All-solid-state lithium metal batteries are widely considered promising next-generation energy storage systems owing to high specific energy and enhanced safety. However, their practical deployment is hindered by high stack pressure and inferior electrochemical performance. Here, we exploit the fast thermodynamic diffusion of fluorine atoms to design a core-shell structured sulfide electrolyte, Li5.4PS4.4Cl1.4F0.2-0.2LiF, featuring 50 nm LiF nanoshell and F-enriched bulk. During electrochemical operation, fluorine atoms diffuse into the LiNi0.83Co0.12Mn0.05O2 positive electrode lattice, enhancing structural robustness and mitigating mechanochemical failure, while the LiF nanoshell stabilizes both the Li metal negative electrode and positive electrode interfaces through spontaneous fluorination diffusion. As a result, full cells demonstrate good electrochemical performance, including long cycle life, high-voltage stability, and robust operation across a wide temperature window. Furthermore, all-solid-state pouch cells operated under a low stack pressure of 2.5 MPa exhibit stable cycling over 350 cycles (1 C) with 85% capacity retention, and achieve a high specific energy of over 400 Wh/kg (based on solid electrolyte, Li metal, and positive electrode materials). This bulk-to-interface fluorination strategy effectively mitigates mechanochemical failures, offering an alternative pathway toward low-pressure, long-life, and high-energy all-solid-state batteries.

Lithium ion battery and new battery technologies have developed rapidly in recent years, while they still encounter substantial challenges, particularly concerning ion transport in the electrolyte and the stability of electrolyte/electrode interfaces. Recently, the lattice matching theory has been utilized in energy storage to efficiently enhance the ion transport kinetics and facilitate uniform interphase growth, which is conducive to battery cycle stability and has garnered increasing attention. In this review, the recent research on lattice matching theory in energy storage is summarized and discussed. We first review the historical development of lattice matching theory and then systematically summarize the application of lattice matching theory in different battery systems in terms of electrolyte, cathode and anode. Lattice-matched interphases tend to exhibit superior kinetics and greater structural stability, thereby enhancing the cycling stability of batteries. At last, we propose the design criteria of various lattice-matched interfaces for advanced batteries. We anticipate that this review will enhance the understanding of the lattice matching theory and serve as a reference for future design of advanced batteries.

Polymer electrolytes (PEs) are widely regarded as a promising platform for solid-state batteries (SSBs), offering the potential to simultaneously achieve high energy density with improved safety. However, in current literature, PEs spanning liquid-percolated gels, liquid-assisted quasi-solids, and truly polymer-governed solids are often indiscriminately grouped as solid polymer electrolytes (SPEs), obscuring their distinct ion transport mechanisms, interfacial behaviors, and practical performance constraints, and leading to misleading performance comparisons and unrealistic expectations regarding solid-state operation. Herein, we establish a mechanistic framework that categorizes PEs into gel polymer electrolytes (GPEs), quasi-solid polymer electrolytes (QSPEs), and all-solid polymer electrolytes (ASPEs) based on their dominant ion-solvation environment and transport pathways. By systematically analyzing the ion-transport mechanisms, interfacial behaviors, and performance-limiting features associated with each PE class, we clarify their defining characteristics and mechanism-imposed limitations. Accordingly, we outline category-specific research priorities and highlight the necessity of mechanism-driven materials design, transparent definitions and reporting, and application-relevant benchmarking. This unified Perspective lays a foundation for consistent interpretation, meaningful comparison across PE systems, and more rational materials design toward the advancement of PE-enabled SSBs.

The relatively low room-temperature ionic conductivity and terrible lithium dendrite growth of polycarbonate-based solid polymer electrolytes (SPEs) seriously restrict their further development for solid-state lithium metal batteries (SSLMBs). Herein, a polycarbonate-based SPE is innovatively designed through facile in situ polymerization of ferroelectric poly(vinylidene fluoride-trifluoroethylene-chlorotrifluoroethylene) (PVTC) and vinyl ethylene carbonate (VEC) monomer (PVTC-g-PVEC). This in situ polymerized PVTC-g-PVEC SPE with polar & horbar;CF2 group and C & boxH;O/C & horbar;O groups greatly promotes the dissociation of Li salts and enhances the transport of Li+. Moreover, the ferroelectric PVTC-g-PVEC SPE can produce spontaneous polarization under external electric fields, which promotes uniform deposition of Li+ and suppresses lithium dendrite growth. In addition, the fabricated PVTC-g-PVEC SPE facilitates the formation of a stable solid electrolyte interface and cathode electrolyte interface, effectively reducing side reactions at the electrode/electrolyte interfaces. Specifically, the Li|PVTC-g-PVEC|Li symmetric cell can exhibit ultra-long cycle stability for more than 10 000 h (>416 days). The assembled LiFePO4|PVTC-g-PVEC|Li cell and high-voltage LiNi0.8Co0.1Mo0.1O2|PVTC-g-PVEC|Li cell exhibit outstanding cycling stability for 1000 cycles at 2C and 500 cycles at 1C, respectively. The pouch batteries also depict high safety against abusive conditions. This in situ polymerized ferroelectric engineering strategy establishes a new pathway for designing high-performance solid-state lithium batteries.

With the rapid development of electric vehicles, aerospace, and military equipment, the demand for lithium-ion batteries in low-temperature environments is growing. Slow ion transport can lead to capacity decay, increased voltage polarization, and lithium dendrite growth. To improve the wide-temperature performance of lithium-ion batteries, various strategies have been adopted, including high-concentration electrolytes (HCEs), localized high-concentration electrolytes (LHCEs), fluorinated electrolytes, weakly solvated electrolytes (WSEs), double-salt electrolytes, and functional additives. This paper systematically reviews the failure mechanisms of low-temperature electrolytes, analyzes issues ranging from ion transport and electrode/electrolyte interface, compatibility to solvation structures, and details optimization strategies for electrolyte composition. The optimization of electrolyte components is treated in three parts: innovations in solvent systems, optimization of lithium salts, and the development of functional additives. It summarizes research progress on novel electrolyte systems. It further surveys the characterization techniques on which these mechanisms and strategies rest. The paper also outlines future research directions for low-temperature electrolytes, emphasizing the importance of multi-modal characterization and intelligent screening strategies. This review aims to provide theoretical guidance and technical references for the design of high-performance low-temperature electrolytes.

Single-crystal Ni-rich LiNi0.8Co0.1Mn0.1O2 (SC-NCM) layered oxides hold great promise for high-energy-density lithium-ion batteries owing to their high capacity and grain-boundary-free structure, which inherently suppresses intergranular cracking and gas evolution. Yet, their practical deployment is severely hindered by coupled bulk structural collapse and interfacial degradation, especially at extreme temperatures. Herein, a diffusion-driven self-separation strategy is developed for SC-NCM, where the intrinsic diffusivity contrast within a single Li1.3Al0.3Ti1.7(PO4)3 (LATP) precursor drives spontaneous phase separation during one-step ball milling, simultaneously achieving conformal LATP coating with Al gradient doping. This dual modification suppresses the unit‑cell volume variation from 6.57% to 1.65% and significantly improves interfacial kinetics, reducing the charge transfer activation energy from 16.61 kJ·mol-1 to 3.76 kJ·mol-1. The Al gradient doping reinforces the lattice framework to mitigate structural degradation, while the conformal LATP coating suppresses interfacial parasitic reactions and accelerates Li+ transport. The modified cathode delivers exceptional wide-temperature cycling stability, retaining 98% capacity after 500 cycles at −20 °C with an average decay rate of only 0.004% per cycle, and 90% after 200 cycles at 60 °C, and 81% capacity retention after 500 cycles at 1 C in graphite-based full cells. This scalable one-step strategy provides a generalizable platform for stabilizing high-capacity oxide cathodes against structural and interfacial degradation.

Metal-sulfur batteries promise sustainable high-energy storage but are plagued by sulfur-induced catalyst deactivation, which hinders long-term sulfur conversion. Here, we present a concave carbon surface confinement strategy as a universal design principle to stabilize metal catalysts against sulfur poisoning. By embedding cobalt nanoparticles within curved carbon cavities, the intimate metal-carbon contact area is dramatically enlarged, triggering strong and reversible electron transfer from cobalt (Co) to the carbon scaffold. This unique interfacial architecture creates a balanced Co2+/Co0 valence state (Co2+/Co0 ratio approaching unity) and maintains it during cycling, effectively outcompeting electron donation to sulfur species and suppressing the formation of strong Co-S bonds. Benefiting from this architecture, the Co catalyst exhibits a persistently low activation energy (0.195 eV) for the rate-determining polysulfide-to-Li2S conversion and avoids the gradual activity loss typically observed with conventional carbon-supported catalysts. Consequently, lithium-sulfur batteries deliver an ultralow capacity decay of 0.044% per cycle over 1000 cycles, while Ah-level pouch cells achieve gravimetric energy densities of up to 505 Wh kg-1 and sustain 457 Wh kg-1 with only 0.32% per-cycle fading. This carbon confinement not only overcomes sulfur poisoning but also provides a general blueprint for designing durable, high-activity metal catalysts in sulfur-rich electrochemical environments.

Hybrid solid electrolytes (HSEs) offer a promising route to high-performance solid-state lithium batteries, but the chemically and structurally heterogeneous phase boundaries between polymers and fillers impede ion transport. The origin of these phase boundaries and how their components and structure govern Li+ transport kinetics remain elusive. Here, we tackle this issue by comprehensively investigating a series of polyethylene oxide-based HSEs with different preparation conditions where various interfacial reactions occur. We reveal that the strong coordination of anions (such as TFSI-, ClO4- and DFOB-) in the polymer phase accelerates the degradation of the polyphosphate framework. This degradation fosters the formation of resistive phase boundaries, which are primarily responsible for sluggish Li+ kinetics, as revealed by nondestructive cross polarization and exchange-NMR measurements. To address this, we propose a novel lithium tricyanomethanide (LiTCM) as a weakly coordinating additive to regulate interfacial chemistry and reconstruct phase boundaries. As a result, the ionic conductivity of HSEs is enhanced up to 5.48 & times; 10(-4) S cm(-1) (60 degrees C). The developed all-solid-state lithium-sulfur batteries deliver a high specific capacity of 973.6 mAh g(-1), with 0.03% capacity fade per cycle over 300 cycles. It also enables LiFePO4||Li batteries to cycle 300 times with a high capacity retention of 89.5%. This work elucidates the close relationship between the interfacial configuration and Li+ diffusion kinetics and offers fundamental insights for HSE design.

The advancement of flexible electronics demands conductive films overcoming brittleness and resource scarcity, integrating high conductivity, superior flexibility, and green fabrication. Herein, an interface synergistic regulation-driven green strategy is reported to construct layered ternary composite films by self-driven assembly of Carboxymethylcellulose sodium (CMC)-modified single-walled carbon nanotubes, reduced graphene oxide, and graphene oxide under ambient conditions using Cu foil as dual substrate/reductant. Mechanistic studies reveal a multi-dimensional coordination-bridging mechanism regulated by the synergy of Cu⁺ and Cu²⁺ with CMC stabilizing single-walled carbon nanotubes and mediating interfacial interactions. The film with ultra-thin and adjustable thickness (1.8-5.1 μm) exhibits excellent flexibility and high conductivity up to recorded 30,030 S/m, which further boosts to 150,313 S/m after 250 ℃ heat-treatment. This low-energy, equipment-free method enables large-area (18.5×18.5 cm2) and patterned processing, addressing key challenges in multicomponent carbon composite fabrication (dispersion, regulation, and energy consumption) and providing a scalable paradigm for high-performance flexible conductive materials.

The capacity configuration of off-grid photovoltaic-battery-hydrogen coupling systems faces three long-standing challenges: strong source-side uncertainty, multi-timescale coupling, and conflicts among economic cost, reliability, and efficiency. To solve these problems, this paper proposes a capacity configuration method called MPC-AMOO, which combines model predictive control and adaptive multi-objective optimization. First, the method uses the Ward algorithm to extract continuous-time segment clustering scenarios. This step keeps temporal continuity and greatly reduces computational cost. Second, it builds a system operation strategy based on model predictive control. This quantifies the system's performance limits and fully uses its operational potential in capacity optimization. Third, it develops an adaptive-weight multi-objective optimization model that balances economic cost, loss of power supply probability, and PV curtailment rate. Simulation comparisons are made with two other methods: an adaptive multi-objective capacity configuration method based on net power strategy (NP-AMOO), and a fixed-weight model predictive control-based capacity configuration method (MPC-FM). The results show that compared with NP-AMOO and MPC-FM, the proposed MPC-AMOO method increases annual economic cost by about 11.76% and 8.03%, respectively. However, it reduces the loss of power supply probability by 66.4% and 60.0%, and reduces the PV curtailment rate by 22.96% and 37.74%. It achieves clear advantages in supply reliability and energy efficiency. Typical weekly operation analysis further confirms that the proposed method has good look-ahead regulation capability under consecutive low-output conditions. It enables safe and coordinated operation of battery and hydrogen storage. This work shows that moderately sacrificing economic cost for better system resilience is a more practical trade-off strategy in capacity configuration of off-grid multi-energy complementary systems.

Highly anticipated silicon (Si) anode usually suffers from low Coulombic efficiency and rapid capacity decay resulting from intrinsically low electrical conductivity and large volume variation during cycling. Chemical vapor deposition (CVD) has been used to decompose silane and deposit Si within porous carbon scaffolds, offering a practical route to confine Si and shorten transport pathways. Herein, low-cost porous carbon derived from coconut shells was synthesized through a synchronous activation strategy using both H3BO3 and KOH, followed by construction of a Si-C anode by one-step CVD process. Benefiting from boron-induced catalytic graphitization, few-layer graphene was generated on the porous carbon surface. The synchronous activation with both H3BO3 and KOH significantly increased the specific surface area, pore size, and pore volume of the porous carbon. Boron and graphene framework coupling is expected to generate a negative Poisson's ratio effect, thereby mitigating mechanical stress associated with Si volume expansion. As a result, the Si-C anode delivered a high initial specific capacity of 2021 mAh g- 1 and maintained 83.7% of the initial capacity after 250 cycles at 540 mA g- 1, demonstrating enhanced cycling stability. This work would offer a cost-effective route for developing highperformance Si-C anodes and biomass-derived porous carbon precursors.

Electrosynthesis of cyclohexanone oxime, the vital precursor for producing nylon-6, through C-N coupling reaction from cyclohexanone and nitrate serves as an environmentally friendly route to substitute for conventional technology. However, an electrocatalyst with a single active site is not sufficient to realize the co-adsorption and co-activation of various reactants, which is not conducive to the C-N coupling processes, resulting in the unsatisfactory selectivity and Faraday efficiency of cyclohexanone oxime. Here, we present a geometrically ordered PdCu (O-PdCu) catalyst with high-density dual active sites to efficiently synthesize cyclohexanone oxime via co-reduction of cyclohexanone and nitrate. Operando measurements and control experiments reveal that O-PdCu can generate more NH2OH intermediates to react with cyclohexanone, and the geometric structure with highly ordered and high-density Pd-Cu dual active sites is more favorable to the C-N coupling process, thereby enhancing the performance of cyclohexanone oxime electrosynthesis. Consequently, the O-PdCu achieves selectivity in organic products and Faradaic efficiency of 100% and 70.75% at -0.4 V vs RHE, respectively. Furthermore, the O-PdCu catalyst facilitates the production of 2.20 g of cyclohexanone oxime with a yield rate of 4.82 mmol cm-2 h-1 at a current of 1.12 A through a large-scale synthesis process. Technoeconomic analysis further indicates that the electrosynthesis of cyclohexanone oxime in our system represents a feasible and economically profitable strategy.

Pulsed electrolysis is widely regarded as a promising strategy for enhancing the performance of the electrocatalytic nitrate reduction reaction (NO3-RR). However, research on the effect of symmetric and asymmetric pulsed electrolysis on the NO3-RR remains elusive. Here, the CuMn alloy serves as a model catalyst to systematically investigate the impact of symmetric and asymmetric pulsed electrolysis on the performance of NO3-RR. A series of operando measurements and control experiments indicate that a suitable asymmetric pulsed electrolysis can optimize the local microenvironment of the NO3-RR, including optimizing the coverage of NO3-, enhancing the generation of key N-containing intermediates, and inhibiting the hydrogen evolution reaction, thereby improving the Faradaic efficiency and yield rate of NH3. Consequently, the Faradaic efficiency and yield rate of NH3 for the optimal asymmetric pulsed electrolysis between a less negative potential time of 2 s and a more negative potential time of 4 s are 94.03% and 9.13 mg h-1 cm-2, respectively, which are 1.42-fold and 2.10-fold higher than those of static electrolysis. Moreover, the Faradaic efficiency of NH3 for the optimal asymmetric pulsed electrolysis was 66.32% at a lower concentration of NO3- (2000 ppm), which is 1.73-fold higher than that of static electrolysis, indicating that the performance of asymmetric pulsed electrolysis is further enhanced in the lower concentration of NO3-, further confirming that asymmetric pulsed electrolysis is a feasible strategy to improve the performance of the NO3-RR.

The development of poly(vinylidene fluoride)-based composite solid-state electrolytes is severely hindered by slow Li+ transport and unstable solid-state electrolyte interphases. This study addresses these challenges by proposing a supramolecular ligand intervention strategy using 18-crown-6 as an additive. Coordination between the large-pore crown ethers and Li+ promotes lithium bis(fluorosulfonyl)imide dissociation and increases the free Li+ concentration, thereby enhancing ion transport with a high ionic conductivity and an improved Li+ transference number. Moreover, this coordination homogenizes the Li+ flux, suppressing side reactions and dendrite formation. Consequently, the modified electrolyte significantly enhances the cycling stability of Li||Li cells up to 800 h with a reduced overpotential. Additionally, the Li||NCM811 cells delivered 84.2% capacity retention after 2500 cycles at 10C, and retained 72.5% capacity after 780 cycles even at a high cut-off voltage of 4.5 V at 5C. Structural and interfacial characterizations confirmed the formation of a dense LiF/Li3N-rich SEI layer, which enhances mechanical strength and ionic transport. This study provides a robust modification approach using supramolecular ligands to achieve high-performance solid-state lithium-metal batteries.

The inherent limitation of Li+ transport and resulting severe concentration polarization in solid-state electrolytes have hindered the practical application of lithium metal batteries. Addressing this challenge, here we create a piezoelectric polymeric composite electrolyte based on poly(vinylidene fluoride) blended with 0.5Ba(Zr0.2Ti0.8)O3-0.5(Ba0.7Ca0.3)TiO3, which exploits volume fluctuations of lithium metal negative electrodes during cycling to activate a piezo-assisted electromechanical coupling effect. The resulting gradient piezo-field within the prepared electrolyte selectively accelerates Li+ while impedes anions movement, thereby effectively suppressing concentration polarization fundamentally. Consequently, the prepared electrolytes exhibit relatively low concentration polarization, enabling a high critical current density of 3.7 mA cm-2, stable Li plating/stripping even at high current density of 2 mA cm-2, and prolonged cycling stability of Li | |Ni0.8Co0.1Mn0.1O2 full cell over 2600 times at the specific current of 900 mA g-1 within a potential window of 2.8 to 4.5 V. This work proposes a mechanical-electrochemical conversion strategy by constructing a piezoelectric electrolyte that actively utilizes the unavoidable volume fluctuation of lithium metal to minimize Li+ concentration gradient, offering a promising pathway towards high-performance lithium metal batteries.

Manganese hexacyanoferrate (MnHCF) has a high output voltage and is expected to be a promising cathode material for high energy density sodium-ion batteries (SIBs). However, the capacity decay problem caused by the Jahn-Teller effect of high-spin Mn3+ restricts its use in sodium-ion batteries. In this study, an elemental modulation strategy is proposed to regulate the electronic state of the ligand field by introducing the nickel element, which can keep the Mn in a low-spin configuration during cycling to inhibit the Jahn-Teller aberration of MnHCF. The nickel-doped MnHCF (NLS2-PW) with low-spin electronic state inhibits the disproportionation and dissolution process of Mn3+ and thus exhibits excellent cycling stability, and its capacity retention is close to 80% after 600 cycles at 2 C with a reduction of the Mn dissolution by ≈70%. Combined with theoretical calculations, it is confirmed that the distortion of the MnN6 octahedron in NLS2-PW is reduced significantly, and the tetragonal phase transition caused by the Jahn-Teller effect during the electrochemical process is also effectively suppressed. This work demonstrates an efficient modulation strategy to enhance the performance of the Prussian blue analog cathode of sodium-ion batteries, being favorable for the design and optimization of relevant PB analogues for SIB applications.

The low concentration and inhomogenous distribution of free lithium ion (Li + ) in composite polymer electrolytes (CPEs) greatly restrict the Li + transport, cycle stability and rate performance of all solid‐state batteries. In this work, lithium zirconate with superficial oxygen (O)‐vacancies (O‐LZO) is reported as a new Li + conductors for polyethylene oxide (PEO)‐based CPEs (PEO@O‐LZO). The O‐LZO demonstrates exceptional Li + transport capability, and its superficial O‐vacancies efficiently adsorb anions to facilitate the dissociation of lithium salts, leading a high concentration of free Li + in CPEs. Furthermore, the electropositive equilibrium charge layer of O‐vacancies avoids the aggregation of Li + near the filler and achieves a stable interface to promote the efficient and continuous Li + transport. These effects contribute to a high Li + conductivity of 1.63 × 10 −4 S cm −1 and a Li + migration number of 0.35 for PEO@O‐LZO at 40 °C. The assembled battery (LiFePO 4 /PEO@O‐LZO/Li) exhibits a capacity of 120 mAh g −1 at 3 C and stable cycling performance with an 80.5% capacity retention after 800 cycles at 1 C and 40 °C, maintaining excellent coulombic efficiency. This work provides a design principle of fillers to regulate Li + concentration and distribution in CPEs for efficient solid‐state lithium metal batteries.