Dendritic Li deposition has been "a Gordian knot" for almost half a century,which significantly hinders the practical use of high-energy lithiummetal batteries (LMBs). The underlyingmechanisms of this dendrite formation are related to the preferential lithium deposition on the tips of the protuberances of the anode surface and also associated with the concentration gradient or even depletion of anions during cycling. Therefore, a synergistic regulation of cations and anions at the interface is vital to promoting dendrite-free Li anodes. An ingenious molecular structure is designed to realize the "cation-anion regulation" with strong interactions between adsorption sites and ions at the molecular level.A quaternized polyethylene terephthalate interlayerwith a "lithiophilic" ester building block and an "anionphilic" quaternary ammonium functional block can guide ions to form dendrite-free Limetal deposits at an ultrahigh current density of 10 mA cm-2, enabling stable LMBs.
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