Charge-Transfer Complex-Based Artificial Layers for Stable and Efficient Zn Metal Anodes

Herein, we report a charge-transfer complex electrolyte additive, 7,7,8,8-tetracyanoquinodimethane (TCNQ), with high Zn affinity, which was tightly adsorbed on the surface of a Zn anode to form a dense and robust interfacial complex layer and suppress the activity of H2O. As verified by comprehensive experimental and computational analyses, this complex layer could construct a Zn–Zn(TCNQ)2 Ohmic contact interface, guide rapid ion/electron transport, ameliorate electric field distribution, and inhibit the direct contact between the active H2O and Zn anode, demonstrating a dendrite-free Zn anode and facile Zn plating/stripping kinetics. Consequently, the Zn||Zn symmetrical cell exhibits a high Zn plating/stripping reversibility of over 1000 h at 20 mA cm–2 and 5 mA h cm–2 and a high depth of discharge (43%). Moreover, the Zn||MnO2 full cell delivers a high capacity of 143.3 mA h g–1 at 2000 mA g–1 even after 4000 cycles and a capacity retention of 94.7% after returning to 100 mA g–1.