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Materials Today Communications · 2025 · IF 4.5

Tri-additive PEGDA-based quasi-solid electrolyte for enhanced ion transport and interface stability in Li-O2 batteries

Jiaqi Wang,Xiqiang Huang,Xingbao Zhu,Yuanguo Wu,Zining Man,Xiangyu Wen,Weiting Qi,Xing Tang,Zhe Lü

Despite their potential to enhance safety and design flexibility in next-generation lithium batteries, particularly lithium-oxygen (Li-O 2 ) systems, solid polymer electrolytes (SPEs) face persistent challenges of insufficient ionic conductivity and high interfacial resistance. To address these limitations, we developed a novel PEGDA-based quasi-solid-state electrolytes (QSEs) through in situ polymerization, strategically incorporating three functional additives: cellulose acetate (CA), N-methyl-2-pyrrolidone (NMP), and fluoroethylene carbonate (FEC). The electrolyte design leverages multiple synergistic mechanisms: hydrogen bonding between CA and NMP optimizes microstructural organization for efficient Li⁺ transport pathways; carbonyl groups in NMP coordinate with Li⁺ to facilitate LiTFSI dissociation, while oxygen-rich functional groups in CA provide supplementary Li⁺ coordination sites; FEC is introduced to further improve interfacial stability. This molecular engineering approach achieves an impressive room-temperature ionic conductivity of 8.54 × 10 −4 S cm −1 and a high lithium-ion transference number of 0.78. The QSE demonstrated excellent cycling stability (>900 h) in lithium symmetrical batteries and significantly improved the discharge capacity (12243 mAh g −1 ) and long-term cycling performance (590 h) of Li-O 2 batteries. These results highlight the efficacy of our multi-functional additive strategy in overcoming fundamental limitations in solid electrolytes, offering important insights for the rational design of high-performance energy storage systems.

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Journal of Material Cycles and Waste Management · 2025 · IF 3

Spent lithium-ion battery recycling: investigation into the inhibition and separation between Li(I) and Al(III) ions

Lou Wen-bo,Liu Dong-yan,Zhao Da,Wang Yun,Sun Zi-cheng,Zou Yi,Niu Xiao-wei,Cheng Quan-guo,Li Jian-zhong,Liu Hong-hui

The recovery of NCM (LiNi x Co y Mn 1-x-y O 2 , abbreviated as NCM) cathode materials from retired lithium-ion batteries is a research hotspot in resource recycling field. Nevertheless, due to aluminum impurities mixed in raw materials, Li(I) and Al(III) ions are easy to combine to form water-insoluble LiAlO 2 during reduction, affecting Li(I) ions’ water-leaching efficiency. In this study, the LiAlO 2 formation environment is analyzed. Thermodynamic analysis reveals that there is generally less spontaneity in the reaction of Li (I) ions with aluminum monomers compared to Al 2 O 3 , and the introduction of CO 2 can inhibit Li-Al-O substance production. Li-Al binding experiments show that there is almost no direct reaction between Li 2 CO 3 and aluminum monomers, but under Ar atmosphere, Li 2 CO 3 and Al 2 O 3 can easily lead to Li-Al binding, a kinetic analysis considers that binding is controlled by chemical reaction, with an activation energy of 57.78 kJ/mol, and the activation energy increases to 88.028 kJ/mol with CO 2 atmosphere. Under reduced optimization conditions (reduction temperature: 500 °C, time: 6 h, and m NCM : m Al  = 1: 0.25), the carbonation water-leaching efficiency can reach 95.1% for Li(I) ions and less than 1% for Ni(II), Co(II), Mn(II), and Al(III) ions. Thus, this work offers a theoretical basis for the industrial Li(I) ions’ recovery from aluminum-containing NCM materials.

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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Bioinspired conductive-catalytic network accelerates rate-determining steps at cathode-electrolyte interface for high-loading Li-S batteries

Cai-Yun Zhang,Chen-Yang Wang,En-Zhu Zhao,Guowei Yu,Hui-Ling Deng,Rui Huang,Zhao-Yun Wang,Pu Hu,Min Yan,Zhitian Liu

Lithium‑sulfur batteries demonstrate substantial promises for evolving into next-generation energy storage systems, but sluggish kinetics of LiPSs conversion and poor interfacial stability at the cathode-electrolyte interface remain critical challenges. Biowaste carbon as hosts is a cost-effective strategy to improve the electrical conductivity of Li-S batteries. However, limited polar sites in raw biowaste carbon restrict the capacity to anchor LiPSs. Herein, we propose a bio-derived hybrid host (PANI@GC) synthesized from waste grapefruit peels and polyaniline to address the rate-determining steps in sulfur electrochemistry. The grapefruit-derived carbon establishes an excellent conductive network that enables rapid electron transfer, while the PANI-integrated numerous polar sites (aromatic amine groups, conjugated π-π stacking) create a catalytically active interface to anchor and accelerate LiPSs conversion kinetics. Due to the conductive-catalytic network, the PANI@GC/S cathode delivers exceptional performance of 1190 mAh g −1 at 0.2C and maintains 779.8 mAh g −1 under stringent conditions (5 mg cm −2 sulfur loading, 8 μL mg −1 E/S ratio). Remarkably, the catalytic interface minimizes capacity fading, exhibiting only 28.9 mAh g −1 loss after 7-day rest, compared to Pure S (152.83 mAh g −1 ). This research pioneers a sustainable strategy to engineer conductive-catalytic networks at cathode-electrolyte interfaces, providing fundamental insights into biowaste utilization for high-energy-density battery systems.

CAS / MDL: 7727-54-0 872-50-4
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Interface compatible organic-inorganic solid electrolyte with intimate electrode/electrolyte interfacial contact for dendrite-free Li metal batteries

Hao Feng,Zhenxi Li,Shilun Gao,Youjia Zhang,Ruijie Guo,Peng-Fei Cao,Huabin Yang

The increasing demand for safe, high-energy-density batteries drives the development of solid-state electrolytes. Organic/inorganic hybrid electrolytes, integrating the benefits of polymer and inorganic electrolytes, exhibit flexibility, high mechanical strength, and superior ionic conductivity. However, interfacial incompatibility between organic/inorganic components and high electrolyte/electrode interfacial resistance restricts their practical applications. Herein, a flexible and high ionic conductive organic/inorganic electrolyte is prepared via the simple electrospinning of Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 @polyacrylonitrile (LAGP@PAN) and then in-situ polymerization of vinylene carbonate (VC). The LAGP fillers are homogenously distributed in PAN fibers, contributing to the compatible interface between the polymer matrix and inorganic reinforcement. The in-situ polymerization of VC to poly(vinylene carbonate) (PVCA) further improves the intimate electrolyte/electrode contact. As a result, the LAGP@PAN/PVCA electrolyte exhibits a high ionic conductivity of 2.05 × 10 −4  S cm −1 at 30 °C. The Li|LAGP@PAN/PVCA|Li symmetric cell can stably cycle for over 2300 h. The Li|LAGP@PAN/PVCA|LiFePO 4 cell exhibits excellent cycling performance with a capacity retention of 88 % after 700 cycles at 1C. Even combined with commercial LiFePO 4 cathode and thin Li foil anode (N/ P  = 2), the full cell also shows stable cycling performance. This study presents a promising approach to mitigate interfacial challenges in solid electrolytes, facilitating the development of Li metal with high-safety and high-energy density.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

N-methylpyrrolidone-based electrolyte modulated CF bond weakening and Interface optimization synergistically enhances Li/CFx batteries energy density

Fei Zhou,Jiangmin Jiang,Gaoyu Zhou,Lingbang Qiu,Wenxuan Fu,Chencheng Xu,Yanhua Cui,Quanchao Zhuang

Lithium/fluorinated carbon (Li/CF x ) batteries have garnered substantial interest from researchers due to their superior energy density and low self-discharge characteristics. However, the strong covalent C F bond in the CF x cathode limits its discharge kinetics, affecting the actual power density and operating voltage. In this work, N -methylpyrrolidone (NMP) with high donor number has proposed as the main solvent of the electrolyte to facilitate the breaking of the C F bond through a bimolecular nucleophilic substitution (S N 2) reaction. This strategy effectively reduces the energy barrier for Li + embedding and improves interfacial reaction potential. Notably, NMP forms a nitrogen-rich cathode-electrolyte interface (CEI) membrane during the discharge process, which enhances interfacial ionic conductivity and stabilizes the electrode-electrolyte interface. The optimized electrolyte system achieves a discharge plateau of 2.7 V and an energy density of 2128 Wh kg −1 at 50 mA g −1 , significantly surpassing that of the conventional electrolyte (COE). This study provides a low-cost electrolyte optimization strategy, offering a promising approach to maintaining the high energy density and discharge voltage of Li/CF x batteries.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Selenium-regulated band structure engineering in CFx cathodes enables high-power and wide-temperature Li/CFx primary batteries

Tingting Liu,Zhian Dou,Zhen Li,Yiran Sun,Chunyi Wang,Longchen Li,Hao Yin,Jiwen Li,Xiaozhong Wu,Jinglin Mu,Pengfei Zhou,Jin Zhou

Li/CF x primary batteries are renowned for their exceptional energy density, yet their practical deployment is hindered by the inherently sluggish kinetics of the CF x cathode. This study addresses this limitation by incorporating selenium (Se) into CF x (denoted as CF x /Se) via a facile low-temperature thermal treatment, significantly enhancing its electrochemical performance. Comprehensive spectroscopic and electrochemical analyses reveal that Se doping induces the formation of C Se bonds, which promote semi-ionic C F bonding, thereby accelerating Li + diffusion and reducing charge transfer resistance. Density functional theory calculations further demonstrate that Se doping modulates the electronic structure of CF x , narrowing its bandgap to establish an efficient conductive network and markedly improving electronic conductivity. The optimized CF x /Se-1 composite (Se:CF x  = 1:9) delivers outstanding performance, achieving a discharge capacity of 383.9 mAh g −1 at a high current density of 20 A g −1 with an energy density of 765.7 Wh kg −1 and a power density of 3.99 × 10 4  W kg −1 . Moreover, CF x /Se-1 exhibits remarkable wide-temperature operability (−35 to 60 °C), retaining a capacity of 485.3 mAh g −1 at 0.5 A g −1 with a stable 2.0 V plateau even at −35 °C. This work underscores the pivotal role of Se doping in tailoring the band structure of CF x , unlocking its potential for high-power and extreme-temperature Li/CF x batteries.

CAS / MDL: 7782-49-2
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

A synergistic strategy for efficient Li+/Mg2+ separation based on γ-CD cavity regulation and histidine electrostatic repulsion

Yinghong Wang,Ping Xiong,Wei Yang,Zhitong Zhang,Xiaoling Xu,Liming Yang,Huiji Xiao,Kai Zhang,Zhenzhou Wang,Wei Zhang,Xubiao Luo

Highly selective Mg 2+ /Li + separation membranes hold significant application prospects in extraction of lithium. However, the high Mg 2+ /Li + concentration ratio commonly found in brines and the very close hydrated ionic radii of the two ions limit the separation efficiency of conventional membranes. This study proposes a dual-phase supramolecular synergistic sieving nanofiltration membrane design strategy. Leveraging the unique molecular recognition unit and hydrophilic external interface characteristics of γ -cyclodextrin ( γ -CD), combined with the multifunctional positively charged groups of histidine, the strategy achieves the directional construction of highly efficient Mg 2+ /Li + sieving channels within the membrane. The strategy is accomplished through the synergistic action of γ -CD’s selective capture of high-valent Mg 2 + and histidine’s electrostatic repulsion effect. During the Mg 2 + /Li + separation process, the fabricated γ -CD-histidine composite membrane (HCF membrane) demonstrates outstanding comprehensive performance. It achieves a remarkably high Li + /Mg 2+ separation factor of 28.98 and maintains excellent separation performance across a wide Mg 2+ /Li + ratio range (1:1–100:1). The enhanced hydrophilicity of the HCF membrane significantly boosts permeate flux, while also exhibiting long-term operational stability and biofouling resistance during continuous operation under high Mg 2+ /Li + ratios. This research enables the high-selectivity separation of Mg 2+ and Li + with concurrent Li + enrichment, demonstrating significant potential for lithium extraction from salt-lake.

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Energy & Environmental Materials · 2025 · IF 14.1

Fluorination Engineering for Stable Interfacial Chemistry in Deep Eutectic Amide-Based Electrolytes Enables High-Performance LiNi0.8Co0.1Mn0.1O2/Li Batteries

Yuanxin Gao,Xinyi Wang,Dong Lv,Zhang Zhang,Jiangpeng Li,Xiaoyan Feng,Jingchao Chai,Yun Zheng,Yu Peng,Yanqing Wang,Yingying Wang,Lingyu Zhu,Zhihong Liu

Fluorinated amide electrolytes represent a promising solution for high-energy density lithium metal batteries, yet their application in Ni-rich layered oxide cathodes is hindered by interfacial instability. This study develops a non-flammable fluorinated amide-based deep eutectic electrolyte modified with fluoroethylene carbonate, which simultaneously enhances ionic conductivity (1.5 × 10 −4 S cm −1 ) and anodic stability (>4.4 V vs Li + /Li). Applied in Li/NCM811 batteries, the fluoroethylene carbonate-based electrolyte enables 83.2% capacity retention after 200 cycles at 0.5 C, significantly outperforming conventional counterparts. ToF-SMIS and XPS tests reveal that fluoroethylene carbonate facilitates the formation of a LiF-rich cathode-electrolyte interphase, suppressing parasitic reactions and improving Li + transport kinetics. Furthermore, the electrolyte demonstrates superior lithium metal compatibility, inhibiting dendrite growth while enhancing thermal safety. These findings underscore the critical role of fluorinated amide electrolytes in stabilizing Ni-rich cathodes and highlight their potential for next-generation high-voltage lithium metal batteries.

CAS / MDL: 815-06-5
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY · 2025 · IF 2.6

Fluorination-promoted structural evolution and enhanced electrochemical performance in low Li-excess manganese-based cation-disordered rocksalt cathodes

Yan Yu,Su Minyi,Yu Hengxin,Sun Yining,Chang Qing,Yuan Songdong,Jiang Guodong

Cation-disordered rocksalt (DRX) oxides have emerged as attractive candidates for high-capacity lithium-ion battery cathodes, owing to their flexible compositional tunability and potential to access both cationic and anionic redox. However, practical application is hindered by oxygen redox instability and sluggish Li + transport, especially in highly lithium-excess systems. In this study, we investigate fluorine-substituted Mn-based DRX cathode with low lithium excess (Li 1.1 Mn 0.7+ x Ti 0.2− x O 2−  x F x ), designed to reconcile the trade-off between Li + diffusion and structural stability. Systematic structural and electrochemical analyses reveal that fluorine doping suppresses oxygen redox activity by boosting the redox capacity contribution by increasing the Mn content. Most notably, fluorine substitution promotes phase transformation from disordered rocksalt to spinel-like domains during cycling via enhanced Mn migration, which in turn significantly enhances Li + transport kinetics. The optimized Li 1.1 Mn 0.8 Ti 0.1 O 1.9 F 0.1 cathode delivers a maximum discharge capacity of 228.7 mAh g − ¹ at 0.1 C and retains 115.4 mAh g −1 at 2 C, outperforming its undoped counterpart (Li 1.1 Mn 0.7 Ti 0.2 O 2 : 203.2 mAh g −1 at 0.1 C; 81.0 mAh g −1 at 2 C). These findings provide the dual role of fluorination in structural tuning and redox modulation, offering a new strategy to optimize low lithium-excess DRX systems through controlled fluorination and phase engineering. Graphical

CAS / MDL: 1317-34-6
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2025 · IF 8.3

Research on the influence of Li+ contents on the electrochemical hydrogen storage properties of BaCe1-xLixO3 solid solutions

Zhiyong Yang,Guofang Zhang,Ruiqin Zhang,Lu Bai,Jianyi Xu,Ping Yuan,Lingliang Kong,Jingyi Zhang,Juan Du

The development of nickel-metal hydride battery anodes has long been limited by the inherent capacity decay of the anodes of the metal alloy materials. In this study, the BaCe 1-x Li x O 3 solid solutions with controlled contents of Li +  ions (x = 0–0.8) were synthesized via combustion method and adopted them as the novel negative materials to offer a breakthrough in overcoming traditional performance constraints. The influences of Li + contents on microstructure and electrochemical hydrogen storage performance were systematically investigated. X-ray Diffraction test (XRD) confirmed that the Li +  ions were successfully incorporated into the BaCeO 3 lattice and substituted at the Ce 4+ sites. The grain sizes were gradually decreased from 73.5 nm (undoped) to 67.0 nm (Li 0.08 ). Scanning Electron Microscope (SEM) and Transmission Electron Microscope (TEM) results further supported the reduction of the grain sizes and proved that the Li +  ions had doped into the lattice of the BaCeO 3 . Spectral tests showed that the Li +  ions induced obvious changes in the lattice structures and the concentration of oxygen vacancies. Electrochemical hydrogen storage performance tests demonstrated that the discharge capacity of BaCe 0.96 Li 0.04 O 3 achieved 212.7 mAh/g, representing 95.1 % improvement over the undoped sample (109.0 mAh/g), along with higher charge retention. Kinetic analysis further confirmed the superior hydrogen storage kinetic behavior of the doped samples. These results fully proved that the doping of Li +  ions can effectively enhance the hydrogen storage performances of BaCeO 3 materials.

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ELECTROCHIMICA ACTA · 2025 · IF 5.6

Recovery of Li and Mn by H3PO4-citric acid leaching from spent LiMn2O4 batteries for synthesis of LiMn0.75Fe0.25PO4

Xiaoping Fan,Kui Liu,Chunfeng Sun,Jiasheng Wang,Hongqiang Wang,Youguo Huang,Qingyu Li,Fenghua Zheng,Peng Xi

Although hydrometallurgy is the primary method for recycling spent lithium-ion batteries (LIBs), handling the waste liquid produced during the leaching process remains a challenge due to the additional procedures and costs involved. This study presents an efficient, closed-loop recycling process for spent LiMn 2 O 4 (LMO) batteries. The waste LMO powders were initially leached with H 3 PO 4 and citric acid (CA) to obtain the leachate containing Li + , Mn 2+ , PO 4 3− and citrate ions. The metal ions leached into the solution are complexed by CA, achieving complete leaching of LMO. The H 3 PO 4 and CA provide both PO 4 3− and carbon sources for subsequent product preparation, minimizing resource waste and secondary pollution. The molar ratio of Li:Mn:Fe:PO 4 3− in the leachate was adjusted to 1:0.75:0.25:1, and LiMn 0.75 Fe 0.25 PO 4 (LMFP) with excellent performance was regenerated by spray drying and calcination. The regenerated LMFP-650 exhibited a capacity retention rate of 89.7% after 500 cycles, significantly improving the structural stability and cycling performance of LMO. This green, closed-loop recycling process prevents secondary pollution and promotes the sustainable development of the battery industry.

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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-14 · IF 15.7

P-block element modulated 1 T phase MoS2 with Ru lattice grafting for high-performance Li | |O2 batteries

Wang Peng,Zhao Danyang,Zhang Peng,Hui Xiaobin,Zhang Zhiwei,Wang Rutao,Wang Chengxiang,Ge Xiaoli,Liu Xiaojing,Li Yuguang C.,Yin Longwei

The metallic phase MoS 2 (1T-MoS 2 ) supported metal-nanocatalyst is an appealing material system for accelerating the redox kinetics of non-aqueous Li | |O 2 batteries. However, the drawbacks associated with the surface orbital steric effect and the internal electron coupling results in a detrimental effect for the stability of 1T-MoS 2 , especially for the interface charge transfer. This makes it difficult to incorporate guest metal nanoparticles without compromising the 1 T phase support. To circumvent these issues, here we propose a p-block element (In-O) doping strategy to stabilize the 1 T phase MoS 2 by moderating the surface orbital steric effect and strengthening the internal chemical bonding, and thus for the epitaxial Ru nanocatalyst graft on the stabilized 1T-MoS 2 for Li | |O 2 batteries. The experimental and theoretical analyzes indicate that the In-O-MoS 2 @Ru enhances the O 2 dissociation and facilitates the adsorption of LiO 2 intermediates. This effect promotes the growth of weakly crystalline Li 2 O 2 films during oxygen reduction reaction, which can be more easily decomposed during the oxygen evolution reaction, thereby enhancing the bifunctional-catalytic kinetics. When employed at the positive electrode for non-aqueous Li | |O 2 batteries, In-O-MoS 2 @Ru shows an overpotential of 0.37 V and a cycling life of 284 cycles at 200 mA g −1 with a final discharge specific capacity of 1000 mAh g −1 at 25 °C.

CAS / MDL: 14898-67-0
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