Dong-Won Kim

A high-MW EVA60 binder with strong adhesion enables a uniform Si–Gr anode during high-temperature drying, highlighting its scalability. All-solid-state Si–Gr/LiNi0.9Co0.05Mn0.05O2 pouch cells deliver stable cycling and robust interfacial integrity.

Lithium metal batteries have a high energy density but suffer from severe volume changes and non‐uniform Li deposition, which hinder their long‐term cycling stability. Herein, we present an innovative strategy employing an electrospun nitrile‐butadiene rubber (NBR)/polyacrylonitrile (PAN) membrane embedded with Li–SiO ₂ nanoparticles as an interlayer for the Li anode. The elastic NBR matrix accommodates the volume deformation induced by Li plating and stripping, while the nitrile groups in PAN guide uniform Li ⁺ ion flux through coordination interactions. Simultaneously, Li–SiO ₂ assists in regulating interfacial Li ⁺ distribution and mechanically reinforces the fibrous network. This synergistic combination improves mechanical resilience, interfacial stability, and Li ⁺ ion transport. As a result, pouch‐type anode‐free LMBs (AFLMBs) incorporating the interlayer and LiNi _0.88 Co _0.10 Al _0.02 O ₂ (active mass: 22.67 mg cm ⁻² ) cathode achieve a capacity retention of 76.9% after 250 cycles at 45°C and 1.0 C, outperforming cells without the interlayer. Moreover, the thickness increase of the pouch cell incorporating the LS‐NP interlayer was limited to 16.6%, nearly half that observed for the cell without the interlayer. Our findings demonstrate that the cooperative functionality of the polymer matrix and Li–SiO ₂ nanoparticles establishes a robust and stable interface, highlighting the promise of the bifunctional interlayer for high‐energy‐density AFLMBs.

Anode-free sulfide all-solid-state lithium batteries have emerged as a platform for achieving increased energy density. However, their practical operation is limited by heterogeneous interfacial reactions and uneven lithium deposition, which degrade reversibility and cycling stability. Among various approaches, silver−carbon (Ag−C) interlayers have attracted attention owing to their lithiophilicity and alloying behavior. Despite these advances, the role of carbon pore architecture in governing lithium deposition remains unclear. Here, we engineer mesoporous carbon hosts with tailored pore sizes to regulate the spatial distribution of Ag nanoparticles, thereby controlling Ag−C interfacial contact in anode-free sulfide ASSLBs. Systematic pore-size tuning promotes a more uniform distribution of Ag−C interfacial contact sites and enables homogeneous lithium deposition. Consequently, the pore-engineered host delivers enhanced cycling stability. This work establishes a clear structure−function relationship between carbon pore architecture and lithium deposition behavior, providing design guidelines for anode-free solid-state batteries.

The rapid transition toward electric vehicles and large-scale energy storage systems has intensified the demand for lithium-ion batteries (LIBs) capable of reliable operation under harsh temperature conditions. However, conventional liquid electrolytes suffer from severe degradation at elevated temperatures. Herein, we report a multifunctional gel polymer electrolyte (GPE) employing a siloxy-functionalized cross-linker, siloxy-pentaerythritol triacrylate (SiO-PETA), to enhance the high-temperature cycling stability and safety of LIBs. The trimethylsilane groups in SiO-PETA effectively scavenge corrosive HF, thereby mitigating cell degradation associated with transition metal dissolution. In addition, the chemically cross-linked polymer matrix encapsulates the liquid components in the GPE, suppressing parasitic side reactions and reducing electrolyte vaporization at elevated temperatures. A graphite/LiNi_0.6Co_0.2Mn_0.2O₂ pouch-type cell employing the GPE exhibits superior capacity retention at 70 °C, markedly outperforming a conventional liquid-electrolyte cell. Furthermore, the GPE provides enhanced safety, as evidenced by stable open-circuit voltage at 150 °C and reduced flammability. These results demonstrate that the SiO-PETA-based GPE effectively suppresses electrolyte and electrode degradation, enabling stable LIB operation at high temperatures.

The expanding electric vehicle market has driven an urgent demand for high‐energy‐density lithium‐ion batteries (LIBs). Solvent‐free dry‐processed electrodes offer strong potential for thick electrode development, but increasing thickness exacerbates the difficulty of uniformly dispersing conductive additives, posing a significant challenge for efficient electron and Li‐ion transport. Herein, we report mechanically pre‐unwound carbon nanotubes (uCNTs) as a morphologically engineered conductive additive with superior dispersibility, enabling continuous and homogeneous conductive networks in high‐loading Ni‐rich NCM811 cathodes. Ultra‐thick dry electrodes (10.5 mAh cm ⁻² , 170 μm) were realized using only 0.5 wt% uCNT—a threefold reduction compared with carbon black—yet delivered 120% higher capacity at 3.0 C and 92.7% capacity retention after 50 cycles. Furthermore, uCNT/natural graphite pouch full‐cells (5.0 mAh cm ⁻² , N/P ratio 1.1) demonstrated 89.5% capacity retention with an average Coulombic efficiency of 99.7% after 200 cycles at 0.2 C, validating the practical applicability of uCNT‐based dry electrodes. These results show that enhanced CNT dispersibility enables continuous conductive networks that alleviate the long‐standing ionic‐electronic transport imbalance in thick electrodes. This work provides a practically scalable, solvent‐free pre‐unwinding strategy that establishes a viable pathway for next‐generation high‐energy LIBs, coupling superior electrochemical performance with sustainable and industrially relevant manufacturing.