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Science China-Materials · 2022 ·Vol. 65 ·期 11 ·2967-2974 · IF 8.64

Interface engineering by gelling sulfolane for durable and safe Li/LiCoO2 batteries in wide temperature range

Yu Xinrun,Hu Xianluo

Lithium-metal batteries (LMBs) with high energy densities have aroused intensive interest in electrical energy storage devices but suffer from the risk of thermal runaway, especially under harsh conditions of high temperature or thermal abuse. Pursuing intrinsically thermally stable electrolytes with higher performance and higher safety beyond commercial liquid electrolytes is a major challenge in this field. Here we report on a unique, highly durable sulfolane-based gel electrolyte constructed by a facile gelling strategy. This method takes advantages of thermotolerant sulfolane as a plasticizer and strong dipole-dipole interactions to achieve the gelation of polymer polyvinylidene fluoride/polyethylene oxide. We systematically investigated the influence of gelled sulfolane on gel formation, lithium plating/stripping, and solid electrolyte interphase. Benefiting from favorable interface engineering, the sulfolane-based gel electrolyte remarkably enhances the cyclic and safety performances of LMBs. When used in the Li/LiCoO 2 battery, the resulting gel electrolyte enables long-term cycling stability at high temperatures up to 90°C. Moreover, the thermal safety of practical Li/LiCoO 2 pouch cells (up to 190°C) has also been demonstrated by accelerating rate calorimetry. These results contribute to the development of high-safety LMBs that require abuse tolerance, high energy, and long calendar life.

✓ 已验证 DOI 高影响因子
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CERAMICS INTERNATIONAL · 2021 · IF 4.527

Rapid preparation and performances of garnet electrolyte with sintering aids for solid-state Li–S battery

Li Yang,Xiao Huang,Changfei Zou,Xiyuan Tao,Lei Liu,Kaili Luo,Peng Zeng,Qiushi Dai,Yongfang Li,Lingguang Yi,Zhigao Luo,Xianyou Wang

Lithium-sulfur (Li–S) batteries are attractive due to their high theoretical energy density . However, conventional Li–S batteries with liquid electrolytes undergo polysulfide shuttle-effect and lithium dendrite formation during charge/discharge process, leading to poor electrochemical performance and safety issues. Garnet type Li 7 La 3 Zr 2 O 12 (LLZO) solid-state electrolyte (SSE) restricts the penetration of polysulfides and exhibits high ionic conductivity at room temperature (RT). Herein, Li 6.5 La 3 Zr 1.5 Nb 0.5 O 12 (LLZNO) ceramic electrolyte using Li 3 PO 4 (LPO) as sintering aids (LLZNO-LPO) is prepared by the rapid sintering method and is applied to construct a shuttle-effect free solid-state Li–S battery . The SSE displays high conductive pure cubic-LLZO phase; during the rapid sintering, LPO melts and junctions the voids between the grains, thus improves Li + conductivity. As a result, the LLZNO-LPO ceramic electrolyte with Li + conductivity of 4.3 × 10 −4  S cm −1 and high critical current density (CCD) of 1.2 mA cm −2 is obtained at RT. The Li–S solid-state battery which utilizes LLZNO-LPO ceramic electrolyte can deliver an initial discharge capacity of 943 mA h·g −1 and 602 mA h·g −1 retention after 60 cycles. In the same time, the initial coulombic efficiency is as high as 99.5%, indicating that the SSE can effectively block the polysulfide shuttle towards the Li anode and fulfill a shuttle-free Li–S battery.

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ELECTROCHIMICA ACTA · 2019 · IF 5.383

Recovery Li/Co from spent LiCoO2 electrode based on an aqueous dual-ion lithium-air battery

Yu Zhou,Wei Shan,Shaofeng Wang,Kwok-ho Lam,Qiang Ru,Fuming Chen,Xianhua Hou

While lithium-ion batteries dominate the field of electronic devices and vehicles, recovery of LiCoO 2 from spent batteries becomes a significant process. Aqueous lithium-air battery and dual-ion battery were blended into a novel electrochemical system as dual-ion lithium-air battery (DLAB) system to recover Li and Co elements from the spent LiCoO 2 (acid solution). In the system, oxygen, LiCoO 2 acid solution and Li 2 Ti 2 (PO 4 ) 3 (LTPO), which has Na + superionic conductor structure and is synthesized by sol-gel method, were used as cathode, dual-ion electrolyte and anode. Relatively low voltage plateaus, stability and insolubility of LTPO make it to be a feasible candidate for this aqueous DLAB. By applying Pt/C as a catalyst for cathode, the full discharged system exhibits a Co ion recovering rate of up to 96.2%. Moreover, this system presents positive discharge plateaus at around 0.47 V and 0.10 V during recovering, demonstrating an output energy density of 43.88 Wh kg −1 . The system shows a green and promising way for the recovery of spent LiCoO 2 battery.

✓ 已验证 DOI 高影响因子
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Journal of Materials Chemistry A · 2022 ·Vol. 10 ·期 30 ·16152-16162 · IF 14.511

A dual-functional interlayer for Li–S batteries using carbon fiber film cladded electron-deficient Li2B4O7

Xin Dai,Kunyang Zou,Weitao Jing,Peng Xu,Junjie Sun,Shengwu Guo,Qiang Tan,Yongning Liu,Tengfei Zhou,Yuanzhen Chen

The electron-deficient property of the atoms in functional materials endow them with tunable adsorption and catalysis effects on polysulfides, thus improving the performance of lithium–sulfur batteries. In this work, Li2B4O7 nanoparticles, which have abundant electron deficiencies derived from the [BO3] Lewis acid units, were uniformly cladded in the carbon nanofibers (LBO–CNF) and employed as interlayers for Li–S batteries. This functionalized interlayer expressed a high adsorption energy of ∼3.6 eV for polysulfides (e.g., Li2S6 and Li2S4) and effectively suppressed the polysulfides' shuttle behavior, delivering a high reversible capacity of 1242.6 mA h g−1 at 0.2C and good cycling performance with a low fading rate of 0.068% per cycle at 1C, thus effectually inhibiting the phenomenon of self-discharge. Besides, the lithiation reaction kinetics was also effectively enhanced, enhancing the rate performance of the battery to 644 mA h g−1 at 5C. This work provides a new strategy to enhance the electrochemical performance of Li–S batteries by applying the compounds of electronic-deficiency B-species and functionalized carbon.

✓ 已验证 DOI 高影响因子
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Journal of Central South University · 2025 ·Vol. 31 ·期 12 ·4437-4448 · IF 4.4

Hetero-metallic lithiophilic sites to assist sustained diffusion-deposition of Li+ toward stable lithium metal anodes

Huang Shao-zhen,He Pan,Yu Hua-ming,Li Hui-miao,Chen Li-bao

Lithium metal stands out as an exceptionally promising anode material, boasting an extraordinarily high theoretical capacity and impressive energy density. Despite these advantageous characters, the issues of dendrite formation and volume expansion of lithium metal anodes lead to performance decay and safety concerns, significantly impeding their advancement towards widespread commercial viability. Herein, a lithium-rich Li-B-In composite anode with abundant lithophilic sites and outstanding structural stability is reported to address the mentioned challenges. The evenly distributed Li-In alloy in the bulk phase of anodes act as mixed ion/electron conductors and nucleation sites, facilitating accelerated Li ions transport dynamics and suppressing lithium dendrite formation. Additionally, these micron-sized Li-In particles in LiB fibers framework can enhance overall structural integrity and provide sufficient interior space to accommodate the volume changes during cycling. The electrochemical performance of Li-B-In composite anode exhibits long-term cyclability, superior rate performance and high-capacity retention. This work confirms that the synergy between a 3D skeleton and hetero-metallic lithiophilic sites can achieve stable and durable lithium metal anodes, offering innovative insights for the practical deployment of lithium metal batteries.

CAS / MDL: 24937-79-9 872-50-4
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Nanomaterials · 2025 ·Vol. 15 ·期 15 ·1144 · IF 4.3

Surface Microstructure Engineering for Enhancing Li-Ion Diffusion and Structure Stability of Ni-Rich Cathode Materials

Huanming Zhuo,Shuangshuang Zhao,Ruijie Xu,Lu Zhou,Ye Li,Yuehuan Peng,Xuelong Rao,Yuqiang Tao,Xing Ou

Surface microstructure of grains vastly decides the electrochemical performance of nickel-rich oxide cathodes, which can improve their interfacial kinetics and structural stability to realize their further popularization. Herein, taking the representative LiNi0.8Co0.15Al0.05O2(NCA) materials as an example, a surface heterojunction structure construction strategy to enhance the interface characteristics of high-nickel materials by introducing interfacial ZnO sites has been designed (NCA@ZnO). Impressively, this heterointerface creates a strong built-in electric field, which significantly improves electron/Li-ion diffusion kinetics. Concurrently, the ZnO layer acts as an effective physical barrier against electrolyte corrosion, notably suppressing interfacial parasitic reactions and ultimately optimizing the structure stability of NCA@ZnO. Benefiting from synchronous optimization of interface stability and kinetics, NCA@ZnO exhibits advanced cycling performance with the capacity retention of 83.7% after 160 cycles at a superhigh rate of 3 C during 3.0–4.5 V. The prominent electrochemical performance effectively confirms that the surface structure design provides a critical approach toward obtaining high-performance cathode materials with enhanced long-cycling stability.

CAS / MDL: 10196-18-6 1310-66-3
✓ 已验证 产品关联 DOI PubMed 高影响因子
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ELECTROCHIMICA ACTA · 2025 · IF 5.6

Zwitterionic liquid electrolyte with efficient Li+ transfer modulated by ion pair for low-temperature lithium battery

Chenye Wang,Yan Dai,Rongrong Cao,Lei Bai,Jie Zhang,Wenjia Wu,Weijie Kou,Jingtao Wang

Zwitterions, covalently tethered by cation and anion, show great potential in the development of safe and high-performance electrolyte owing to the inherent characteristics of non-volatility, non-flammability, and electrification but non migration. The interaction between cations and anions in zwitterionic-lithium salt electrolyte is supposed to influence the lithium ions (Li + ) migration efficiency, but being rarely studied. Herein, zwitterionic liquid (ZIL) electrolytes with three different anionic groups (−PO 4 − , −SO 3 − , −COO − ) were synthesized. We demonstrate that the −PO 4 − group with the most negative electrostatic potential exerts the strongest competitive coordination effect on Li + , weakening Li + -TFSI − binding and promoting lithium salt dissociation. This coordination also facilitates a lower migration energy barrier for Li + and lessens intermolecular forces between zwitterions, reducing the freezing point. The ZIL-P electrolyte with the −PO 4 − group shows high Li + transference number (0.54 at −40 °C) and ionic conductivity (1.57 × 10 −4 S cm −1 at −20 °C), outperforming most liquid electrolytes. The enhanced Li + transfer results in excellent cycling stability, with a 98.1% capacity retention after 500 cycles at 0.5C. Furthermore, the gel electrolyte constructed with ZIL-P and silicon-based framework improved battery performance: LFP|SiGE-ZIL-P|Li after 600 cycles with capacity retention rate of 98.5% at 0.5C and −20 °C.

CAS / MDL: 24937-79-9 872-50-4
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POLYMER · 2025 · IF 4.5

Improved gel polymer electrolyte via imidazolium ionic liquid for stabilizing the interface of Li metal batteries

Xiuling Dong,Xinyi Ge,Wei Chen,Shuangqing Li,Zheng Xing,Qingguo Zhang,Zhong-Xia Wang

The interface problem between Li anode and gel polymer electrolytes (GPEs) hinder the performance improvement and application of Li metal batteries (LMBs). Herein, a GPE showcasing high ionic conductivity (3.91 mS cm −1 ) and elastic modulus (6.04 MPa) as GPE based on poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) was devised by introducing ionic liquids (ILs). The reconfiguration of Li ion solvation environment and the formation of LiF-rich solid electrolyte interface (SEI) protective layer have improved the interface problem. The LMB assembled from an optimized GPE- ET0.25 has stable Li deposition and excellent electrochemical properties , making the Li||LiFePO 4 (LFP) battery attaining an impressive long-cycle capacity retention rate of 96.0 %. This study emphasizes the advantages of IL aligned GPEs design, and the significance of forming stable SEI to improve battery performance, and provides ideas for the design of flexible LMBs with high safety and high performance.

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FUEL · 2025 · IF 7.5

Suppressing Adverse Effects of redox mediator shuttling in Li-air batteries by using silicon-based anode

Qinghui Yan,Min Wu,Huafeng Zhou,Haoshen Huang,Zhengfei Chen,Haiyong He,Zixuan Liu

Lithium-air batteries (LABs) are highly attractive for their highest energy density among all energy storage systems, but the high reactivity and volumetric variation of lithium metal anode (LMA), as well as the inter-electrode crosstalk (shuttling) by soluble species, e.g. redox mediators (RMs), impose arduous challenges for their practicality. Traditional countermeasures such as LMA protecting structures and solid-state electrolytes (SSEs) increase heft, complexity and cost, diminishing LAB’s core advantage—the ultrahigh energy density. In this work, a high-capacity (1750 mAh g -1 SCC ) silicon-carbon composite (SCC) material was synthesized and used as the anode in a Li-ion air battery, exhibiting superior cyclability (86 cycles under 300 mAh g -1 carbon ) compared to that with LMA (61 cycles), and physical characterizations revealed no deposition of RM on the SCC anode despite the absence of SSEs to prevent shuttling, demonstrating their excellent compatibility. This work showcases the prospects of silicon-based anodes to address LABs’ anode stability issue and improve cell cyclability while retaining most of the energy density.

✓ 已验证 产品关联 DOI 高影响因子
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DESALINATION · 2025 · IF 9.8

Configuring 5TiO2·2H2O/C composite-type adsorbents for effectively recovering Li+ from original Salt Lake brines

Xuemei Zhuo,Chunxi Hai,Yanxia Sun,Shengde Dong,Luxiang Ma,Xin He,Qi Xu,Masayoshi Fuji,Takashi Shirai,Yuan Zhou

Spinel-structured titanium‑lithium adsorbents have emerged as a promising solution for efficiently recovering Li + from Salt Lake brines with high Mg/Li ratio, owing to their stable structure, minimal dissolution loss, and excellent cycling stability. However, their practical application remains limited due to low adsorption capacity and prolonged equilibration times. In this study, we developed a novel 5TiO 2 ·2H 2 O/C adsorbents, synthesized by eluting Li 4 Ti 5 O 12 /C precursors with 0.15 mol/L HCl, which exhibits high adsorption capacity and minimal dissolution loss. Under optimal conditions, the 5TiO 2 ·2H 2 O/C adsorbents reached adsorption equilibrium within 5 h at 60 °C in a 600 ppm LiOH solution, with a maximum adsorption capacity of 41.84 mg/g and a titanium dissolution loss of only 0.29 %. The adsorption selectivity of the 5TiO 2 ·2H 2 O/C adsorbents was found to be strongly pH-dependent. In a 170 ppm Li + solution, the adsorbents demonstrated superior cycling stability in original Salt Lake brines, outperforming those in LiCl and Li 2 SO 4 solutions. This study provides valuable insights into the formation and mechanisms of action of these adsorbents, offering significant implications for the efficient recovery of Li + from various brines.

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MACROMOLECULAR RAPID COMMUNICATIONS · 2025 · IF 4.3

Large-Scale Preparation of Fluorinated Antifouling Nanofiltration Membranes with High Ion Selectivity for Li+/Mg2+ Separation

Bo Peng,Shuai Gu,Hongwei Lu,Juntao Tang,Chunyue Pan,Guipeng Yu

Developing high-efficiency antifouling nanofiltration (NF) membranes is crucial to address the dual challenges of low separation selectivity and severe membrane fouling in lithium extraction from high Mg 2+ /Li + ratio salt-lake brines. This study presents an efficient strategy based on one-step dip-coating surface modification. By grafting 1, 2-epoxy-3,3,3-trifluoropropane (TFO) molecules onto a PEI-TMC polyamide (PA) base membrane, a unique bipolar electrostatic potential reconstruction was triggered, simultaneously and significantly enhancing both the separation selectivity and antifouling performance of the membrane. In simulated high Mg 2+ /Li + ratio brine (2000 ppm, Mg 2+ /Li + = 30:1), the PA-TFO 0.75 membrane demonstrated exceptional integrated performance by achieving a high Li + /Mg 2+ selectivity of 20.5 (9.76 times higher than commercial NF membranes) while maintaining a high water permeance of 14.65 L m −2 h −2 bar −1 , and exhibiting an outstanding flux recovery ratio (FRR) approaching 100.6% (a 151% improvement over the pristine membrane), thereby meeting industrial fouling resistance standards. Critically, this strategy enabled the continuous fabrication of large-area membranes (60 m × 0.298 m). The assembled spiral-wound module (1812-type) retained a Li + /Mg 2+ selectivity of 19.5 in the same simulated brine, providing an efficient, antifouling, and scalable industrial-scale solution for lithium extraction from high Mg 2+ /Li + ratio salt lakes.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Materials Today Chemistry · 2025 · IF 6.7

Li4SiO4 coating enables stable interfaces and voltage suppression in Ni-rich cathodes for Li-ion batteries

Jean Pierre Mwizerwa,Chenlong Gao,Changyong Liu,Wenfei Lu,Menghao Yang,Jun Shen

Constructing a robust, highly Li-ion-conductive surface layer is an effective strategy to improve the interfacial stability of nickel-rich cathodes like LiNi 0 . 8 Co 0 . 1 Mn 0 . 1 O 2 (NCM811). However, existing methods often fail to balance ion/electron conductivity with suppression of surface phase transformations, leading to poor rate capability, cycling stability, and energy density. This work introduces an in-situ solution-phase formed coating of Li 4 SiO 4 (LSO) that creates a continuous ion/electron-conductive network across NCM811 particles. This LSO enhances lithium-ion transport, builds a stable electrode/electrolyte interface, and alleviates mechanical stress during cycling. As a result, NCM811@LSO exhibits improved electrochemical performance, including reduced voltage decay and stable operation at high voltages. The LSO coating suppresses surface degradation, intergranular cracking, and parasitic reactions by shielding active sites and reducing direct electrolyte contact. It also mitigates electrode polarization and localized overcharging during long-term cycling. Full-cell tests using graphite and SiO/C anodes confirm high energy densities, reaching 765 Wh kg −1 in NCM811@LSO//graphite cells. Furthermore, density functional theory (DFT) calculations support the experimental findings, revealing that LSO promotes favorable interfacial chemistry, suppresses internal cracking, inhibits nickel migration, and prevents irreversible phase transformations. Compared to traditional coatings, the multifunctional LSO layer offers superior protection and conductivity, making it a promising approach for developing advanced, high-energy-density lithium-ion batteries.

CAS / MDL: 13048-33-4
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