Yuanfu Deng

This research proposes a nitrogen-doped carbon-coated transition metal selenide heterostructure (ZnSe-CoSe ₂ @NC) as an efficient catalyst to enhance bidirectional sulfur conversion in PVDF-based solid-state lithium-sulfur batteries.

Lithium–sulfur (Li–S) batteries are prominent candidates for next‐generation energy storage systems owing to their exceptional theoretical energy density (2600 Wh kg ⁻¹ ). Nevertheless, their practical application is hindered by the polysulfide shuttle effect, sluggish sulfur redox kinetics, and lithium dendrite growth. To mitigate these issues, an ultrathin (≈530 nm) tannic acid‐Ti ₃ C ₂ T _x (TA‐MXene) layer is designed. Density functional theory calculations demonstrate that both TA and MXene exhibit excellent anchoring capability for lithium polysulfides. Experiments reveal that TA‐MXene's sub‐nanometer interlayer channels simultaneously suppress polysulfide migration and accelerate lithium‐ion desolvation. The resultant anion‐rich solvation structure fosters an inorganic‐rich solid electrolyte interphase formation, mitigating lithium dendrite growth. Consequently, a Li–S cell with TA‐MXene‐modified separator achieves a high specific capacity of 603.1 mAh g ⁻¹ at 4.0 C and retain 90.3% capacity after 100 cycles at 0.2 C. Notably, under high sulfur loading (3.5 mg cm ⁻² ) and lean electrolyte (10 µL mg _S ⁻¹ ), the cells demonstrate exceptional cycling stability over 300 cycles at 0.2 C while delivering a remarkable mass/areal specific capacity of 1158.0 mAh g ⁻¹ /4.0 mAh cm ⁻² at 0.1 C. This work establishes a new design principle for separator modifications, demonstrating how ultrathin, lightweight architectures can integrate multifunctionality to overcome the intrinsic limitations of Li–S batteries.

Herein, we summarize the research on polymer-based solid-state lithium–sulfur batteries according to four areas—solid electrolytes, sulfur cathodes, lithium anodes, and interfacial interactions—as well as future development targets.

The rampant “top‐growth” dendrites, hydrogen evolution reaction (HER), and zinc (Zn) self‐corrosion severely impede the further development of rechargeable aqueous zinc ion batteries. To address these challenges, a novel double‐layer gradient coating consisting of a zincophilic Sn inner layer and an organic polymer outer layer (OSA/PAM@Sn) is constructed on the surface of the Zn anode. The organic outer layer, composed of cross‐linked oxidized sodium alginate and polyacrylamide (OSA/PAM), not only serves as a physical barrier to isolate active water but also accelerates Zn ²⁺ diffusion by facilitating the desolvation process of [Zn(H ₂ O) ₆ ] ²⁺ due to its plentiful polar functional groups, thereby effectively suppressing the detrimental HER and Zn self‐corrosion. Simultaneously, the loose Sn inner layer can offer abundant nucleation sites to induce uniform “bottom‐to‐top” Zn deposition with low overpotential. Benefiting from the synergistic effect of the designed double‐layer gradient coating, the OSA/PAM@Sn‐Zn anode exhibits remarkable reversibility, with lifespans of over 5000 and 1200 h at 1 mA cm ⁻² –1 mAh cm ⁻² and 5 mA cm ⁻² –5 mAh cm ⁻² in symmetric cells, respectively. Additionally, the MnO ₂ ||OSA/PAM@Sn‐Zn full battery also displays an improved rate performance and cycle stability. This work emphasizes the importance of synergistic effects in interface design to achieve side reaction‐free and dendrite‐free Zn anodes.

Correction for ‘H₂O assisted in improving the electrochemical performance of a deep eutectic electrolyte formed by choline chloride and magnesium chloride hexahydrate’ by Kaixiang Zou et al., J. Mater. Chem. A, 2024, 12, 33257–33267, https://doi.org/10.1039/D4TA05504G.

H ₂ O introduction reduced the interaction between ions and hydrogen bonds, enhancing the ion transport and diffusion in the electrolyte.