Hydrogen bond-anchored interfacial engineering for stable and high-performance aqueous zinc-ion batteries

Rechargeable aqueous Zn-ion batteries (AZIBs) are regarded as a sustainable energy storage for stationary energy storage applications, but they suffer from serious side reactions and uncontrolled Zn dendrite growth. Herein, a hydrogen bond-anchored phytic acid-zinc (PA-Zn)/hydrogel protective layer is established on Zn anodes, with the PA-Zn interlayer mediating the robust interfacial adhesion between the hydrogel and Zn substrate. The sulfonate-functionalized hydrogel framework (– SO 3 − ) accelerates Zn 2+ desolvation kinetics, homogenizes the ionic flux, and regulates the electric field distribution. The in situ -formed PA-Zn layer enhances Zn 2+ mobility through phosphate/carboxylate chelation while suppressing water-induced side reactions by creating a dehydrated interface. Serving as a stabilizing mediator, this interlayer also reinforces the hydrogel–electrode interface through hydrogen bonding, significantly enhancing the stability of Zn anodes. As a result, the PA-Hn@Zn anode exhibits a high average coulombic efficiency (CE) of 99.42% and excellent cycling stability of 2400 h. Moreover, PA-Hn@Zn||KVOH full cells retain a capacity of 1 62 mAh g −1 over 3000 cycles at 5 A g −1 . This hydrogen bond-anchored interfacial engineering strategy offers a promising pathway for developing advanced Zn anodes and promotes the commercialization of AZIBs. • The hydrogen-bond anchoring strategy constructs a stable hybrid hydrogel protective layer on Zn anodes, addressing the issues of poor interface adhesion and protective layer failure. • The sulfonate-functionalized hydrogel framework and in situ formed PA-Zn interlayer synergistically accelerate Zn 2+ desolvation kinetics and suppress water-induced side reactions. • The integrated design of the hybrid hydrogel layer enables ultralong cycling stability and high reversibility of Zn anodes, promoting the practical application of aqueous Zn-ion batteries.