Symmetry Donor–Acceptor Molecule Regulating Hydrogen-Bonding Network for Improved Metal Zinc Anode

The issues of zinc dendrites and side reactions caused by active water molecules have seriously affected the development of aqueous zinc batteries (AZBs). Herein, a symmetry hydrogen-bond donor–acceptor molecule additive named 1,3-bis(hydroxymethyl)urea (BHMU) can preferentially adsorb on the anode surface and lock up water molecules through hydrogen bonding, thus isolating water molecules and reducing side reactions caused by active water molecules. With these advantages, the mixed electrolyte containing BHMU additive impels a reversible Zn anode with a high Coulombic efficiency (99.7% over 1000 cycles at 1 mA cm^–2), while it also enables a stable symmetric cell operated at 1 mA cm^–2 (1 mAh cm^–2, 6.89% DOD_Zn) for 2250 h and 10 mA cm^–2 (10 mAh cm^–2, 68.9% DOD_Zn) for 350 h. More importantly, the Zn||PTO full battery also delivered superior cycling stability and higher capacity after 3000 consecutive 3000 cycles of circulation at 5 A g^–1. This study has great significance for the use of symmetry donor–acceptor molecules to modulate the solvation structure and the interface stability of the Zn anode in aqueous electrolytes.