Regulating Interfacial Chemistry with Biobased Multifunctional Cellulose Levulinate Ester for Highly Reversible Zinc Ion Batteries

The unstable Zn interface, stemming from dendritic and parasitic side reactions, has posed significant challenges to the large-scale implementation of aqueous zinc ion batteries (ZIBs). Herein, a biobased multifunctional cellulose levulinate ester additive, featured by an acetyl propyl ketone moiety, was proposed to regulate the Zn anode/electrolyte interface chemistry. The well-designed cellulose levulinate ester exhibits strong adsorption capacity, fascinating in-situ protective layer, and exposed both hydrogen-bonding acceptor and donor due to the keto-enol tautomerism. The in-situ constructed organic-inorganic bilayer solid-electrolyte interphase enriched with ZnCO3-ZnF2-ZnS component effectively inhibits Zn dendrites, alleviates corrosion, and improves cycle stability. Consequently, the Zn(OTf)2/CLE electrolyte demonstrates highly reversible plating/stripping capability, enabling cycling for more than 2800 h in the shelving-recovery test, affirming their adaptability for long-term aqueous ZIBs. As a conceptual verification, the assembled Zn//MnO2 cells display exceptional cycle stability with a high capacity retention of 78.6% after 3000 cycles. The in-situ construction of a protective layer on the Zn anode using a biobased multifunctional cellulose levulinate ester additive offers an effective strategy for achieving high-performance Zn metal anodes in aqueous ZIBs.