Longwei Yin

Composite solid electrolytes (CSEs) hold immense promise for high‐energy‐density solid‐state lithium metal batteries, yet their practical application remains severely hampered by filler agglomeration and sluggish interfacial Li ⁺ transport. Herein, dual‐functional supramolecular bridging networks are constructed by employing lithiated carboxymethyl cellulose (CMC‐Li) as dynamic bridges to interconnect polydopamine (PDA)‐modified Li _6.28 Al _0.24 La ₃ Zr ₂ O ₁₂ (LLZAO) fillers within a PVDF‐HFP matrix. This synergistic architecture helps promote a more uniform filler dispersion and actively mediates ion solvation dynamics via simultaneous anion trapping and cation extraction. Crucially, this dual‐regulation fundamentally mitigates the space‐charge layer (SCL) effect at organic‐inorganic boundaries, actively unlocking a highly efficient trans‐phase Li ⁺ percolation pathway through the LLZAO ceramic bulk, thereby bypassing conventionally sluggish interfacial routes. The resulting spatially homogeneous ion flux may reduce localized current hotspots and suppress lithium dendrite proliferation. Consequently, the optimized PVPL electrolyte empowers Li||Li symmetrical cells to maintain stable plating/stripping over 1400 h. Furthermore, LiFePO ₄ ||PVPL||Li full cells deliver 83% capacity retention after 400 cycles at 2 C, while NCM811||PVPL||Li cells maintain 88% capacity retention over 200 cycles. This dual‐functional bridging strategy establishes a generalizable and effective paradigm for engineering advanced CSEs with optimized structural and Li ⁺ transport kinetics.

Solid‐state lithium metal batteries (SLMBs) hold promise for next‐generation high‐energy‐density energy storage batteries, but encounter critical challenges of intrinsically sluggish Li ⁺ transfer kinetics and poor electrolyte/electrode interfacial stability. Herein, a Keggin‐type polyoxometalate (POM), lithium silicotungstate (Li ₄ SiW ₁₂ O ₄₀ , SiWLi), acting as a functional additive is introduced into the cationic poly(ionic liquid) (PIL) electrolyte to modulate the Li ⁺ coordination environment. The cationic groups of PIL and SiW ₁₂ O ₄₀ ⁴⁻ anions of SiWLi collectively promote the sufficient dissociation of LiTFSI through electrostatic interactions. Profiting from the anchoring effect of PIL toward TFSI ⁻ and the strong steric‐hindrance effect of large‐size SiW ₁₂ O ₄₀ ⁴⁻ , anions movement is effectively restrained to achieve a high Li ⁺ transference number of 0.82. Moreover, the introduction of SiW ₁₂ O ₄₀ ⁴⁻ helps to construct more contact ion pairs coordination, inducing an anions‐derived LiF‐rich SEI layer to facilitate the stable Li metal anode without dendrite formation. The designed composite solid‐state electrolyte supports the stable operation of Li||Li cells for over 3000 h at 0.3 mAh cm ⁻² . When paired with LiFePO ₄ (LFP) cathodes, the full cells deliver specific capacities of 145.03 mAh g ⁻¹ (99.5% retention after 600 cycles). This work provides an effective strategy for using steric‐hindrance POMs to regulate Li ⁺ solvation structure, boosting the design of high‐performance SLMBs.

All-solid-state lithium batteries (ASSLBs) feature reliable safety, high energy density, and stable cycling, stepping into the key development and application stage. However, a main challenge impeding their further commercialization arises from the complex mechano-(electro)chemical coupling effects at the cathode active material (CAM)/solid-state electrolyte (SSE) interface, which critically governs interfacial contact integrity, ion transport efficiency, and overall cell performance and lifespan. Innovatively, this review decouples and independently analyzes two core degradation pathways: mechanical failure induced by stress accumulation and structural evolution and (electro)chemical degradation driven by space charge layer (SCL) formation, elemental diffusion, and interfacial reactions. Corresponding stabilization strategies are critically evaluated, including strain-mitigating designs such as single-crystal cathodes, near-zero-strain materials, deformable electrolytes, and pressure-adaptive assembly, complemented by (electro)chemical passivation through coating and buffer layers. Ultimately, this work elaborates in detail on the integrated coupling mechanisms, surveys advanced characterization techniques, and proposes future research directions, offering theoretical and methodological guidance for ASSLB development.

Overcoming sluggish reaction kinetics is critical for advancing lithium-oxygen batteries (LOBs). In the MnO6 octahedra of manganese oxyhydroxide, the Jahn-Teller effect induces lattice distortion that provides highly promising active sites; however, uncontrolled lattice distortion leads to material instability, particularly under high current densities. Capitalizing on this characteristic, this work presents a highly efficient Mo-doped MnOOH catalyst with engineered oxygen vacancies. The catalyst was synthesized via a facile one-step hydrothermal method. Incorporating high-valence Mo cations into the MnOOH lattice enables precise regulation of the Mn³⁺-mediated Jahn-Teller distortion while simultaneously maintaining structural stability. Consequently, the resulting Mo-MnOOH catalyst significantly optimizes the adsorption energetics of oxygen-containing intermediates, thereby tailoring the growth morphology and deposition behavior of Li₂O₂. Electrochemical testing reveals that the Mo-MnOOH catalyst achieves an ultra-high charge/discharge capacity of 35,141/35,139 mAh g⁻¹ at 200 mA g⁻¹ and demonstrates stable cycling for over 1,600 cycles at a high current density of 1,000 mA g⁻¹. This work provides a novel perspective for harnessing the Jahn-Teller effect in manganese-based catalysts for practical energy storage applications.

Silicon, known for its high Li⁺ storage capacity, low redox potential, abundant reserves, and low cost, is regarded as a promising anode material for all-solid-state lithium-ion batteries (ASSLBs). Nevertheless, its practical application is hindered by severe volume expansion and sluggish reaction kinetics. Herein, Si@Mg₃N₂ composites are synthesized via a vacuum evaporation method, wherein ultrasmall Mg₃N₂ nanoparticles with an average size of 9 nm are uniformly coated onto the surface of commercial silicon microsheets. During the initial lithiation process, these Mg₃N₂ nanoparticles undergo an in situ phase transformation, forming a Li-Mg-Si alloy, Li-Mg alloy, and Li₃N irreversibly. The resulting Li-rich substances with the mixed ionic/electronic conductive function effectively mitigate the substantial volume expansion associated with the Li-Si alloying reaction (reducing it from 210% to 38.6%), thereby enhancing electrode kinetics and mechanical stability. As a result, the Si@Mg₃N₂ composite anode delivers a reversible capacity of 2619 mAh g^-1 at 0.1 A g^-1 and maintains a discharge capacity of 1460 mAh g^-1 even at a high rate of 5 A g^-1 in half-cell configurations. Furthermore, ASSLBs incorporating the Si@Mg₃N₂ anode exhibit excellent rate capability (50.8 mAh g^-1 at 40 C) and robust cycling stability (61.6% capacity retention after 1000 cycles).

Low-crystallinity Ga ₂ S ₃ /C nanowires possess more active sites and lower Na ⁺ diffusion barrier, thus delivering better sodium storage performance in specific capacity and rate capability than its high-crystallinity counterpart.

Roughness and fragility of bottom-up interfaces in perovskite solar cells accelerate device degradation and increase maintenance costs, while conventional interface engineering often fails to address issues at multiple interfaces simultaneously. Here, trimethyl(cyanomethyl)ammonium iodide is employed for a dual-interface self-regulation. Solution containing this molecule selectively desorbs non-covalently bonded self-assembled molecules, facilitating deprotonation of P-OH groups on self-assembled molecules. The resulting -PO^- headgroups undergo secondary homogeneous assembly, converting weakly adsorbed self-assembled molecules into stable bonded P-O-metal species and reducing potential barriers in the bottom depletion region. Simultaneously, trimethyl(cyanomethyl)ammonium iodide is extracted to the perovskite surface, spontaneously forming a one-dimensional n-type capping layer with a robust edge-sharing skeleton and enhancing quasi-Fermi level splitting at the interface. This coupled interfacial reinforcement leads to a high efficiency of 27.05% (certified 26.61%) and maintains over 95% of the initial efficiency after 2,100 hours of continuous operation at 65 °C.

Pseudocapacitive materials employ rapid, non-diffusion-limited faradaic processes to store charge, demonstrating significant potential for fast-charging batteries and supercapacitors. However, the high redox potentials of existing pseudocapacitive anodes substantially lower the overall cell voltage and energy density. Here, a cation-disordered rock-salt lithium titanium oxyfluoride (DRX-Li _x TiOF ₂ , 0 < x < 2) is reported to reversibly accommodate approximately 1.19 mol of Li ⁺ (~ 310 mAh g ⁻¹ ) and delivers high-rate performance (exceeding 64.4 C) via pseudocapacitive Li ⁺ storage within a low potential window extending down to 0.1 V vs. Li ⁺ /Li. This pseudocapacitive behavior is characterized by several structural and electrochemical features: the absence of phase transformation during Li ⁺ intercalation, quasi-rectangular cyclic voltammetry curves, sloping charge/discharge profiles and a surface-controlled current response. We further reveal that the pseudocapacitive characteristics originate from a three-dimensional percolation network that facilitates fast Li ⁺ migration with low energy barriers, enabled by a cation/anion-disordered structure arising from the mixed occupancy of Li/Ti cations and O/F anions. Owing to its low operating potential and high-rate capability, DRX-Li _x TiOF ₂ allows a lithium-ion capacitor to attain 4.0 V cell voltage and achieve energy and power densities several times higher than those obtained with conventional anodes, such as battery-type Li ₄ Ti ₅ O ₁₂ or pseudocapacitive materials like Nb ₂ O ₅ and TiO ₂ .