Commercial polypropylene (PP) separators offer low cost and established manufacturability, but their limited electrolyte affinity and thermal dimensional stability can restrict their performance in sodium-ion batteries. In this study, a commercial Celgard 2400 separator was modified through a multistep route comprising polydopamine (PDA) deposition, L-lysine-assisted SiO2 colloid treatment, and a final 1,1′-carbonyldiimidazole-assisted interfacial treatment. A binder-assisted PP-SiO2 separator was used as a physical-coating control. SEM, EDS, and ATR-FTIR supported the formation of a relatively dispersed SiO2-containing surface layer with retained visible microporous features and a modified interfacial chemical environment. PP-PDA-SiO2 exhibited a total thickness of 26.90 ± 0.36 μm and apparent area shrinkage ratios of 18.42 ± 1.44

Although lithium-sulfur (Li-S) batteries have broad market prospects owing to their high theoretical energy density and potential cost-effectiveness, their practical application still faces serious shuttle effects of polysulfides (LiPSs) and sluggish redox kinetics. In this study, a cobalt-organic framework, ZIF-67, decorated balsa wood matrix (ZIF-67/BW) was utilized to prepare a cobalt-nitrogen-encapsulated carbon host (Co-N/CBW) with dual-stage-order microchannels for self-standing cathodes in high-performance Li-S batteries. The first-stage-order microchannels inherited from wood provided fast transmission paths for electrolyte. The ZIF-67 derived Co-N carbon particles with the second-stage-order microchannels provided strong chemical adsorption and enhanced conversion kinetics for LiPSs. Owing to these advantages, the Co-N/CBW/Li2S8 cathode exhibited a high initial discharge specific capacity of 1213.1 mAh g-1 at 0.1 C and good cycling stability at 0.5 C (590 mAh g-1 after 200 cycles). By increasing the sulfur loading to 5.97 mg cm-2, the cathode maintained a remarkable area-specific capacity (3.42 mAh cm-2) after 100 cycles. This work proposes a strategy for the cooperation of the catalyst and matrix, providing more possibilities for the development of Li-S batteries. (c) 2025 The Society of Powder Technology Japan. Published by Elsevier B.V. and The Society of Powder Technology Japan. All rights are reserved, including those for text and data mining, AI training, and similar technologies.

The electrochemical performance of Li composite anodes can be enhanced by introducing a three-dimensional host structure with a gradient configuration. However, the undesirable Li dendrites and Li top-growth behavior are difficult to tackle since the conventional lithiophilicity/conductivity gradient is quickly attenuated with the cycling. Herein, a pore-size gradient is hybridized with a lithiophilic gradient by simply infiltrating molten Li-Mg alloy into the bottom of a double-layered carbon paper host consisting of a macroporous carbon fiber (CF) layer and a microporous carbon black (CB) particle layer. When the CF layer is on the upper side and the Li-Mg alloy is composited with the CB layer at the bottom, the as-formed dual-gradient electrode with the positive pore-size gradient shows the best performance compared with the nongradient, single lithiophilicity gradient, and negative pore-size dual-gradient Li composite electrodes. The symmetric cell with the positive pore-size dual-gradient electrode runs for 2200 h at 1 mA cm-2 and 1 mAh cm-2 in a carbonate-based electrolyte, and LiFePO4-based full cell with an extremely low negative/positive ratio of ∼1.26 demonstrates capacity retention of ∼85.7% after 650 cycles. The synergistic effect between the positive pore-size gradient and lithiophilicity gradient ensures a bottom-up Li deposition behavior and prevents the growth of Li dendrites, leading to improved performance toward practical applications.

Lithium (Li) metal anode (LMA) is one of the most promising anodes for high energy density batteries. However, its practical application is impeded by notorious dendrite growth and huge volume expansion. Although the three-dimensional (3D) host can enhance the cycling stability of LMA, further improvements are still necessary to address the key factors limiting Li plating/stripping behavior. Herein, porous copper (Cu) foam (CF) is thermally infiltrated with molten Li-rich Li-zinc (Li-Zn) binary alloy (CFLZ) with variable Li/Zn atomic ratio. In this process, the LiZn intermetallic compound phase self-assembles into a network of mixed electron/ion conductors that are distributed within the metallic Li phase matrix and this network acts as a sublevel skeleton architecture in the pores of CF, providing a more efficient and structured framework for the material. The as-prepared CFLZ composite anodes are systematically investigated to emphasize the roles of the tunable lithiophilicity and hierarchical structure of the frameworks. Meanwhile, a thin layer of Cu-Zn alloy with strong lithiophilicity covers the CF scaffold itself. The CFLZ with high Zn content facilitates uniform Li nucleation and deposition, thereby effectively suppressing Li dendrite growth and volume fluctuation. Consequently, the hierarchical and lithiophilic framework shows low Li nucleation overpotential and highly stable Coulombic efficiency (CE) for 200 cycles in conventional carbonate based electrolyte. The full cell coupled with LiFePO4 (LFP) cathode demonstrates high cycle stability and rate performance. This work provides valuable insights into the design of advanced dendrite-free 3D LMA toward practical application.

The low-tortuosity microchannels of wood-based carbon matrix in free-standing cathodes for lithium sulfur batteries (LSBs) were a double-edged sword, which brought in both a high energy density due to a high sulfur loading and severe shuttle effect for poor cycling stability. Herein, a layer of cellulose aerogel extracted from the wood wall was coated on the inner surface of the low-tortuosity microchannels of the wood plate, which was further transformed into a hierarchical carbon matrix using in free-standing cathode for LSBs. The decorated cathode exhibited a maximal specific capacity of 1377.2 mAh g−1 due to the enhanced utilizing ratio of active materials and exceptional cycling stability even under a high current density (1 C) for more than 500 cycles. Furthermore, the decorated cathode maintained good cycling stability with a higher sulfur areal loading (6.3 mg cm−2). The cellulose-based carbon aerogel coated on the inner surface of low-tortuosity microchannels provided a large specific surface area. This decoration strategy not only provided physical restriction on polysulfides but also increased conversion sites for polysulfides, improving the cycling performance of the wood-based free-standing cathode of LSBs. This work provided a potential structural design strategy for the advanced free-standing cathode of LSBs.

The graphite-based hybrid Li-ion/metal anode holds great promise to be one of the ultimate anode choices, owing to its high specific capacity (often up to 500 mAh/g), obviously superior to 372 mAh/g of the commercial graphite anode. Unfortunately, Li deposition on the top surface of the conductive graphite host can easily drive Li dendrite growth, dead Li accumulation, and the blockage of Li+ transport pathways, leading to low host space utilization and cycling stability deterioration. Herein, a graphite host with lithiophilicity and reactive activity dual-gradient is constructed by integrating a surface insulation passivation and a bottom lithiophilicity modification to realize the "bottom-up" deposition behavior for hybrid Li-ion/metal anode. The conformal coating layer of electrical insulating and lithiophobic polymer can efficiently retard Li+ reduction and deposition on the top surface of the conductive host, while the decorated Ag nanoparticles with high lithiophilicity on the host bottom enable much lower Li nucleation barrier, thereby guiding the preferential bottom-up Li deposition. Li dendrite growth is effectively inhibited and the synergistic effects realize high space utilization of the host. Consequently, the hybrid graphite-Li anodes with 600 mAh/g of lithiation capacity (similar to 3.0 mAh cm(-2)) deliver significantly improved cycling stability over 500 cycles with a negligible capacity fading rate of 0.05 % per cycle at 1 C in LiFePO4-based full-cells (N/P ratio = 1.9).

Much attention has been paid to lithium sulfur battery due to its high energy density. However, low S loading and poor cycling stability have hindered their commercialization. In this work, a porous carbon film with rich heteroatom doping was prepared from the Penicillium chrysogenum hyphae film by freezing drying and high-temperature carbonization. Then the carbon film loaded polysulfide solution was utilized as a self-supporting cathode for Li-S batteries. The self-supporting cathode exhibited good rate performance (513.1 mAh/g at 1C) and improved cycling stability (more than 400 cycles) under a high current density (0.5C). This is mainly attributed to the abundant heteroatoms that provided active sites with superior adsorption ability for lithium polysulfide, which not only enhanced the cycling stability but also facilitated the conversion kinetics. Besides, the fibrous network morphology with affluent porous structures inherited from hyphae provided a large specific surface area and sufficient space for accommodating active substances. This work shows the great potential of hyphae derived porous carbon electrodes for high-performance energy storage applications.

Constructing suitable anode materials with high specific capacity, cyclic performance as well as low-cost have been mainly restricted by the large K+radius for inorganic counterparts in potassium-ion batteries recently. Herein, the potassium storage performance and reaction mechanism of temperature-depended organic iron terephthalate (FeC8H4O4) were comparatively investigated in difluoro-sulfonimide potassium (KFSI)-based ester and ether electrolytes. The as-prepared FeC8H4O4-250 with rough surface area and larger specific surface area, showed the best electrochemical performance than that of FeC8H4O4-150 and FeC8H4O4. It was disclosed that the potassium storage mechanism of FeC8H4O4-250 is based on the reversible enolation reaction of carbonyl and the conversion of Fe2+ into Fe nanoparticles, consequently resulting in high specific capacity. In addition, the results suggest that FeC8H4O4-250 exhibits better cycling stability in KFSI/DME electrolyte than in KFSI/ EC+DEC, which is mainly because the salts and solvents in KFSI/EC+DEC contribute to the formation of a stable and robust SEI that inhibits the decomposition of the electrolyte. Our work is of significant to explore highperformance electrode materials for next-generation energy storage systems.

Poly(ethylene oxide) polymer electrolyte composited with high content of succinonitrile organic plasticizer has excellent ionic conductivity at room temperature. Unfortunately, the poor interface stability between this novel solid polymer electrolyte (SPE) and Li metal anode leads to limited cycling performance, which seriously hinders its commercial applications. Herein, the electrospun nanofibers framework of polyacrynitrile (PAN) is introduced as a three-dimensional polymer filler, which can not only provide a robust skeleton for improved mechanical stability, but also inhibit the growth of Li dendrites with increased Li ion transference number from 0.28 to 0.41. Meanwhile, the Li anode is modified via constructing a dense Li-Sn alloy layer, offering a perfectly passivated anode surface and eliminating the side reaction between metallic Li and SPE efficiently. Hence, the interface compatibility and structure stability between the anode and the polymer electrolyte are greatly improved in the prolongated cyclic testing due to the synergistic effect of PAN reinforced SPE and Li-Sn alloy layer coated Li. As a result, the symmetrical battery can cycle stably for 2400 h at 25 degrees C under 0.1 mA cm-2 and 0.1 mAh cm-2, while the LiFePO4 based full battery can keep a good capacity retention of 85 % even after 500 cycles at 0.5 C. This work demonstrates that the combination of modifying SPE and building advanced interface layer on the Li anode is an effective measure to optimize the room temperature cycling performance of polymer solid-state Li battery.

Herein, we report a self-supporting and flexible K2TP/MWNCTs/C anode material prepared by electrostatic spinning and controlled medium temperature heat treatment in potassium-ion batteries. The results show that the flexible carbon cladding and stably conductive network structure can facilitate the transport of K+ and electron. The as-synthesized K2TP/MWNCTs/C flexible anode can exhibit a high specific capacity of 150.6 mAh g(-1) after 100 cycles at a current density of 50 mA g(-1). These results are of significant to explore highperformance organic flexible devices.

Li-rich dual-phase Li-Cu alloy is a promising candidate toward practical application of Li metal anode due to its in situ formed unique three-dimensional (3D) skeleton of electrochemical inert LiCux solid-solution phase. Since a thin layer of metallic Li phase appears on the surface of as-prepared Li-Cu alloy, the LiCux framework cannot regulate Li deposition efficiently in the first Li plating process. Herein, a lithiophilic LiC6 headspace is capped on the upper surface of the Li-Cu alloy, which can not only offer free space to accommodate Li deposition and maintain dimensional stability of the anode, but also provide abundant lithiophilic sites and guide Li deposition effectively. This unique bilayer architecture is fabricated via a facile thermal infiltration method, where the Li-Cu alloy layer with an ultrathin thickness around 40 μm occupies the bottom of a carbon paper (CP) sheet, and the upper part of this 3D porous framework is reserved as the headspace for Li storage. Notably, the molten Li can quickly convert these carbon fibers of the CP into lithiophilic LiC6 fibers while the CP is touched with the liquid Li. The synergetic effect between the LiC6 fibers framework and LiCux nanowires scaffold can ensure a uniform local electric field and stable Li metal deposition during cycling. As a consequence, the CP capped ultrathin Li-Cu alloy anode demonstrates excellent cycling stability and rate capability.

Abstract Lithium-sulfur batteries, as a promising electrochemical energy storage device, are impeded by sluggish reaction kinetics and poor cycle life under high sulfur loading. Herein, a natural wood disc derived carbon matrix with anisotropic and aligned microchannels decorated with carbonized cellulose aerogel was proposed to serve as a host for self-supporting sulfur/carbon composite cathodes (S/DBWC/CCA) in Li-S batteries. The obtained cathodes were capable of high sulfur areal loading (3.1 and 6.3 mg cm-2). Furthermore, exceptional cycling stabilities were achieved not only under a high current density (1 C) but also under a high sulfur areal loading of 6.3 mg cm-2. The improved performance is attributed to the synergistic effect of the ordered microchannels with low tortuosity and 3D conductive network of carbonized cellulose aerogel. This work provides an ideal host derived from natural resources for viable Li-S batteries with excellent cycling stability, which is a potential strategy for structural design of advanced energy storage devices.

The seriously dissolution of the intermediate into the organic electrolyte has been the key limitation for metal-organic compounds in K-ion batteries. Here, we initially inhibit the dissolution of intermediate products (TCNQ0) with a highly conducting polymer (polypyrrole, PPy) coated on the CuTCNQ. And the adsorption energy between the conductive polymer PPy and the intermediate product TCNQ can be significantly enhanced (-0.55 eV) as compared to the TCNQ molecules (0.21 eV), which can restrain the free intermediate product dissolved in the organic electrolyte, resulting in an enhanced cyclic stability as well as rate performance. Additionally, the highly conductive PPy exhibits flexible structure, which can weaken the interface effect between the electrode and the coating layer. This work provides further understanding on surface coating on metal-organic compounds and has significant basic scientific sense for the in-depth research of K-ion batteries.

Developing suitable electrode materials with high flexibility, superior cyclic performance and low-cost have been the new topic and difficulty in the up-coming wearable flexible device. Herein, organic potassium terephthalate (K2TP) with MWCNTs and conductive polymer PEDOT:PSS co-coated K2TP/2MWCNTs/PP composite endowing continuous conductive network, was initially developed as a pliable and free-standing anode material for potassium ion batteries. By analyzing the internal microstructure, external topography and varies electrochemical characterization of the prepared samples, the incorporation of reasonable MWCNTs and PEDOT:PSS allows for the construction of a continuous conductive network with a large specific surface area, the creation of an effective electron transfer channel, an improvement in the kinetics of K+ diffusion and the maintenance of structural integrality. A preeminent specific capacity of 154.3 mAh g+1 can be maintained after 100 cycles at the current density of 50 mA g+1, prevailing over the majority of claimed anode materials employed in K-ion batteries. Furthermore, a high-performance all-organic full battery based on flexible anode and cathode material was successfully assembled delivering an extraordinary energy density of 320 Wh Kg-1. These results can put forward the practical application of organic electrode materials in systems for massive-scale energy storage.

Many kinds of nanostructured metal oxides were introduced in cathodes of Li-S batteries for high sulfur utilization and effective confinement for polysulfides. Herein, Gd2O3 nanoparticles modified wave-like carbon host, which are derived from soybean residue by activation and pyrolysis processes. After the activated soybean residue derived carbon (ASC) host modified by Gd2O3 nanoparticles, the ASC-Gd was integrated with sulfur by melting method and then used as cathode in lithium-sulfur (Li-S) batteries. According to the electrochemical results of ASC-Gd/S cathode, a high initial discharge capacity (1343 mAh g(-1) at 0.1 C) and improved cycling stability were exhibited, which was attributed to the strong adsorption ability for polysulfides and ultrahigh specific surface area of the ASC. As a result, the Gd2O3 nanoparticles modified wave-like biomass carbon was a promising host material of Li-S batteries with high performances.

AbstractDue to large sulfur (S) content and simple manufacturing techniques, free‐standing cathodes for lithium‐sulfur (Li−S) batteries are gaining a lot of attention recently. Waste office paper, which is consumed in large quantities annually, was used to make a free‐standing paper‐based carbon (FPC) substrate, which inherited fiber‐like morphology. In addition, reduced graphene oxide (rGO) nanosheets modified FPC (rGO@FPC) host was also prepared by a vacuum filtration method. After S impregnation, the FPC/S and rGO@FPC/S free‐standing cathodes were employed in Li−S batteries. The rGO@FPC/S free‐standing cathode exhibited extremely competitive electrochemical performance, including a reversible discharge capacity of 315 mAh g−1 at 0.5 C after 500 cycles. This is due to the uniform S distribution, which boosts the utilization ratio, and the significant blocking action for polysulfide ions, which prevents the redox shuttle effect.

Layered vanadium-based metal oxides were regarded as promising cathode materials accounting for suitable K+ transport channels as well as high work potential in K-ion batteries. Nevertheless, because of the large radius of K+ and the rigid structure of inorganic materials, the typical K0.486V2O5 suffers from volume expansion seriously in the repeated charging and discharging processes along with poor ionic and electronic conductivity, consequently determining inevitably poor electrochemical properties. Herein, we proposed a stabilized polymer (PAN) matrix on K0.486V2O5 nanobelts by a liquid-assisted methodology and further electrospinning technology. As a result, a nanocomposite containing a 3D conductive and interconnected mesh structure was thus constructed. By avoiding the full carbonization of polyacrylonitrile (PAN) with appropriate thermal treatment, the elastic properties of the PAN precursor can be retained, effectively inhibiting the volume effect, and the stabilized PAN-encapsulated matrix can also greatly accelerate transport rates of K+ and electrons at a high rate as well as restrict the decomposition of organic electrolytes and side reactions. This work can supply significant basic scientific value of the polymer surface coating methodology for the far-reaching development of inorganic cathode materials in K-ion batteries.

Biomass carbon materials with high theoretical specific capacity, low cost and pollution-free, play an essential role in secondary batteries as anode materials or modified substrates. This review classifies biomass based on its resource and composition and introduces the application of biomass raw fibers, biomass extracts, biomass synthetic fibers, and other materials in lithium-sulfur, potassium-ion, sodium-ion and lithium-ion batteries. It provides a systematic review of the processing methods of different forms of biomass materials. Additionally, the perspectives are also proposed for next-generation biomass carbon materials-based ion batteries.

Exploration of suitable electrode hosts with large open channels that can reversibly accommodate K. with large radius have been extensively investigated. Nevertheless, the reported inorganic counterparts were inevitably restricted by the difficulty of large K. diffusion capability in crystal structure and the huge volume change. Herein, we report a bifunctional vanadium-based metal-organic framework (MIL-47) with double active centers and larger lamellar spacing that could serve as both cathode and anode material, respectively by controlling the redox potential range in potassium-ion batteries. The results suggest that the stable K-storage mechanism is the reversible rearrangement of the conjugated carboxyl groups of organic terephthalic acid into enolate and the reversible redox activity of V ions, with the specific capacity of 272 mAh g(-1) (0.01-1.5 V) and 50 mAh g(-1) (1.5-3.8 V) at the current density of 10 mA g(-1) for MIL-47 anode and MIL-47 cathode, respectively. The unsaturated functional group of MIL-47 and the intermediate bridged V atom not only provide multi-dimensional channels for electron and ion transport but also stabilize its crystal structure. Additionally, a symmetric full-cell in potassium-ion batteries based on MIL-47 was constructed successfully by avoiding the utilization of K metal with safety concerns. Our results provide new insight into structure design for next-generation large-scale energy storage applications. (C) 2022 Elsevier Inc. All rights reserved.

Solid-state lithium metal batteries have emerged as promising energy storage systems due to large energy storage density and low-risk safety hazard.However, high-interface resistance between the garnet-based electrolyte and Li metal anode is one of the major challenges for all-solid-state batteries.Herein, a straightforward modification method is reported, rather than relying on hot pressing under an inert atmosphere or high-cost fabrication techniques to produce metastable nanocoating on garnet electrolyte surface.Fresh Li metal/cobalt-modified solid-state electrolyte/Li metal batteries are placed at room temperature for 48 hours under a tiny pressure of 1 MPa, however the interfacial resistance between the garnet and Li metal reduces from 5,800 -8,200 Ω cm 2 to only 162 Ω cm 2 .At a current density up to 1.6 mA cm -2 , the symmetrical batteries exhibit a stable signal voltage of about 190 mV.The maximum voltage fluctuation is less than 7 mV for the batteries during 160 Li-striping/plating cycles at 0.25 mA cm -2 .Excellent electrochemical performance and easy-to-industrial modification method are beneficial for the commercialization of Li metal all-solid-state batteries.