Artificial organic-inorganic hybrid interface enables reversible Zn anodes

Commercial application of Zn metal anodes is severely hindered by uncontrollable dendrites and unfriendly side reactions. Herein, an artificial organic-inorganic hybrid interface (defined as H-PA) is designed and constructed through layer-by-layer stacking of Al2O3 and polyurea at molecule-atom level. Experiments and theoretical calculations show the H-PA fragment electronegativity and electron-donating sites corresponding to polar groups are beneficial for coordinating with Zn ions, thereby exhibiting favorable zincophilic properties and fast Zn ion transport/de-solvation kinetics. Simultaneously, the H-PA interface can reduce Zn atom diffusion barrier and limit hydrogen evolution reaction. As a consequence, the H-PA interface with mechanical stability can not only regulate uniform Zn ions flux, but also inhibit side reactions. The Zn@H-PA anode exhibits outstanding electrochemical reversibility with a long service life of 5800 h at 1.0 mA cm- 2 with 1.0 mAh cm- 2 and 5000 h at 2.0 mA cm- 2 with 2.0 mAh cm- 2. Meanwhile, the VO2//Zn@H-PA cell displays superior cycling stability and rate capability. Moreover, the pouch cell shows an excellent cycle performance with 90 % capacity retention after 100 cycles even at lean electrolyte (E/C ratio= 15 mu L mAh- 1), limited Zn supply (N/P ratio= 4.5). More importantly, this hybrid strategy at atomic-molecular level provides a reference idea for artificial protective layer design of batteries.