Abstract
Hydrogel electrolyte has emerged as an effective strategy for stabilizing zinc anode. Despite certain advancements in network design, solely relying on simple combinations of traditional polymer chains or single-function monomers is far from satisfactory in overcoming multiple challenges faced by zinc-ion battery. Herein, a novel multifunctional monomer, benzo-15-crown-5-acrylamide (BCAm), is designed and introduced into hydrogel network (PBCM-HE), aiming to regulate solvation sheath structure with supramolecular macrocyclic units. Specifically, rigid benzene rings in BCAm units can stabilize conformation of crown ether and bestow PBCM-HE excellent mechanical properties with tensile-strength of 105 kPa and compressive-strength of 0.6 MPa. Critically, the locally electron-rich ether bonds in supramolecular macrocycle can optimize solvation structure of hydrated zinc ions and promote ion transport, stabilizing interface interaction between electrolyte and Zn anode. Given this, PBCM-HE possesses outstanding ionic conductivity (61.7 mS cm(-1)) and remarkable transference number (0.86). Besides, the Zn||PBCM-HE||MnO(2) full cells show excellent discharge specific capacity of 290.9 mAh g(-1) at 0.1 C with Zn uniform deposition. This work innovatively develops a novel hydrogel electrolyte network with multifunctional monomer through one-step polymerization, providing new insights and possibilities for monomer design and selection in hydrogel electrolytes, further paving the way for exploring high-performance electrolytes in zinc-based devices.