Simultaneously Suppressing Shuttle Effect and Dendrite Growth in Lithium–Sulfur Batteries via Building Dual‐Functional Asymmetric‐Cellulose Gel Electrolyte

Abstract Polysulfides huttling and interfacial instability of Lithium‐anode are the main technical issues hindering commercialization of high‐energy‐density lithium−sulfur batteries. Simply addressing the problem of polysulfide shuttling or lithium dendrite growth can result in safety hazards or short lifespan. To synchronously tackle the aforementioned issues, the authors have designed an asymmetric cellulose gel electrolyte, a defective and ionized UiO66/black phosphorus heterostructure coating layer (Di‐UiO66/BP) and a cationic cellulose gelelectrolyte (QACA). Defective and ionized engineered UiO66 particles significantly enhances performance of UiO66/BP layer in anchoring free polysulfides, promoting smooth and effective polysulfide conversion and expediting the redox kinetics of sulfur cathode, therefore suppressing polysulfide shuttling. QACA electrolyte with numerous cationic groups can interact with anions via electrostatic adsorption, thus enhancing lithium‐ion transference number and contributing to formation of stable solid electrolyte interface to suppress lithium dendrite growth. Owing to the superior performance of QACA/Di‐UiO66/BP, the final cells exhibit outstanding electrochemical performance, presenting high sulfur utilization (1420.1 mAh g −1 at 0.1 C), high‐rate capacity (665.4 mAh g −1 at 4 C) and long cycle lifespan. This work proposes a strategy of designing asymmetric electrolytes to simultaneously address the challenges in both S‐cathode and Li‐anode, which contributes to advanced Li−S batteries and their practical application.