Manipulating the Host−Guest Chemistry of Cucurbituril to Propel Highly Reversible Zinc Metal Anodes

Rechargeable aqueous zinc-ion batteries are practically plagued by the short lifespan and low Coulombic efficiency (CE) of Zn anodes resulting from random dendrite deposition and parasitic reactions. Herein, the host−guest chemistry of cucurbituril additive with Zn²⁺ to achieve longstanding Zn anodes is manipulated. The macrocyclic molecule of cucurbit[5]uril (CB[5]) is delicately designed to reconstruct both the CB[5]-adsorbed electric-double layer (EDL) structure at the Zn interface and the hydrated sheath of Zn²⁺ ions. Especially benefiting from the desirable carbonyl rims and suitable hydrophobic cavities, the CB[5] has a strong host−guest interaction with Zn²⁺ ions, which exclusively permits rapid Zn²⁺ flux across the EDL interface but retards the H₂O radicals and SO₄²⁻. Accordingly, such a unique particle redistributor warrants long-lasting dendrite-free deposition by homogenizing Zn nucleation/growth and significantly improved CE by inhibiting side reactions. The Zn anode can deliver superior reversibility in CB[5]-containing electrolyte with a ninefold increase of cycle lifetime and an elevated CE of 99.7% under harsh test conditions (10 mA cm⁻²/10 mA h cm⁻²). The work opens a new avenue from the perspective of host−guest chemistry to propel the development of rechargeable Zn metal batteries and beyond.