐hydroxy‐2,2,6,6‐tetramethylpiperidine‐1‐oxyl organic cathode riveted on graphene delivers a high reversible capacity and maintains a long cycle life. An innovative microfluidic‐assisted 3D printing strategy is proposed to successfully realize 3D hierarchical porous Zn powder aerogel anode with 2D conductive MOF/MXene heterostructure. More importantly, a zinc‐organic full battery matched with 4‐hydroxy‐2,2,6,6‐tetramethylpiperidine‐1‐oxyl organic cathode riveted on graphene delivers a high reversible discharge capacity and maintains a long cycle life of 1200 cycles with a capacity retention of 96.8%.