Anion‐tethered Single Lithium‐ion Conducting Polyelectrolytes through UV‐induced Free Radical Polymerization for Improved Morphological Stability of Lithium Metal Anodes

Abstract

Single Li+ ion conducting polyelectrolytes (SICs), which feature covalently tethered counter‐anions along their backbone, have the potential to mitigate dendrite formation by reducing concentration polarization and preventing salt depletion. However, due to their low ionic conductivity and complicated synthetic procedure, the successful validation of these claimed advantages in lithium metal (Li0) anode batteries remains limited. In this study, we fabricated a SIC electrolyte using a single‐step UV polymerization approach. The resulting electrolyte exhibited a high Li+ transference number (t+) of 0.85 and demonstrated good Li+ conductivity (6.3×10−5 S/cm at room temperature), which is comparable to that of a benchmark dual ion conductor (DIC, 9.1×10−5 S/cm). Benefitting from the high transference number of SIC, it displayed a three‐fold higher critical current density (2.4 mA/cm2) compared to DIC (0.8 mA/cm2) by successfully suppressing concentration polarization‐induced short‐circuiting. Additionally, the t+ significantly influenced the deposition behavior of Li0, with SIC yielding a uniform, compact, and mosaic‐like morphology, while the low t+ DIC resulted in a porous morphology with Li0 whiskers. Using the SIC electrolyte, Li0||LiFePO4 cells exhibited stable operation for 4500 cycles with 70.5 % capacity retention at 22 °C.

In‐Situ Polymerization Confined PEGDME‐Based Composite Quasi‐Solid‐State Electrolytes for Lithium Metal Batteries

“…This enhanced cationic transference number holds great potential in mitigating polarization effects and improving battery rate performance. [40,41] The LSV curves of PP SPE and PP-LTPO CSE are depicted in Figure 2d. Considering the difference of the responding delay and current intensity caused by the interface factor of the plate electrode, the responding current density is first normalized.…”

Toward Simultaneous Dense Zinc Deposition and Broken Side‐Reaction Loops in the Zn//V2O5 System

“…This interaction increases the transferable Zn 2 + number and decreases Zn 2 + concentration gradients at the interface, thus improving the electrochemical properties of hydrogel electrolytes. [22] In this context, by introducing BN nanosheets into a biomass-based hydrogel electrolyte, we have successfully constructed a rapid Zn 2 + -conducting hydrogel electrolyte (R-ZSO) with both high ionic conductivity and high Zn 2 + transference number. This innovative R-ZSO hydrogel electrolyte construction is anticipated to simultaneously address and resolve the crossinfluencing electrode problems in the Zn//V 2 O 5 battery system.…”