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Small · 2024 ·Vol. 20 ·期 36 ·2401497 · IF 13

Zero Voltage-Degradation of Li2MnO3 with Ultrathin Amorphous Li─Mn─O Coating

Shiqi Liu,Jie Wan,Boya Wang,Chenghan Li,Yulong Wang,Lin Wang,Haipeng Wu,Nian Zhang,Xu Zhang,Haijun Yu

Manganese-based lithium-rich layered oxides (Mn-LLOs) are promising candidate cathode materials for lithium-ion batteries, however, the severe voltage decay during cycling is the most concern for their practical applications. Herein, an Mn-based composite nanostructure constructed Li 2 MnO 3 (LMO@Li 2 MnO 3 ) is developed via an ultrathin amorphous functional oxide Li x MnO y coating at the grain surface. Due to the thin and universal LMO amorphous surface layer etched from the lithiation process by the high-concentration alkaline solution, the structural and interfacial stability of Li 2 MnO 3 are enhanced apparently, showing the significantly improved voltage maintenance, cycle stability, and energy density. In particular, the LMO@Li 2 MnO 3 cathode exhibits zero voltage decay over 200 cycles. Combining with ex situ spectroscopic and microscopic techniques, the Mn 2+/4+ coexisted behavior of the amorphous LMO is revealed, which enables the stable electrochemistry of Li 2 MnO 3 . This work provides new possible routes for suppressing the voltage decay of Mn-LLOs by modifying with the composite functional unit construction.

研究领域: 材料科学 · 电化学 · 储能 · 锂离子电池 · 纳米材料
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ACS Applied Materials & Interfaces · 2017 · IF 7.504

Prelithiation Activates Fe2(MoO4)3 Cathode for Rechargeable Hybrid Mg2+/Li+ Batteries

Nan Wang,Hancheng Yuan,Yanna NuLi,Jun Yang,Jiulin Wang

The development of rechargeable Mg-based batteries with a high energy density is restricted by the high-voltage cathodes and the parasitic side reactions between the battery components and electrolytes operating at relatively high potentials. Here, we develop a hybrid Mg2+/Li+ cell using a monoclinic or orthorhombic Fe2(MoO4)3 cathode, a Mg anode, and a simple (PhMgCl)2–AlCl3 + LiCl electrolyte. Hastelloy-C alloy is proposed as a current collector of high-voltage cathode for the hybrid Mg2+/Li+ battery within a Swagelok-type cell. The application of the Hastelloy-C alloy current collector breaks the crucial bottleneck of incompatibility between the currently available current collectors and electrolytes. The hybrid cell features a low voltage polarization between the discharge and charge profiles, which is in favor of practical applications. On the other hand, because all Li+ ions are supplied by the electrolyte in a hybrid Mg2+/Li+ battery, a high Li+ concentration is required to operate at high capacities for the hybrid battery. We further show the first-hand evidence about the compensation of Li+ ions by simply soaking the cathode in the hybrid electrolyte. The prelithiation of Li+ ions into monoclinic Fe2(MoO4)3 significantly enhances the cycling stability and reversibility.

研究领域: 材料科学 · 电化学 · 能源存储 · 无机化学 · 电池技术
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ACS Applied Energy Materials · 2020 · IF 4.473

Enabling Solid-State Li Metal Batteries by In Situ Forming Ionogel Interlayers

Yanke Lin,Ke Liu,Maochun Wu,Chen Zhao,Tianshou Zhao

The pressing need for advanced energy storage devices with high energy density and safety is leading research to solid-state Li metal batteries (SSLMBs). However, the advancement of this type of battery is impeded by the incompatibility and the inferior interfacial contact between solid-state electrolytes and electrodes. In this work, the issues are addressed by introducing the PEGDA/Pyr13TFSI ionogel into the interfaces between a NASICON-type Li1.3Al0.3Ti1.7(PO4)3 (LATP) solid electrolyte and the electrodes via a simple drop-coating and in situ polymerization method. It is demonstrated that the formed robust and elastic ionogel interlayers not only preclude the adverse reactions between the LATP pellet and the Li metal anode but also significantly reduce the interfacial resistances. As a result, the cycling life of the Li/Li symmetric cell with the ionogel interlayers reaches up to 300 h, whereas the cell using the bare LATP dies after only 10 h. More notably, the Li/ionogel/LATP/ionogel/LiFePO4 full battery delivers a high capacity of 152.5 mAh g–1 at 0.5 C at 60 °C with a retention of 91.5% after 200 cycles, in a sharp contrast to the value of as low as 46 mAh g–1 even at 0.1 C given by the Li/ionogel/LATP/LiFePO4 cell. These encouraging results demonstrate that the interfacial modification strategy proposed in this work is effective in constructing stable, compact, and durable interfaces between solid electrolytes and electrodes, thereby paving the way for high-performance SSLMBs.

研究领域: 电化学 · 材料科学 · 能源存储 · 固态电池 · 界面工程 · 高分子化学
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JOURNAL OF CATALYSIS · 2026 · IF 6

Forming interfacial Li-Ni-Fe hydride enables room-temperature alkyne semi-hydrogenation

Qiongyu Wang,Ziheng Zhang,Xilun Zhang,Hua Xie,Ling Jiang,Fei Chang

Catalytic alkyne semi-hydrogenation is a pivotal industrial transformation currently constrained by the limitations of existing heterogeneous catalysts: precious metals (e.g., Pd) face high costs, while non-precious alternatives (e.g., Ni, Cu, Fe) generally require harsh reaction conditions (100–200 °C, 10–40 bar H 2 ). To address these persistent challenges, we propose a novel strategy integrating alkali metal hydrides, serving simultaneously as hydrogen donors and anionic “ligands” into transition metal systems. Herein, we report a NiFe-LiH composite catalyst that enables efficient and highly selective liquid-phase semi-hydrogenation of alkynes—including aliphatic, aromatic, and heteroatom-substituted substrates under very mild conditions (25 °C, ≤3 bar H 2 ). Mechanistic investigations reveal that reactive hydride species (H − ) are integral to the hydrogenation catalysis. Critically, the formation of unique Li-Ni-Fe-H interfacial species facilitate synergistic interactions wherein anionic hydrides coordinate with transition metals, modulating their electronic states to simultaneously enhance catalytic activity and selectivity. This work demonstrates room-temperature activation and transformation of alkynes enabled by a catalytic Li-Ni-Fe-H system, offering a promising new pathway for developing efficient non-noble metal catalysts for selective hydrogenation reactions.

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CHEMICAL ENGINEERING JOURNAL · 2026 · IF 12.5

Continuous microdroplet countercurrent extraction for lithium recovery from high Mg/Li brines

Rujie Li,Yangyang Wang,Yi Jing,Shanxu Han,Xinyu Gao,Yajuan Liu,Chencan Du,Zhiyong Zhou

Lithium's critical role in energy storage drives demand for efficient recovery from high Mg/Li mass ratio brines. Traditional liquid-liquid extraction techniques face limitations in mass transfer and operational performance. In this study, we propose a continuous countercurrent microdroplet-based extractor integrating a T-junction microdisperser with a millimeter-scale column, utilizing a TCPP/NaBPh 4 /2-octanone system for selective Li + recovery. Systematic investigation of microdroplet dynamics revealed stabilized diameters of 145 μm (with a 20% column holdup) during extraction and 160 μm (with a 25% column holdup) during stripping. Optimized operation achieved >99% Li extraction and > 95% stripping efficiency, while reducing Mg/Li mass ratio from 274 to 0.44 in the organic phase. Remarkably, within a column height of 25 cm, the number of theoretical stages achieved for the extraction and stripping were 2.13 and 2.29, respectively. The volumetric mass transfer coefficient reached 0.119 s −1 , representing an improvement of one to two orders of magnitude compared to conventional devices. This microreactor approach demonstrates that precise microdroplet size control enhances mass transfer intensification, offering an efficient solution for strategic lithium recovery from high Mg/Li brines.

CAS / MDL: 111-13-7 115-96-8
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DESALINATION · 2025 · IF 9.8

Dual-phase anion engineering for boosting lithium capture by Li/Al-LDHs

Yujiao Cao,Chenghao Qiu,Jipeng Li,Jun Chen,Jianguo Yu,Sen Lin

Lithium aluminum layered double hydroxides (Li/Al-LDHs), the most widely industrialized lithium adsorbents dependent on the unique acid-free desorption, while exhibited limited capacity in low-salinity systems. Herein, an anion regulation strategy was developed to enhance Li + extraction by introducing and controlling multivalent anions. Experiments confirmed Li + adsorption capacity of Li/Al-LDHs could increase from 0.40 mg/g to 5.83 mg/g by introducing SO 4 2− in a chloride solution containing 2 g/L Mg 2+ . It was well explained by density functional theory (DFT) calculations that the highly charged anions in solution would induce higher ionic strength and adsorption energy to enhance Li + extraction of Li/Al-LDHs. Furthermore, an interlayer repair method effectively replaced accumulated divalent anions within the interlayers using easily elutable Cl − ions, facilitating Li + release from the laminates and ensuring cycling stability. Besides, multiple cycles remaining stable enhanced capacities further confirmed the sustained effectiveness of this strategy for boosting Li + capture from low-salinity systems.

CAS / MDL: 9002-86-2
研究领域: 材料科学 · 环境工程 · 无机化学 · 储能
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AICHE JOURNAL · 2025 · IF 4

Ultrathin nanofiltration membrane based on MXene interlayer for efficient Li+/Mg2+ separation

Zhengyi Huang,Mengmeng Jia,Yanna Wu,Haojie Chen,Shuming Li,Zong Lu,Yanying Wei,Haihui Wang

Nanofiltration (NF) membranes with sub-nano structure are promising for the extraction of lithium from brine resources, yet often face a trade-off between separation efficiency and permeation rate. Here, the ultrathin nanocomposite membranes (TFN AM ) with high Li + /Mg 2+ selectivity and permeability are prepared by introducing the positive aminated-MXene interlayer in the process of interfacial polymerization (IP). This interlayer modulates the diffusion behavior of amine monomers and reduces the thickness of the polyamide (PA) layer by six times; meantime, it provides excellent positive charge on the membrane surface. The aminated-MXene interlayer endows the high positive charge density of TFN AM enhancing the Donnan exclusion effect on the improvement of Li + /Mg 2+ selectivity. As a result, the TFN AM exhibits a high permeability of 12.5 L m −2 h −1 bar −1 and a Li + /Mg 2+ selectivity of 17.5, while maintaining performance over 100 h. This work proposes a facile and effective strategy to address the challenge of NF membrane limitations and advance lithium recovery technologies from brines.

CAS / MDL: 2370-88-9 7789-24-4
研究领域: 材料科学 · 膜技术 · 分离科学 · 纳米技术 · 可持续能源资源
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CHEMISTRY-A EUROPEAN JOURNAL · 2019 ·Vol. 25 ·期 12 ·3112-3118 · IF 5.16

FeOOH Nanocubes Anchored on Carbon Ribbons for Use in Li/O2 Batteries

Zhipeng Lin,Hao Zhang,Guofeng Liang,Yanqi Jin,Hongbin Zeng,Jiawang Li,Jian Chen,Weihong Zhang,Fangyan Xie,Yanshuo Jin,Hui Meng

Graphical Composite nanostructured cathode : FeOOH nanocubes with a core–shell structure and anchored on carbon ribbons have been prepared. The carbon ribbons improve the conductivity of the system and make more of the FeOOH surface available for electrochemical reaction. An Li/O 2 battery with FeOOH as the cathode material shows a specific capacity of 14816 mAh g −1 cathode and a long-term stability of 67 cycles over 400 h (see figure). A composite of FeOOH nanocubes anchored on carbon ribbons has been synthesized and used as a cathode material for Li/O 2 batteries. Fe 2+ ion-exchanged resin serves as a precursor for both FeOOH nanocubes and carbon ribbons, which are formed simultaneously. The as-prepared FeOOH cubes are proposed to have a core–shell structure, with FeOOH as the shell and Prussian blue as the core, based on information from XPS, TEM, and EDS mapping. As a cathode material for Li/O 2 batteries, FeOOH delivers a specific capacity of 14816 mA h g −1 cathode with a cycling stability of 67 cycles over 400 h. The high performance is related to the low overpotential of the oxygen reduction/evolution reaction on FeOOH. The cube structure, the supporting carbon ribbons, and the -OOH moieties all contribute to the low overpotential. The discharge product Li 2 O 2 can be efficiently decomposed in the FeOOH cathode after a charging process, leading to higher cycling stability. Its high activity and stability make FeOOH a good candidate for use in non-aqueous Li/O 2 batteries.

研究领域: 材料科学 · 能源存储与转换
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ACS Sustainable Chemistry & Engineering · 2025 · IF 7.3

Enhanced Li-Ion Transport in Ceramic/Polymer Electrolytes via Interfacial Molecular Bridging

Lin Lin,Wei Han,Guang Li,Jingjing Zhang

The widespread adoption of composite solid electrolytes (CSEs) in solid-state lithium metal batteries has been significantly impeded by insufficient room-temperature ionic conductivity, primarily due to high energy barriers for Li-ion transport across ceramic/polymer interfaces. While interfacial modification has emerged as a key strategy, the structural and mechanistic principles governing efficient ion transport remain poorly understood. Here, we address this challenge through an innovative interface engineering approach, constructing a molecular bridge between Li7La3Zr2O12 nanofibers (LLZO NFs) and poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) using a 3-(methacryloyloxy)propyltrimethoxysilane (MPS) linker. This design achieves multiple synergistic effects: (1) robust chemical bonding enables uniform dispersion of ceramic nanofibers even at high loadings (60 wt %); (2) polar MPS moieties effectively adsorb and reorganize solvated species at the ceramic/polymer interface; and (3) optimized Li+ coordination via dual bonding configurations (Li···O═C with MPS and Li···F–C with PVDF-HFP) drastically reduces the interfacial energy barrier (−0.456 eV), creating continuous ion transport highways across the interface. Systematic investigation of the linker’s structure–property relationship reveals key design principles for interfacial chemistry. The resulting composite electrolyte (CLPH–OH) with 60 wt % of functionalized LLZO NFs delivers an exceptional ionic conductivity of 8.3 × 10–4 S cm–1 at room temperature. Remarkably, Li//CLPH–OH//Li symmetric cells achieve stable cycling for 2000 h at 0.1 mA cm–2, and LiFePO4 full cells retain 93.6% capacity after 300 cycles at 0.5 C. This study provides both fundamental insights into interfacial ion transport mechanisms and a strategy for designing high-performance solid-state electrolytes through precise molecular-level interface engineering.

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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2025 · IF 14.3

Highly compressible garnet thin films for high-energy-density Li metal batteries

Xianzhun Huang,Haojie Liu,Wenyi Xiang,Lihan Chen,Xinran Li,Bangzhuang Xue,Jian Ma,Yueyue Wu,Chengwei Wang,Yinhua Bao,Weiwei Ping

Oxide-based electrolytes are promising with high ion conductivity and a wide electrochemical window (0–5 V). However, the brittleness and poor compressibility severely inhibit their application. Here, inspired by the “flexible eggshell membrane”, we fabricated a 20 µm, flexible and compressible Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 thin film by in-situ healing the LLZTO crystal chips with poly(di(ethylene glycol) ethyl ether acrylate) electrolytes. Fracture mechanics analysis demonstrates the superior mechanical properties of the flexible LLZTO films. With the package pressure increasing from 0.6 to 1.4 t, the Li metal symmetric cell displays a decreasing internal resistance from ∼281 to ∼156 Ω cm 2 , corresponding to the low limit of ion conductivity from ∼0.6 × 10 −4 to ∼2.1 × 10 −4 S/cm. The symmetric cell can be a stable cycle for ∼220 h at 0.4 mA/cm 2 and ∼300 h at 0.1 mA/cm 2 with a bending angle of 30°. The full cell LiFePO 4 /LLZTO/Li shows a superior rate performance of 150 mA/g and a long cycle life of ∼200 cycles. Pairing with the LiNi 0.8 Co 0.1 Mn 0.1 O 2 , the cell displays a Coulombic efficiency of ∼99.7 % for ∼150 cycles. These results indicate that we have successfully fabricated flexible and compressible LLZTO films, and this will open an avenue for the application of high-energy-density thin film batteries.

CAS / MDL: 1314-23-4 554-13-2
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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-14 · IF 15.7

γ-Ray irradiated polyacrylamide networks enable high-performance Li||S pouch cells

Zou Zhijuan,Liu Pengfei,Dou Ruiyang,Liu Kaijun,Wang Yunlong,Song Lixian,Tong Liping,Yin Guolu,Kang Wenbin,Cai Wenlong,Zhang Yaping,Chen Hongbing,Song Yingze

Binders are essential for maintaining positive electrode integrity in Li||S batteries and significantly affect their performance. However, commercial linear binders often have disordered networks, poor binding efficiency, and insufficient mechanical strength. To address these challenges, three-dimensional covalent binders offer a promising solution. Traditional methods for producing cross-linked binders require additives and result in poorly controlled polymer networks due to the stochastic nature of liquid-phase polymerization. Moreover, the mechanisms by which reticulated binders stabilize the positive electrode remain unclear, requiring investigation under operando conditions. Herein, we present an approach to tailor cross-linked polyacrylamide networks using solid-state operando γ-ray irradiation chemistry, which eliminates additives and produces a pure, ordered network with remarkable binding capabilities. By integrating in situ high-resolution optical frequency domain reflectometry, multiscale synchrotron radiation characterization, and virtual simulations, this study reveals the role of binders in dynamically encaging and confining sulfur. Specifically, γ-ray-enabled polyacrylamide networks enhance battery performance through mechanical strengthening, optimized sulfur regeneration, and improved re-occupancy. Consequently, the well-designed composite positive electrode structure with only 5.0 wt% binder improves soft-packaged Li||S battery performance across various scenarios. Notably, a 1.2-Ah pouch cell achieves 410.1 Wh kg −1 specific energy with a low electrolyte/sulfur ratio of 3.0 µL mg –1 .

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Functional Materials Letters · 2025 · IF 1.1

Porous CuF2 derived from MOFs as cathode materials for Li-ion batteries

Hanchen Xu,Zhiyong Yu,Lujia Tian,Suni Du,Yichun Zhao,Jingsai Cheng,Hanxing Liu,Zhongzhi Yuan

Copper fluoride (CuF 2 ) has demonstrated great potential as a cathode material for LIBs owing to its high energy density. In this study, a two-step synthesis method was proposed to prepare porous CuF 2 by using Cu-based metal-organic frameworks (MOFs). N 2 adsorption-desorption isotherms, along with SEM and TEM analyses, proved that the intermediates CuO exerted a certain influence on the pore structure of the final CuF 2 products. The porous CuF 2 achieved a first discharge capacity of 554 mAh ⋅ g − 1 at 0.1C. At a high current density of 5C, it delivered a rate capacity of 413 mAh ⋅ g − 1 within 1.5–4.2 V. The results of electrochemical impedance spectroscopy show that varying degrees of porosity influence the lithium-ion diffusion coefficient, leading to differences in electrochemical performances.

研究领域: 材料科学 · 电化学 · 储能
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