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JOURNAL OF POWER SOURCES · 2025 · IF 7.9

Fluorine doping induced accelerated Li+ kinetics in conversion-type Fe3O4 anode

Shasha Guo,Mohamed Ait Tamerd,Jiayi Li,Jianwei Wu,Xinyue Shi,Chih-Wen Pao,Zhiwei Hu,Jiwei Ma

Magnetite (Fe 3 O 4 ) is a potential anode for high-energy-density lithium-ion batteries thanks to its high theoretical capacity and cost-effectiveness. Yet, the capacity decay and limited kinetics induced by the structure damage along the conversion process need to be emphasized before its practical application. In this study, we propose an intrinsic modulation of Fe 3 O 4 using fluorine doping to considerably boost the cycle stability and rate capability. Benefiting from the enlarged metal-anion distance and improved electronic conductivity induced by the fluorine dopants, the as-prepared Fe 3 O 3.94 F 0.06 anode provides a low-energy-barrier path for the Li + intercalation, which is responsible for the enhanced kinetics. The present study emphasizes the essential role of anion modification on conversion-type transition metal oxides that enable boosting the electrochemical performance towards high-energy-density battery applications.

研究领域: 材料科学 · 电化学 · 能源存储 · 无机化学 · 固态化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF MATERIALS SCIENCE · 2025 · IF 3.9

Dendrite-suppressing Li–S batteries through triple-component polymer electrolyte design

Wang Zhaokun,Li Chen,Pan Yanrui,Ma Yue,Ye Mingfu,Shi Xixi,Zhang Hongzhou,Song Dawei,Zhang Lianqi

Lithium-sulfur (Li–S) batteries are considered as one of the most promising next-generation energy storage devices. However, due to the high working current density and the shuttle of polysulfides, a large number of dendrites and corrosion are formed on Li anode, restricting the wide application of Li–S battery. Herein, a triple-component gel polymer electrolyte (PHMA) comprising poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)–polyacrylonitrile (PAN)–polymethyl methacrylate (PMMA) is developed, the excellent processability and Li ion conductivity of PVDF-HFP, the excellent polysulfide adsorption capability of PAN and the excellent wettability of PMMA are significantly enhanced after compositing, then uniform Li ions deposition is regulated and the growth of Li dendrite is greatly suppressed. In addition, the shuttle effect of polysulfides is greatly suppressed through physical, chemical and weak hydrogen bonding adsorption provided by the diversification of polar groups. Given these advantages, an ionic conductivity of 4.0 × 10 –3  S cm −2 is achieved and a minor polarization voltage of 15 mV is exhibited for Li//Li cell after 1000 h cycling, in situ optical microscope-electrochemical cell further robustly confirms the enhanced stability of Li foil. As a result, S/PHMA/Li battery delivers stable cycling performance with a capacity decay of 0.5% per cycle after 100 cycles at 0.2 C. Graphical

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ACS Nano · 2024 · IF 15.8

Zn and Cl Coregulated MXene Catalyst Enhances Li-CO2 Battery Reversibility

Xue Tian,Huan Liu,Bin Cao,Peng Zhang,Yanze Li,Yanchao Ou,Haonan Cui,Mengyao Xu,Bin Xu

MXenes are promising cathodes for Li–CO2 batteries owing to their high electrical conductivity and efficient CO2 activation function. However, the effects of adsorption and electronic structures of MXene on the full life cycle of Li–CO2 batteries have been rarely investigated. Here, we employ a coregulation approach to enhance the adsorption–decomposition of lithium carbonate (Li2CO3) by introducing Zn and Cl surface groups onto the Ti3C2 MXene (Zn–Ti3C2Cl2) catalyst. The incorporation of Cl surface groups enhances Li2CO3 adsorption on the MXene catalyst surface, resulting in the formation of small-sized and uniform Li2CO3. Additionally, the introduction of Zn shifts the d-band centers of titanium and promotes CO2 evolution reaction (CO2ER) activity, thereby facilitating the decomposition of discharge products. As a result, the Li–CO2 battery based on the Zn–Ti3C2Cl2 catalyst exhibits an ultralow overpotential (0.72 V) at 200 mA g–1 and stable cycling for up to 1500 h. This work validates the efficacy of promoting reversibility in Li–CO2 batteries by adjusting the adsorption-decomposition process.

研究领域: 材料科学 · 电化学
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ACS Energy Letters · 2022 · IF 23.991

Local Li+ Framework Regulation of a Garnet-Type Solid-State Electrolyte

Furong Sun,Yubo Yang,Shu Zhao,Yongtao Wang,Mingxue Tang,Qingzhen Huang,Yang Ren,Heng Su,Boya Wang,Ning Zhao,Xiangxin Guo,Haijun Yu

Garnet-type solid-state electrolytes Li7La3Zr2O12 (LLZO) for high-energy-density batteries have attracted extensive attention. However, stabilizing the high-conductive cubic phase and improving its ionic conductivity remain challenges of current research. Here, a Ca–W dual-substitution strategy has been designed, and the effect of doping on cubic phase formation and Li+ mobility has been investigated thoroughly. The results indicated that the partial substitution of Ca2+ at the La3+ site and W6+ at the Zr4+ site can effectively stabilize the cubic phase while reducing the endothermic enthalpy during the synthesis. Moreover, Ca–W dual substitution regulates the local Li+ framework by increasing Li+ occupancy at the 96h site, which can significantly lower the Li+ migration barrier and thus improve the ionic conductivity by two orders of magnitude. This work addresses the challenge of stabilizing a highly conductive cubic phase with low-energy consumption and represents a major breakthrough in understanding how to improve the ionic conductivity by regulating local structures.

研究领域: 材料科学 · 固体离子学 · 储能技术 · 电池技术
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ADVANCED MATERIALS · 2022 ·Vol. 35 ·期 2 ·2208974 · IF 32.086

Ultrafast Non-Equilibrium Synthesis of Cathode Materials for Li-Ion Batteries

Wei Zhu,Jingchao Zhang,Jiawei Luo,Cuihua Zeng,Hai Su,Jinfeng Zhang,Rui Liu,Enyuan Hu,Yuansheng Liu,Wei-Di Liu,Yanan Chen,Wenbin Hu,Yunhua Xu

The synthesis of cathode materials plays an important role in determining the production efficiency, cost, and performance of lithium-ion batteries. However, conventional synthesis methods always experience a slow heating rate and involve a complicated multistep reaction process and sluggish reaction dynamics, leading to high energy and long time consumption. Herein, a high-temperature shock (HTS) strategy is reported for the ultrafast synthesis of cathode materials in seconds. The HTS process experiences an ultrahigh heating rate, leading to a non-equilibrium reaction and fast reaction kinetics, and avoids high energy and long time consumption. Mainstream cathode materials (such as LiMn 2 O 4 , LiCoO 2 , LiFePO 4 , and Li-rich layered oxide/NiO heterostructured material) are successfully synthesized with pure phases, oxygen vacancies, ultrasmall particle sizes, and good electrochemical performance. The HTS process not only provides an efficient synthesis approach for cathode materials, but also can be extended beyond lithium-ion batteries.

研究领域: 材料科学 · 电化学 · 能源存储
✓ 已验证 DOI 高影响因子
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RSC Advances · 2025 ·Vol. 15 ·期 29 ·23819-23826 · IF 4.6

S-decorated Mo2C as efficient catalyst for Li–O2 battery system

Yanhong Ding,Zhichao Gao,Rongpeng Lin,Yong Cao,Haoyang Liu,Yulin Zhou,Haifeng Xu,Jiayi Liu,Fangqi Ren,Yirong Zhu

Lithium–oxygen (Li–O2) batteries are considered an important candidate for the next generation of energy storage systems due to their ultra-high theoretical energy density (11 586 mA h g−1), but their slow kinetic reactions, high overpotential and cyclic instability seriously limit their practical applications. In this study, sulfur modified Mo2C (S@Mo2C) cathode materials were prepared by hydrothermal synthesis by sulfur (S) doping to optimize the electronic structure and catalytic activity of Mo2C (Mo2C). Experiments show that S@Mo2C exhibits significantly improved electrochemical performance compared to commercial Mo2C: its specific capacity is up to 3955 mA h g−1 (commercial material only 508 mA h g−1), the charge and discharge overpotential is reduced to 0.26 V (53.6%), and the capacity retention rate remains 77.8% after 250 cycles. X-ray diffraction (XRD), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) analysis showed that the introduction of sulfur induced the formation of a heterostructure of MoS2/MoS3 in the Mo2C lattice, which enhanced the conductivity and oxygen reduction/precipitation (ORR/OER) activity of the material. In addition, sulfur doping promotes the formation of highly conductive amorphous Li2O2 and effectively inhibits the accumulation of insulating ring Li2O2, thus significantly improving the cycle stability and energy efficiency of the battery. This study provides a new structural regulation strategy for the design of high efficiency lithium oxygen battery catalysts.

研究领域: 能源存储 · 材料科学 · 电化学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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Energy Storage Materials · 2022 · IF 20.831

Double-salt electrolyte for Li-ion batteries operated at elevated temperatures

Long Chen,Jianhao Lu,Yibo Wang,Pan He,Shaobo Huang,Yan Liu,Yanzhou Wu,Gaoping Cao,Li Wang,Xiangming He,Jingyi Qiu,Hao Zhang

Lithium ion batteries (LIBs) have swept the whole energy storage field. However, the current mainstream lithium batteries are difficult to operate stably at high temperature (>60°C) due to the decomposition of electrolyte and solid electrolyte interphase (SEI), the cathode metal elements dissolution behavior, and potential thermal runaway. Here, We report a double-salt electrolyte with lithium bis(fluorosulfonyl)imide (LiFSI) and lithium difluoro(oxalato)borate (LiDFOB) as electrolyte salt, fluoroethylene carbonate (FEC), and tetra(ethylene glycol) dimethyl ether (TEGDME) as cosolvent, which delivers excellent ionic conductivity, high electrochemical stability and satisfactory ability to impede the dissolution of Fe element under elevated temperature (70°C). In addition, the electrolyte is benefited to form a robust and thermal-resistance solid-electrolyte interface (SEI) layer on the surface of graphite (Gr) anode, which shows improved decomposition temperature (86°C). The assembled thermally stable and high-safety 1300 mAh 18650-type LiFePO 4 |Gr cell shows high Coulombic efficiency (∼99.7%), improved cycling stability with discharge capacity 871.1 mAh after 200 cycles at 0.5 C and 70°C. This work affords a splendid strategy for address the unstable interface at both cathode and anode for safe high-temperature LIBs.

研究领域: 材料科学 · 电化学
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Energy Storage Materials · 2022 · IF 20.831

Imidazolium bromide: A tri-functional additive for rechargeable Li-O2 batteries

Jingning Lai,Nan Chen,Fengling Zhang,Bohua Li,Yanxin Shang,Liyuan Zhao,Li Li,Feng Wu,Renjie Chen

High energy density lithium-oxygen (Li-O 2 ) batteries require soluble catalysts to accelerate the kinetics of oxygen reduction/evolution reaction (ORR/OER), and require SEI forming additives to protect lithium metal anode from side reaction with solvents, reduced oxygen species and soluble catalysts. In this study, a tri-functional additives 1-methyl, 3-benzyl, 1H imidazolium bromide (IMPBr) is dissolved in the dimethyl sulfoxide (DMSO)-based electrolyte to solve the problems of the slow dynamic process of ORR and OER, and protect the lithium anode by suppressing the dendrite formation in O 2 atmosphere. During discharging, IMP + has a strong binding ability to the intermediate product O 2 − , and Br − is highly associated with Li + , helping drive the solvation mechanism. During charging, Br − mediates the decomposition of battery discharge products and reduces the charge overpotential. Meanwhile, the positively charged IMP + can be attracted to the surface of the anode via electric attraction, in situ forming a stable SEI layer to prevent DMSO, Br 3 – , and Br 2 from attacking the lithium metal and growth of lithium dendrites. The synergy effect of the IMP + and Br – improves the cycle and rate performance of the Li-O 2 battery.

研究领域: 电化学 · 材料科学
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ELECTROCHIMICA ACTA · 2017 · IF 4.798

Hybrid Mg2+/Li+ batteries with Cu2Se cathode based on displacement reaction

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

Based on a displacement reaction mechanism, Cu 2 Se is a good candidate for non-insertion-based cathode materials of rechargeable magnesium batteries . Nevertheless, its relatively low electronic conductivity leads to a poor rate capability and an unsatisfactory cycling performance. In this work, we firstly reported the improved electrochemical performance of Cu 2 Se cathode based on displacement reaction for Mg batteries triggered by a Li salt additive in a typical magnesium electrolyte 0.4 mol dm −3 (PhMgCl) 2 -AlCl 3 /THF. Cu 2 Se materials with different morphologies and particle sizes were synthesized by a solvothermal process and a hydrothermal method , respectively. Cu 2 Se with smaller particle sizes by the hydrothermal method exhibits a higher specific capacity (152.7 mAh g −1 first discharge capacity at 0.02 C) but poor cycling performance in 0.4 mol dm −3 (PhMgCl) 2 -AlCl 3 /THF electrolyte. LiCl was added in the magnesium electrolyte to promote the displacement reaction of the Cu 2 Se material. An initial discharge capacity of approximately 239.7 mAh g −1 with 48.4% capacity retention after 20 cycles at 0.1 C can be obtained for Cu 2 Se in 0.4 mol dm −3 (PhMgCl) 2 -AlCl 3 +1.0 mol dm −3 LiCl/THF electrolyte. Furthermore, the cycling performance and rate capability are enhanced by in situ homogeneously anchoring Cu 2 Se particles onto the surface of the reduced graphene oxide (rGO) nanosheets . Cu 2 Se/rGO composite with 10 wt% rGO exhibits 64.2% capacity retention after 20 cycles at 0.1 C, and a more than 120 mAh g −1 reversible capacity at 0.2 C in the hybrid Mg 2+ /Li + electrolyte.

研究领域: 材料科学 · 电化学 · 能源存储技术
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ANGEWANDTE CHEMIE-INTERNATIONAL EDITION · 2015 ·Vol. 54 ·期 14 ·4338-4343 · IF 11.261

Recycling Application of Li–MnO2 Batteries as Rechargeable Lithium–Air Batteries

Yuxiang Hu,Tianran Zhang,Fangyi Cheng,Qing Zhao,Xiaopeng Han,Jun Chen

Graphical Never say die : Depleted Li–MnO 2 batteries could be further utilized as rechargeable Li–O 2 batteries with admitted oxygen. Thus, when the manganese oxide electrode was lithiated in situ and exposed to air (see picture), the resulting battery showed superior performance, including high capacity, a low overpotential, high rate capability, and high cycling stability. The ever-increasing consumption of a huge quantity of lithium batteries, for example, Li–MnO 2 cells, raises critical concern about their recycling. We demonstrate herein that decayed Li–MnO 2 cells can be further utilized as rechargeable lithium–air cells with admitted oxygen. We further investigated the effects of lithiated manganese dioxide on the electrocatalytic properties of oxygen-reduction and oxygen-evolution reactions (ORR/OER). The catalytic activity was found to be correlated with the composition of Li x MnO 2 electrodes (0< x <1) generated in situ in aprotic Li–MnO 2 cells owing to tuning of the Mn valence and electronic structure. In particular, modestly lithiated Li 0.50 MnO 2 exhibited superior performance with enhanced round-trip efficiency (ca. 76 %), high cycling ability (190 cycles), and high discharge capacity (10 823 mA h g carbon −1 ). The results indicate that the use of depleted Li–MnO 2 batteries can be prolonged by their application as rechargeable lithium–air batteries.

研究领域: 材料科学 · 能源技术 · 环境科学
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SOLID STATE IONICS · 2021 · IF 3.785

Functionalized gel polymer electrolyte membrane for high performance Li metal batteries

Baichuan Han,Pengfeng Jiang,Shuai Li,Xia Lu

Inorganic solid-state electrolytes have high ionic conductivity and stability, which demonstrate the promising application in building solid batteries excepting their poor interface compatibility. Hence, making the solid electrolytes flexible, such as the combination with polymer is an important strategy in mitigating such problem. In this context, a robust membrane is fabricated with nanosized Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 particles being filled into the porous PVDF-HFP as gel polymer electrolyte (GPE). This membrane displays a high ionic conductivity of 3.57 × 10 −4  S cm −1 , a large Li-ion transference number of 0.62, as well as the good mechanical strength and thermal stability. The as prepared Li/GPE/Li symmetric cell demonstrates an underlying electrochemical activation in stabilizing the membrane-electrode interface, which seems to be balancing the trade-off between the Li diffusion and side reactions at the interface. The fabricated LiFePO 4 |GPE|Li coin cell delivers a high Coulombic efficiency of 98%, a good rate capability at 2C (about 120 mAh g −1 ) and capacity retention of 92% after 110 cycles (150 mAh g −1 , 0.4C) at room temperature. This important design provides a rewarding avenue to address the interface compatibility and develop composite electrolytes for high performance Li metal batteries .

研究领域: 材料科学 · 电化学
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CARBON · 2019 · IF 7.466

Fe-doped LiMnPO4@C nanofibers with high Li-ion diffusion coefficient

Hao Yang,Cuimei Fu,Yijian Sun,Lina Wang,Tianxi Liu

Olivine-type LiMnPO 4 (LMP) cathodes have gained enormous attraction for Li-ion batteries (LIBs) due to high discharge platform, theoretical capacity and thermal stability. However, it is still challenging to achieve encouraging Li-storage behavior owing to the low electronic conductivity and slow Li-ion diffusion rate of LMP. Here, the electrochemical behavior of fibrous LiFe x Mn 1-x PO 4 @carbon (LF x M 1-x P@C, x = 0, 0.25, 0.5, 0.75, 1) composites with different Fe doping amounts is investigated. Among the composites, LF 0.5 M 0.5 P@C demonstrates a superior cell performance due to a higher Li-ion diffusion coefficient (D Li ), resulting from a proper Fe doping ratio and a more uniform morphology. At a current rate of 0.2 C (1 C = 170 mA g −1 ), the LF 0.5 M 0.5 P@C cathode delivers a specific capacity of 150 mAh g −1 up to 500 cycles with a capacity retention of 119%. A longer-term cycling at 5 C for 2000 cycles can be maintained with a reversible capacity exceeding 102 mAh g −1 . The fundamental study provides an insightful guidance for future design of cathode materials with high performance.

研究领域: 材料科学 · 电化学
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