Building a highly concentration responsive optical thermometer via tunable electron transfer pathways supported by intervalence charge transfer states.

The thermal-coupled levels (TCLs) of lanthanides have attracted great attention in the field of optical thermometer, offering an efficient method to achieve non-contect temperatuer feedback in complex environment. However, the iner 4f electrons are shielded, which becomes the core obstacle in improving the sensing performance. This issue is now circumvented by constructing an electron transfer pathway between Tm3+(1D2) and Eu3+(5D0) configurations. As a result, the electron transfer barrier is related to the relative temperature sensitivity, giving an insight into the modulation mechanism. Compared to the conventional TCLs systems, the relative temperature sensitivity of this strategy is highly concentration-responsive, increasing from 5.56 to 10.1 % K-1 as the Eu3+ molar concentration rises from 0.3 to 0.5 mol%. This work reveals the inner emission mechanism based on IVCT-supported emission mode, and presents the highly adjustability of sensing performance.

Reflectance spectroscopy analysis and lithium content estimation in lithium-rich rocks and stream sediments: Insights from Tuanjie Peak, Western Kunlun, China.

Lithium, a rare metal of strategic importance, has garnered heightened global attention. This investigation delves into the laboratory visible-near infrared and short-wavelength infrared reflectance (VNIR-SWIR 350 nm-2500 nm) spectral properties of lithium-rich rocks and stream sediments, aiming to elucidate their quantitative relationship with lithium concentration. This research seeks to pave new avenues and furnish innovative technical solutions for probing sedimentary lithium reserves. Conducted in the Tuanjie Peak region of Western Kunlun, Xinjiang, China, this study analyzed 614 stream sediments and 222 rock specimens. Initial steps included laboratory VNIR-SWIR spectral reflectance measurements and lithium quantification. Following the preprocessing of spectral data via Savitzky-Golay (SG) smoothing and continuum removal (CR), the absorption positions (Pos2210nm, Pos1910nm) and depths (Depth2210, Depth1910) in the rock spectra, as well as the Illite Spectral Maturity (ISM) of the rock samples, were extracted. Employing both the Successive Projections Algorithm (SPA) and genetic algorithm (GA), wavelengths indicative of lithium content were identified. Integrating the lithium-sensitive wavelengths identified by these feature selection methods, A quantitative predictive regression model for lithium content in rock and stream sediments was developed using partial least squares regression (PLSR), support vector regression (SVR), and convolutional neural network (CNN). Spectral analysis indicated that lithium is predominantly found in montmorillonite and illite, with its content positively correlating with the spectral maturity of illite and closely related to Al-OH absorption depth (Depth2210) and clay content. The SPA algorithm was more effective than GA in extracting lithium-sensitive bands. The optimal regression model for quantitative prediction of lithium content in rock samples was SG-SPA-CNN, with a correlation coefficient prediction (Rp) of 0.924 and root-mean-square error prediction (RMSEP) of 0.112. The optimal model for the prediction of lithium content in stream sediment was SG-SPA-CNN, with an Rp and RMSEP of 0.881 and 0.296, respectively. The higher prediction accuracy for lithium content in rocks compared to sediments indicates that rocks are a more suitable medium for predicting lithium content. Compared to the PLSR and SVR models, the CNN model performs better in both sample types. Despite the limitations, this study highlights the effectiveness of hyperspectral technology in exploring the potential of clay-type lithium resources in the Tuanjie Peak area, offering new perspectives and approaches for further exploration.

In Situ Forming Asymmetric Gel Polymer Electrolyte Enhances the Performance of High-Voltage Lithium Metal Batteries.

With the rapid evolution of electric vehicle technology, concerns regarding range anxiety and safety have become increasingly pronounced. Battery systems with high specific energy and enhanced security, featuring ternary cathodes paired with lithium (Li) metal anodes, are poised to emerge as next-generation electrochemical devices. However, the asymmetric configuration of the battery structure, characterized by the robust oxidative behavior of the ternary cathodes juxtaposed with the vigorous reductive activity of the Li metal anodes, imposes elevated requisites for the electrolytes. Herein, a well-designed gel polymer electrolyte with asymmetric structure was successfully prepared based on the Ritter reaction of cyanoethyl poly(vinyl alcohol) (PVA-CN) and cationic ring-opening polymerization of s-Trioxane. With the aid of the sieving effect of separator, the in situ asymmetric gel polymer electrolyte has good compatibility with both the high-voltage cathodes and Li anodes. The amide groups generated by PVA-CN after the Ritter reaction and additional cyano groups can tolerate high voltages up to 5.1 V, matching with ternary cathodes without any challenges. The functional amide and cyano groups participate in the formation of the cathode electrolyte interface and stabilize the cathode structure. Meanwhile, the in situ formed ether-based polyformaldehyde electrolyte is beneficial for promoting uniform Li deposition on anode surfaces. Li-Li symmetric cells demonstrate sustained stability over 2000 h of cycling at a current density of 1 mA cm-2 for 1 mAh cm-2. Furthermore, the capacity retention rate of Li(Ni0.6Mn0.2Co0.2)O2-Li cells with 0.5 C cycling after 300 cycles is 92.2%, demonstrating excellent cycle stability. The electrolyte preparation strategy provides a strategy for the progress of high-performance electrolytes and promotes the rapid development of high-energy-density Li metal batteries.

Dramatic Enhancement Enabled by Introducing TiN into Bread-like Porous Si-Carbon Anodes for High-Performance and Safe Lithium Storage.

Doping modifications and surface coatings are effective methods to slow volume dilatation and boost the conductivity in silicon (Si) anodes for lithium-ion batteries (LIBs). Herein, using low-cost ferrosilicon from industrial production as the energy storage material, a bread-like nitrogen-doped carbon shell-coated porous Si embedded with the titanium nitride (TiN) nanoparticle composite (PSi/TiN@NC) was synthesized by simple ball milling, etching, and self-assembly growth processes. Remarkably, the porous Si structure formed by etching the FeSi2 phase in ferrosilicon alloys can provide buffer space for significant volume expansion during lithiation. Highly conductive and stable TiN particles can act as stress absorption sites for Si and improve the electronic conductivity of the material. Furthermore, the nitrogen-doped porous carbon shell further helps to sustain the structural stability of the electrode material and boost the migration rate of Li-ions. Benefiting from its unique synergistic effect of components, the PSi/TiN@NC anode exhibits a reversible discharge capacity up to 1324.2 mAh g-1 with a capacity retention rate of 91.5% after 100 cycles at 0.5 A g-1 (vs fourth discharge). Simultaneously, the electrode also delivers good rate performance and a stable discharge capacity of 923.6 mAh g-1 over 300 cycles. This research can offer a potential economic strategy for the development of high-performance and inexpensive Si-based anodes for LIBs.

Investigation of polypyrrole based composite material for lithium sulfur batteries.

With the rising demand for electricity storage devices, the performance requirements for such equipment have become increasingly stringent. Lithium-sulfur (Li-S) batteries are poised to be among the next generation of energy storage systems. However, before they can be commercially viable, several challenges must be addressed, including low sulfur conductivity and the shuttle effect. Herein, polypyrrole based sulfur composite was prepared by simple method in hydrothermal teflon lined autoclave for Li-S battery. The S/SP/ppy/PVDF electrode exhibited the initial discharge capacity of 662 mAh g- 1 at 0.5 C and 637 mAh g- 1 after 100 cycles. The Coulombic efficiency was 96% all along charge/discharge cycling. Moreover, Li-S coin cells were assembled and tested to demonstrate the potential application and scale-up of the polypyrrole-sulfur composite.

Biomimetic Aramid Nanofiber/ß-FeOOH Composite Coating for Polypropylene Separators in Lithium-Sulfur Batteries.

Aramid nanofibers (ANFs), with attractive mechanical and thermal properties, have attracted much attention as key building units for the design of high-performance composite materials. Although great progress has been made, the potential of ANFs as fibrous protein mimetics for controlling the growth of inorganic materials has not been fully revealed, which is critical for avoiding phase separation associated with typical solution blending. In this work, we show that ANFs could template the oriented growth of ß-FeOOH nanowhiskers, which enables the synthesis of ANFs/ß-FeOOH hybrids as composite coatings for polypropylene (PP) separators in Li-S batteries. The modified PP separator exhibits enhanced mechanical properties, heightened thermal performance, optimized electrolyte wettability, and improved ion conductivity, leading to superior electrochemical properties, including high initial specific capacity, better rate capability, and long cycling stability, which are superior to those of the commercial PP separators. Importantly, the addition of ß-FeOOH to ANFs could further contribute to the suppression of lithium polysulfide shuttling by chemical immobilization, inhibition of the growth of lithium dendrites because of the intrinsic high modulus and hardness, and promotion of reaction dynamics due to the catalytic effect. We believe that our work may provide a potent biomimetic pathway for the development of advanced battery separators based on ANFs.

Preparation and Performance Investigation of Carbon-Coated Li1.2Mn0.2Ti0.6O2/C Cathode Materials.

Mn-based cation disordered rock-salt (DRX) cathode materials exhibit promising application prospects due to their cost-effectiveness and high specific capacity. However, the synthesis methods commonly employed for these materials rely on the solid-state reaction method and mechanochemistry method, primarily attributed to the influence of low-valence states of Mn. Currently, sol-gel approaches for preparing Mn-based DRX cathode materials are limited to systems involving Mn3+. Furthermore, there is a paucity of research regarding the modification of Mn-based DRX. To address this concern, the submicrometer-sized carbon-coated Li1.2Mn0.2Ti0.6O2/C materials were synthesized via a one-step sintering process using the sol-gel method with sucrose as the carbon source, resulting in smaller particle sizes compared to those prepared by the solid-state reaction at the same temperature. When employed as a cathode material for lithium batteries, samples prepared with 10 wt % sucrose exhibited exceptional cycling stability by delivering an initial discharge specific capacity of 119.6 mA h g-1 (at a current density of 20 mA g-1). After 20 charge-discharge cycles, a reversible specific capacity of 91.0 mA h g-1 was achieved, with a capacity retention rate of 76.1%. This approach provides distinctive insights and strategies for the preparation and modification of manganese-titanium-based disordered rock-salt cathode materials.

Laser-Induced Solid-Phase Strategy to Synthesize Single-Atomic Lithiophilic Sites Enabled Dendrite-Free Lithium Deposition on Graphene Matrix.

The introduction of metal Single-atom (SA) to construct lithium-philic active sites shows the ability to guide uniform lithium deposition and improve the stability of lithium hosts. Nevertheless, the development of facile and expedient methods for synthesizing SA remains a considerable challenge. Herein, The SA metal loaded on graphene (Bi@LrGO) is designed by laser-induced solid-phase strategy. The bismuth salts simultaneously decompose under the high local temperature and in the reductive atmosphere induced by laser to form SA metal. Simultaneously, graphene oxide (GO) nanosheets absorb photon energy to be reduced/graphitized into graphene, which serves as anchoring sites for Bismuth Sing-atom (Bi SA) immobilization. The SA metals, supported on the graphene not only provide sufficient lithiophilic sites but also significantly increase the adsorption energy (-2.11 eV) with lithium atoms, promote the uniform nucleation and deposition of lithium, and inhibit the growth of lithium dendrites. Additionally, the layered structure of the graphene film adapts to the volume change during the repeated lithium plating/stripping process. Therefore, the symmetrical battery-based Li deposited on Bi@LrGO (Bi@LrGO@Li) achieves an ultra-long stable cycle life of ≈2400 h at 1 mA cm-2. In particular, a full cell with LiFePO4 cathode provides a good capacity retention of 81.2% at 4 C after 600 cycles.

Study on the Commercial Metalized Plastic Current Collector PET-Cu and PP-Cu Toward High-Energy Lithium-Ion Battery.

Commercial metalized plastic current collector (MPCC) is receiving widespread attention from the business and academic communities, due to its properties of excellent electrical conductivity and low mass density. However, the application of MPCC on the side of copper is rarely studied. Herein, sandwich-like polyethylene terephthalate-based (PET) and polypropylene-based (PP) copper (Cu) current collectors via magnetron sputtering and electroplating are fabricated. Most importantly, the electrical performance, mechanical safety quality, and revealed the corresponding failure mechanism for the MPCC cells are first systematically evaluated. First, during the 45 °C electrical cycling tests, PET-Cu CC (82.67%) and PP-Cu CC (82.32%) cells both have comparable capacity retention with the traditional Cu CC (Tra-Cu CC) cell (84.55%) after 500 cycles. The slight reduction in the cycling performance is induced by the crack of the Cu layer around the embedded SiO2 particle for PET-Cu CC cell and the detachment of Cu layer for PP-Cu CC cell. Second, during the nail-penetration test, MPCC cells maintain no fire and explosion for more than 5 min, since the heat-shrinkable function of polymeric film can interrupt the continuous Joule heat released by internal short-circuit. This work provides important guidance for the large-scale application of MPCC in the field of lithium-ion batteries.

Confined Polyethylene Glycol Anchored in Kaolinite as High Ionic Conductivity Solid-State Electrolyte for Lithium Batteries.

Solid-state electrolytes (SSEs) have garnered significant attention as critical materials for enabling safer, energy-dense, and reversible electrochemical energy storage in batteries. Among the various types of solid electrolytes developed, composite polymer electrolytes (CPEs) have stood out as some of the most promising candidates due to their well-rounded performance. In this study, we choose polyethylene glycol (PEG) as the covalent grafting intercalant and lithium perchlorate as carrier source to prepare a fast lithium ion conductor, K-PEG-Li doped with clay-based active filler as a CPE. The CPE exhibits excellent lithium conduction (4.36 × 10-3 S cm-1 at 25 °C and 3.32 × 10-2 S cm-1 at 115 °C), great mechanical performance with good tensile strength (6.07 MPa) and toughness (strain 313%), and convincing flame-retardancy. These outstanding conducting and mechanical functionalities indicate that such a clay-based active filler doped composite polymer electrolyte will find promising application in solid-state lithium batteries.

Enhanced Critical Current Density in the Garnet Oxide Electrolyte by a Silver Interlayer.

Ta-doped Li6.4La3Zr1.4Ta0.6O12 (LLZTO) for solid-state lithium batteries demonstrates encouraging performance; however, they encounter issues with lithium dendrite formation that impede their widespread use. Herein, we design a LLZTO ceramic with an interlayer containing a mixed dense layer of Ag and LLZTO, prepared by one-step sintering. The Ag-rich interlayer in LLZTO can hinder the growth and the penetration of lithium dendrites though the reaction between Ag and lithium metal. Compared with the Ag-free counterpart, a higher critical current density of 0.6 mA cm-2, in addition to a longer life span under a current density of 0.2 mA cm-2, is achieved by adopting the interlayer in LLZTO. This research offers novel insights into the engineering of garnet-based solid electrolytes, tailored for the advancement of high-rate lithium metal batteries.

Aligned Ion Conduction Pathway of Polyrotaxane-Based Electrolyte with Dispersed Hydrophobic Chains for Solid-State Lithium-Oxygen Batteries.

A critical challenge hindering the practical application of lithium-oxygen batteries (LOBs) is the inevitable problems associated with liquid electrolytes, such as evaporation and safety problems. Our study addresses these problems by proposing a modified polyrotaxane (mPR)-based solid polymer electrolyte (SPE) design that simultaneously mitigates solvent-related problems and improves conductivity. mPR-SPE exhibits high ion conductivity (2.8 × 10-3 S cm-1 at 25 °C) through aligned ion conduction pathways and provides electrode protection ability through hydrophobic chain dispersion. Integrating this mPR-SPE into solid-state LOBs resulted in stable potentials over 300 cycles. In situ Raman spectroscopy reveals the presence of an LiO2 intermediate alongside Li2O2 during oxygen reactions. Ex situ X-ray diffraction confirm the ability of the SPE to hinder the permeation of oxygen and moisture, as demonstrated by the air permeability tests. The present study suggests that maintaining a low residual solvent while achieving high ionic conductivity is crucial for restricting the sub-reactions of solid-state LOBs.

Reductive Dissolution of NCM Cathode through Anaerobic Respiration by Shewanella putrefaciens.

The consumption of lithium-ion batteries (LIBs) has considerably increased over the past decade, leading to a rapid increase in the number of spent LIBs. Exposing spent LIBs to the environment can cause serious environmental harm; however, there is a lack of experimentally obtained information regarding the environmental impacts of abandoned cathode materials. Here, we report the interactions between Shewanella putrefaciens, a microorganism commonly found in diverse low-oxygen natural settings, and LiNi0.6Co0.2Mn0.2O2 (NCM622) under anaerobic conditions. We present compelling evidence that the anaerobic respiration of Shewanella putrefaciens triggers ∼59 and ∼78% dissolution of 0.2 g/L pristine and spent NCM622, respectively. We observed that Shewanella putrefaciens interacted with the pristine and the spent NCM622 under anaerobic conditions at a neutral pH and room temperature and induced the reduction of Ni, Co, and Mn, resulting in the subsequent dissolution of Li, Ni, Co, and Mn. Moreover, we found that secondary mineralization occurred on the surface of reacted NCM622. These findings not only shed light on the substantial impact of microbial respiration on the fate of discarded cathode materials in anaerobic environments but also reveal the potential for sustainable bioleaching of cathodes in spent LIBs.

Selective Methylation of Cyclic Ether Towards Highly Elastic Solid Electrolyte Interphase for Silicon-based Anodes.

Silicon (Si)-based anodes offer high theoretical capacity for lithium-ion batteries but suffer from severe volume changes and continuous solid electrolyte interphase (SEI) degradation. Here, we address these challenges by selective methylation of 1,3-dioxolane (DOL), thus shifting the unstable bulk polymerization to controlled interfacial reactions and resulting in a highly elastic SEI. Comparative studies of 2-methyl-1,3-dioxolane (2MDOL) and 4-methyl-1,3-dioxolane (4MDOL) reveal that 4MDOL, with its larger ring strain and more stable radical intermediates due to hyperconjugation effect, promotes the formation of high-molecular-weight polymeric species at the electrode-electrolyte interface. This elastic, polymer-rich SEI effectively accommodates volume changes of Si and inhibits continuous side reactions. Our designed electrolyte enables Si-based anode to achieve 85.4% capacity retention after 400 cycles at 0.5 C without additives, significantly outperforming conventional carbonate-based electrolytes. Full cells also demonstrate stable long-term cycling. This work provides new insights into molecular-level electrolyte design for high-performance Si anodes, offering a promising pathway toward next-generation lithium-ion batteries with enhanced energy density and longevity.

Artificial Lithium Channels Built from Polymers with Intrinsic Microporosity.

In sharp contrast to numerous artificial potassium channels developed over the past decade, the study of artificial lithium-transporting channels has remained limited. We demonstrate here the use of an interesting class of polymers with intrinsic microporosity (PIM) for constructing artificial lithium channels. These PIM-derived lithium channels show exceptionally efficient (γLi+ > 40 pS) and highly selective transport of Li+ ions, with selectivity factors of > 10 against both Na+ and K+. By simply adjusting the initial reaction temperature, we can tune the transport property in a way that PIMs synthesized at initial reaction temperatures of 60 °C and 80°C exhibit improved transport efficiency and selectivity, respectively, in the dioleoyl phosphatidylcholine  membrane.

Dual-Interphase-Stabilizing Sulfolane-Based Electrolytes for High-Voltage and High-Safety Lithium Metal Batteries.

High-voltage Li metal battery (HV-LMB) is one of the most promising energy storage technologies to achieve ultrahigh energy density. Nevertheless, electrolytes reported to date are difficult to simultaneously stabilize the Li metal anode and high-voltage cathode, especially without the assistance of expensive and corrosive high-concentration Li salts. Herein, a dual-interphase-stabilizing (DIS) and safe electrolyte that bypasses the high-concentration Li salt is reported. The electrolyte consists of high-flash-point sulfolane as solvent, molecular-orbital-engineered additives that enable stable B-F rich cathodic interphase, and unique C-F rich organic anodic interphase. The stable cycling of both Li metal anode and 4.75 V-LiCoO2 cathode in the DIS electrolyte (> 500 cycles) is demonstrated. HV-LMB pouch cells of a high energy density (435 Wh kg-1) can sustainably operate for more than 100 cycles. Moreover, the low cost and high thermal stability of the DIS electrolyte offer superior cost-effectiveness and safety for large-scale applications of HV-LMBs in the future.

Effect of preparation design on fracture resistance of molars restored with occlusal veneers of different CAD-CAM materials: an in vitro study.

BACKGROUND: Occlusal veneer had been evaluated for mechanical properties using lithium disillicate. However, studies evaluating the mechanical properties of occlusal veneer with different preparation designs and ceramic materials are lacking. So, this in vitro study aimed to evaluate the fracture resistance of occlusal veneers with two designs fabricated from two different ceramic materials. MATERIAL AND METHODS: Fourty mandibular third molars were distributed to 2 groups (n = 20) according to preparation design: group (O) anatomical occlusal reduction and group (OA) anatomical occlusal and 1 mm axial reduction. Each group was additionally subdivided into two subgroups (n = 10) according to ceramic materials; in subgroup X, lithium disilicate (e.max CAD, Ivoclar AG, Schaan, Liechtenstein) was used, and in subgroup S, zirconia-reinforced lithium silicate (ZLS) (Vita Suprinity, VitaZahnfabrik, Bad Säckingen, Germany) was used. All specimens were cemented with a light-cure resin cement (Choice 2, Bisco, Schaumburg, USA). 5000 thermocycles were applied to all specimens with both temperatures of 5 °C and 55 °C in two water baths; the dwell time was 30s at each bath, and the transfer time was 10s. Then all specimens were subjected to a fatigue simulation under dynamic loading of 200 N for 250,000 cycles. A universal testing machine (5500R/1123, Instron, Norwood, USA) was used to evaluate the fracture strength with a crosshead speed of 1 mm/min. All data were analyzed statistically by using a two-way ANOVA, and for some violations of assumptions, these results were compared with those obtained by the nonparametric test (Scheirer Ray Hare) (α = 0.05). RESULTS: A statistically significantly higher fracture resistance in the 'OA' (3389 N) compared to the 'O' (2787 N) group regardless of the ceramic material (P < .001) and a statistically significantly higher fracture resistance in the 'X' (3295 N) compared to the 'S' (2881 N) regardless of the preparation design (P = .015). CONCLUSIONS: For occlusal veneers, all preparation designs and materials (such as Vita Suprinity and e.max CAD) had clinically acceptable fracture resistance values that were greater than the maximal biting forces. On the other hand, the e.max CAD with occlusal veneer, including axial reduction design, demonstrated the maximum fracture resistance value. Finally, no relationship between fracture strength and mode of failure was found.

Artificial Electron Channels Enable Contact Prelithiation of Li-Ion Battery Anodes with Ultrahigh Li-Source Utilization.

Contact prelithiation is widely used for compensating the initial capacity loss of lithium-ion batteries (LIBs). However, the low Li-source utilization suffering from the deteriorated contact interfaces results in cycling degeneration. Herein, Li-Ag alloy-based artificial electron channels (AECs) are established in Li source/graphite anode contact interfaces to promote Li-source conversion. Due to the shielding effect of the Li-Ag alloy (50 at. % Li) on Li-ion diffusion, the dry-state corrosion of contact interfaces is restricted. The unblocked electronic conduction across the AEC-involved interface not only facilitates the Li source conversion but also accelerates the prelithiation kinetics during the wet-state process, resulting in an ultrahigh Li-source utilization (90.7%). Thereby, implementing AEC-assisted prelithiation in a LiNi0.5Co0.2Mn0.3O2 pouch cell yields a 35.8% increase in energy density and stable cycling over 600 cycles. This finding affords significant insights into the construction of an efficient prelithiation technology toward the development of high-energy LIBs.

A Versatile Metal-Organic-Framework Pillared Interlayer Design for High-Capacity and Long-Life Lithium-Sulfur Batteries.

Developing high-performance lithium-sulfur batteries is a promising way to attain higher energy density at lower cost beyond the state-of-the-art lithium-ion battery technology. However, the major issues blocking their practical application are the sluggish kinetics and parasitic shuttling reactions for sulfur and polysulfides. Here, pillaring multilayer graphene with the metal-organic framework (MOF) demonstrates the substantial impact of a versatile interlayer design in tackling those issues. Unlike regular composite separators reported so far, the participation of tri-metallic Ni-Co-Mn MOF (NCM-MOF) as pillars supports the construction of an ion-channel interconnected interlayer structure, unexpectedly balancing the interfacial concentration polarization, spatially confining the soluble polysulfides and vastly affording lithiophilic sites for highly efficient polysulfide sieving/conversion. As a demonstration, we show that the MOF-pillared interlayer structure enables outstanding capacity (1634 mAh g-1 at 0.1C) and longevity (average capacity decay of 0.034% per cycle in 2000 cycles) of lithium-sulfur batteries. Besides, the multilayer separator can be readily integrated into the high-nickel cathode (LiNi0.91Mn0.03Co0.06O2)-based lithium-ion batteries, which efficiently suppresses the undesired phase evolution upon cycling. These findings suggest the potential of "gap-filling" materials in fabricating multi-functional separators, bring forward the pillared interlayer structure for energy-storage applications.

A Room-Temperature Lithium-Restocking Strategy for the Direct Reuse of Degraded LiFePO4 Electrodes.

The sustainable development of lithium iron phosphate (LFP) batteries calls for efficient recycling technologies for spent LFP (SLFP). Even for the advanced direct material regeneration (DMR) method, multiple steps including separation, regeneration, and electrode refabrication processes are still needed. To circumvent these intricacies, new regeneration methods that allow direct electrode reuse (DER) by rejuvenating SLFP electrodes without damaging its structure are desired. Here, a 0.1 M lithium triethyl borohydride/tetrahydrofuran solution, which has the proper reductive capability to reduce Fe3+ in SLFP to Fe2+ without alloying with the aluminum current collector, is selected as the lithiation/regeneration reagent to restock the Li loss and regenerate SLFP electrodes. By soaking the SLFP electrodes in the lithiation solution, we successfully rejuvenated the crystal structure and electrochemical activity of SLFP electrodes with structural integrity within only 6 minutes at room temperature. When being directly reused, the regenerated LFP electrodes deliver a high specific capacity of 162.6 mAh g-1 even after being exposed to air for 3 months. The DER strategy presents significant economic and environmental benefits compared with the DMR method. This research provides a timely and innovative solution for recycling spent blade batteries using large-sized LFP electrodes, boosting the closed-loop development of LFP batteries.