Rational design of epoxy functionalized ionic liquids electrolyte additive for hydrogen-free and dendrite-free...

Despite the high safety and low cost associated with aqueous Zn-ion batteries (ZIBs), uncontrolled Zn dendrite growth and parasitic reactions induced by water significantly diminish their stability. Herein, a new epoxy functionalized ionic liquid, 4-methyl-4-glycidylmorpholin bis[(trifluoromethyl)sulfonyl]imide (MGM[TFSI]), has been developed to mitigate water reactivity for stable ZIBs. It was found that the MGM⁺ cation disrupts the hydrogen bond network of water, hindering its adsorption on Zn anodes, thereby suppressing water decomposition and enhancing anode stability. Additionally, preferential adsorption of MGM⁺ cations on the Zn anode surface mitigates tip effects, suppresses dendrite growth, and promotes the formation of a ZnF₂ solid electrolyte interphase layer, effectively isolating the anode from the bulk electrolyte. As a result, benefiting from the well-designed MGM⁺-based electrolyte, Zn//Zn cells achieve significantly enhanced cycling stability, lasting over 2000 h at 1 mA cm^-2 with 1 mAh cm^-2. Furthermore, Zn//MnO₂ full cells deliver remarkable stability, retaining approximately 89 % of their initial capacity after 3000 cycles at 5 A/g. This work proposes that the MGM[TFSI] additive can effectively regulate the interfacial chemistry of the Zn anode, providing an opportunity to design advanced electrolytes for highly reversible ZIBs and beyond.