Multifunctional MXene-Bonded Transport Network Embedded in Polymer Electrolyte Enables High-Rate and Stable Solid-State Zinc Metal Batteries

Sluggish transport kinetics and unstable electrode-electrolyte interface are the main obstacles that greatly impair the electrochemical performance of solid-state Zn metal batteries. Herein, the concept of multifunctional MXene bonded transport network-embedded poly(vinylidene fluoride co-hexafluoropropylene)/Zn(OTf)(2) solid polymer electrolyte (PH/MXene SPE) is proposed as all-in-one strategy for designing robust SPE. In order to uncover the mechanism of such rational designed SPE on regulating the ion transport, as well as the interphase chemistry and Zn deposition, comprehensive research including density functional theory calculation, simulation, and multiple characterization techniques are carried out. As the results indicate, the formation of hydrogen bond network between the MXene nanofiller and PH polymer benefits fast and homogeneous ion transport. Then, the in situ formation of stable organic/inorganic hybrid interphase is capable to ensure the efficient interfacial transport kinetics and uniform Zn deposition. When such PH/MXene SPE is applied, ultrastable Zn plating/stripping behavior with small polarization voltage can be realized. In addi, solid-state Zn/VO2 batteries with significantly improved rate performance and cyclic stability also can be demonstrated. The unique strategy proposed in this work offer a new insight into SPE design and the development of high-performance solid-state Zn metal batteries.

Automated summary

The concept of multifunctional MXene bonded transport network-embedded poly(vinylidene fluoride co-hexafluoropropylene)/Zn(OTf)(2) solid polymer electrolyte (PH/MXene SPE) is proposed as an all-in-one strategy for designing robust solid polymer electrolyte. Through comprehensive research including density functional theory calculation, simulation, and multiple characterization techniques, the mechanism of the rational designed solid polymer electrolyte on regulating ion transport, interphase chemistry, and zinc deposition is uncovered. The PH/MXene SPE enables ultrastable zinc plating/stripping behavior and demonstrates significantly improved rate performance and cyclic stability in solid-state Zn/VO2 batteries. The unique strategy proposed in this work offers a new insight into solid polymer electrolyte design and the development of high-performance solid-state Zn metal batteries.