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Journal of Energy Storage · 2023 · IF 9.4

A new fluorine-containing sulfone-based electrolyte for advanced performance lithium metal batteries

Sa Xue,Yang Zhou,Xiangyang Liu,Maogang He

Lithium dendrite growth greatly limits the application of lithium metal batteries . Herein, a new fluorine-containing sulfone-based electrolyte is proposed for lithium metal batteries. Benefiting from the synergistic effect of lithium bis(fluorosulfonyl)imide (LiFSI) and fluoroethylene carbonate (FEC), a LiF-rich stable SEI with compact and uniform morphology is formed on lithium metal anode , suppressing the Li dendrite formation and enhance the cycling life. In Li||Cu half-battery, a remarkable Coulombic efficiency of 95.9 % within 130 cycles and 93.5 % within 100 cycles are realized at 0.5 mA·cm −2 and 1 mA·cm −2 , respectively. In Li||Li symmetric battery , the cycling life is about 480 h at 1.0 mA·cm −2 which is double as the commercial electrolyte. Moreover, in Li||LiFePO 4 battery, a significantly improved capacity retention of 94.3 % with a high average Coulombic efficiency of 99.8 % after 100 cycles is achieved at 0.5C. The designed new fluorine-containing sulfone-based electrolyte provides new strategy toward high energy density lithium metal batteries.

研究领域: 材料科学 · 电化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

The effect of AlF3 as an electrolyte additive on Li anode in Li-O2 batteries

Guiru Sun,Zexu Zhang,Daming Yang,Yan Wang,Wei Lu,Mei Liu,Ming Feng

Li metal is considered as an ideal anode for Li-O 2 batteries because of its unbeatably theoretical specific capacity and low electrode potential. Unfortunately, the growth of Li dendritic and the sensitivity to electrolyte and O 2 hinder the practical applications of Li anode. Herein, AlF 3 as an electrolyte additive is firstly employed in a Li-O 2 battery, which can boost the formation of LiF@Al-Li@Al 2 O 3 -rich SEI film via in-situ spontaneous reactions of AlF 3 with Li anode in O 2 atmosphere. The generated SEI film contributes to inducing the homogeneous nucleation of Li and reducing the disgusting side reactions, which can suppress the growth of Li dendrite and improve the cyclability of Li anode. Benefiting from the rational design, both the Li-O 2 and the Li|Li symmetric batteries with AlF 3 electrolyte exhibit low overpotential and good cycling stability. We hope this work could provide a facile way to in-situ construct a stable SEI film to alleviate the uneven Li nucleation for Li-O 2 batteries.

研究领域: 材料科学 · 电化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Novel strategies for constructing highly efficient silicon/carbon anodes: Chemical prelithiation and electrolyte post-treatment

Dan Hu,Caiyun Wu,Qiubo He,Shuju Zhang,Shiquan Wang,Rong Zeng,Yanqing Zhang,Jianwen Liu

Chemical prelithiation is an effective method to compensate for the loss of active lithium due to the formation of solid electrolyte interface, effectively addressing the issue of low initial coulombic efficiency (ICE) in silicon/carbon (Si/C) materials. Herein, the Si/C anode is prelithiated in a 1 M lithium-phenanthrene/2-methyltetrahydrofuran (Li-Phe/2-MTHF) solution in our work, and the prelithiated Si/C anode is followed by post-treatment with commercial electrolytes containing lithium difluorobis(oxalato)phosphate (LiDFBOP). The PSi/C-L 0.5 , originated from the reaction between residual Li-Phe/2-MTHF and the commercial electrolyte containing 0.5 wt% LiDFBOP, possesses the artificial SEI film, which not only contains a proper amount of LiF but also is rich in Li 2 C 2 O 4 and Li 3 P. Among them, LiF and Li 2 C 2 O 4 ensures the stability of the SEI film. Simultaneously, the synergistic effect of Li 3 P and LiF improves its Li + transport kinetics. Therefore, the ICE of PSi/C-L 0.5 reaches 92.50 %, and almost no drop in capacity occurs after 100 cycles at 0.5 A/g. Furthermore, the capacity stays steady at about 270 mAh/g through nearly 500 cycles at 1 A/g, achieving an impressive capacity retention rate of 97.8 %, significantly outperforming un-treated Si/C. This study offers new directions for constructing SEI films with stable structures and high Li + kinetics transport.

研究领域: 材料科学 · 电化学
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ACS Applied Energy Materials · 2025 · IF 5.5

Dual Additives to Stabilize the Electrode–Electrolyte Interface of Lithium-Rich Layered Cathodes for High-Energy Batteries

Boyang Zhang,Xiaola Li,Ziyang Liang,Wenzhao Huang,Yuqing Liu,Chenyu Liu,Zhan Lin,Dong Luo

Lithium-rich manganese-based oxides (LMOs) are regarded as promising cathodes for next-generation high-energy Li-ion batteries due to their ultrahigh discharge capacity (>250 mAh/g) and low cost. However, their practical application is significantly hindered by issues such as transition metal dissolution and structural evolution under high working voltage. In this study, a stable SEI protective film based on carbon phosphorus is successfully constructed by introducing two solid–liquid interface-stabilizing additives, ethylene carbonate (VC) and tri(pentafluorophenyl)borane (TPFPB), into the base electrolyte. This significantly enhances the interface stability between the lithium-rich manganese-based cathode material and the electrolyte, suppresses the generation of harmful HF and the dissolution of transition metals, thereby improving the overall stability of the electrode–electrolyte system. Experimental results indicate that after 200 cycles, the capacity retention of the LMO cathode is increased by 21% due to the significant suppression of nanopore formation and phase transitions. This additive optimization strategy provides promising technical guidance for the application of lithium-rich manganese-based oxide cathode materials in next-generation high-energy-density rechargeable batteries.

CAS / MDL: 872-50-4
研究领域: 材料科学 · 电化学 · 能源存储
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Surfaces and Interfaces · 2023 · IF 6.2

Pentafluoropyridine additive induced SEI film regulation and remarkable performance improvement of the lithium primary batteries

Ping Li,Enmin Xu,Yingke Zhou,Jialu Liu,Zhongzhi Yuan,Xiaohui Tian

Lithium primary batteries with lithium metal anode are extensively applied in the portable appliances and electronic fields for the high specific energy and power, low self-discharge and wide operating temperature. However, the application of lithium metal anode causes the safety and stability issues. Herein, the pentafluoropyridine (C 5 F 5 N) was applied as an electrolyte additive in lithium primary battery, to construct a suitable surface layer on lithium anode to increase the stabilization and electrochemical performance . With C 5 F 5 N additive, the discharge capacity of the Li primary battery increases to 422.1 mAh/g at 0.01 C, compared to 62.2 mAh/g of the pristine battery. Meanwhile, the storage performance of the batteries was also greatly enhanced with the C 5 F 5 N additive. After stored for 60 days at room temperature, the Li primary battery with additive displays a specific discharge capacity of 180.7 mAh/g, much higher than the pristine battery without additive (43.6 mAh/g). The significant improvements in capacitive and storage performances are attributed to the additive induced inhibition of decomposition of solvents and lithium salts and tuning of SEI composition on lithium anode surface. The C 5 F 5 N is a promising electrolyte additive for the further development and application of high-performance Li primary batteries.

CAS / MDL: 7784-18-1 700-16-3
研究领域: 材料科学 · 电化学
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Journal of Energy Storage · 2025 · IF 9.8

Application of a cost-effective boron-based electrolyte additive in high-voltage lithium metal battery

Jian Lv,Zhuyu Wang,Yihuan Zhou,Weihao Yu,Qinggong Jia

Due to long-term operation under high voltage, the cathode of lithium metal battery undergoes parasitic reactions with the electrolyte, resulting in non-conductive polymers that severely affect the battery's electrochemical performance and kinetics. In addition, the safety performance of the battery is seriously compromised by severe lithium deposition on the lithium metal side. The use of electrolyte additives is one of the most cost-effective strategies for improvement. A low-cost boron-based additive bis(pinacolato)diboron (BDB) has been proposed in this work which has relatively high activity during battery charging and discharging. A protective cathode electrolyte interface (CEI) film was formed by BDB on the surface of NCM811 in advance to resist HF and solvent erosion. Furthermore, the solid electrolyte interface (SEI) film that BDB participates in on the lithium metal surface exhibits high ion conductivity and effectively inhibits the formation of lithium dendrites, thereby ensuring the safe operation of lithium metal batteries. The lithium metal battery utilizing BDB not only exhibits optimal electrochemical performance with a high cut-off voltage of 4.6 V, but also demonstrates potential for further development in the realms of rapid charging and discharging.

研究领域: 材料科学 · 电化学 · 能源存储技术
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Porous membrane host-derived in-situ polymer electrolytes with double-stabilized electrode interface enable long cycling lithium metal batteries

Yali Liu,Youlong Xu

The application of solid polymer electrolytes (SPEs) has been impeded by the low ionic conductivity, narrow oxidation potential and poor mechanical strength. Herein, we designed a novel in-situ PVDF-HFP/Poly 1,3-dioxolane (PDOL) polymer electrolyte with dual-salts and functional plasticizers of succinonitrile (SN)/fluoroethylene carbonate (FEC). One of the dual-salts, Lithium difloro(oxalato)borate (LiDFOB), could initiate the polymerization of DOL in-situ in the porous PVDF-HFP host to improve the interfacial compatibility. SN is beneficial to the improvement of ionic conductivity and the stability of high voltage cathodes, while the FEC can generate the LiF-rich SEI on Li metal anode. The PVDF-HFP host can further restrict the motion of anion and increase the strength of the SPE. Therefore, the as-obtained SPE exhibits a thin thickness of ∼ 32 μm, high ionic conductivity of 1.06 × 10 −4 S cm −1 at room temperature, an enlarged electrochemical window of 5.86 V versus Li/Li + and high lithium-ion transference number t Li+ of 0.72. Benefited from the synergetic effect, the Li/LiFePO 4 cell delivers a high initial capacity of 141.7 mAh g −1 at 2C with a capacity retention of 94.99% after 1000 cycles. This three-dimensional porous film-derived in-situ polymer electrolytes provide a new sight and simple strategy for designing polymer electrolytes, exhibiting attractive potential in flexible and high-energy–density solid-state batteries.

研究领域: 材料科学 · 电化学 · 能源存储
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Isocyanate Additives Improve the Low-Temperature Performance of LiNi0.8Mn0.1Co0.1O2||SiOx@Graphite Lithium-Ion Batteries

Fujuan Han,Zenghua Chang,Rennian Wang,Fengling Yun,Jing Wang,Chenxi Ma,Yi Zhang,Ling Tang,Haiyang Ding,Shigang Lu

LiNi0.8Mn0.1Co0.1O2||SiOx@graphite (NCM811||SiOx@G)-based lithium-ion batteries (LIBs) exhibit high energy density and have found wide applications in various fields, including electric vehicles. Nonetheless, its low-temperature performance remains a challenge. One of the most efficacious strategies to enhance the low-temperature functionality of battery is the development of appropriate electrolytes with low-temperature suitability. Herein, p-tolyl isocyanate (PTI) and 4-fluorophenyl isocyanate (4-FI) are used as additive substances to integrate into the electrolytes to improve the low-temperature performance of the battery. Theoretical calculations and experimental results indicate that PTI and 4-FI can both preferentially generate a stable SEI on the electrode surface, which is beneficial to reduce the interfacial impedance. As a result, the additive, i.e. 4-FI, is superior to PTI in improving the low-temperature performance of the battery due to the optimization of F in the SEI membrane components. At room temperature, the cyclic stability of the NCM811/SiOx@G pouch cell increases from 92.5% (without additive) to 94.2% (with 1% 4-FI) after 200 cycles at 0.5 C. Under the operating temperature of −20 °C, the cyclic stability of the NCM811/SiOx@G pouch cell increases from 83.2% (without additive) to 88.6% (with 1% 4-FI) after 100 cycles at 0.33 C. Therefore, a rational interphase design involving the modification of the additive structure is a cost-effective way to improve the performance of LIBs.

研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Stabilizing the SiOx Anode by a Highly Elastic Quasi-Solid Polyether-Based Electrolyte via an In Situ Fabrication

Mengyue Yu,Jian Ma,Lei Dong,Minghao Huang,Bangzhuang Xue,Yi Sun,Hongfa Xiang

Silicon monoxide (SiOx, x ≈ 1) has been a promising candidate of anode materials for next-generation lithium-ion batteries due to its high specific capacity (∼2600 mA h g–1). However, huge volume expansion and the resultant repeated destruction of the solid electrolyte interphase (SEI) are key challenges to the practical application of the SiOx anode. In this work, a highly elastic quasi-solid polymer electrolyte (QSPE) is demonstrated for batteries employing an SiOx anode, which is prepared via in situ cationic ring-opening polymerization employing 1,3,5-trioxane (TXE) as the monomer, 1,3,2-dioxathiolane 2,2-dioxide (DTD) as both the initiator and film-forming additive, and fluoroethylene carbonate as the plasticizer. This TXE-based QSPE possesses excellent ionic conductvity properties, including an extremely low glass-transition temperature of −94.3 °C, a high ionic conductivity of 1.36 mS cm–1 at 25 °C, and a high Li+ transference number of 0.66. The long poly-TXE skeleton endows the polymer electrolyte with a high elastic modulus of 42 MPa, helping to effectively suppress the volume expansion of the SiOx anode during cycling. DTD participates in the construction of a robust SEI containing Li2SOx species, mitigating the structural collapse of SiOx particles. As a result, the cyclic stability of the SiOx anode has been remarkably enhanced─the Li||SiOx half-battery with the in situ TXE-based QSPE achieves 81.9% capacity retention after 200 cycles at 0.5C, exhibiting significant improvement over its liquid-state counterparts and showing promising application potential.

CAS / MDL: 613-33-2
研究领域: 材料科学 · 电化学 · 能源存储
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CHEMISTRY-A EUROPEAN JOURNAL · 2023 ·Vol. 29 ·期 64 ·e202301774 · IF 4.3

Amorphous TiO2 shells: an Essential Elastic Buffer Layer for High-Performance Self-Healing Eutectic GaSn Nano-Droplet Room-Temperature Liquid Metal Battery

Lian Li,Kaizhao Wang,Kaijun Wang,Tianyou Chen,Jing Wang,Zhongshan Deng,Qingming Chen,Weijun Zhang,Jin Hu

Graphical The amorphous titanium dioxide is used to coat eGaSn nanodroplets (eGaSn NDs) to construct the core-shell structure of eGaSn@TiO 2 nanodroplets (eGaSn@TiO 2 NDs). The amorphous TiO 2 shell forms a stable SEI film, alleviates volume expansion, and provides electron/ion transport channels. The resulting eGaSn@TiO 2 NDs exhibit high capacities of 580, 540, 515, 485, 456 and 426 mAh g −1 at 0.1, 0.2, 0.5, 1, 2 and 5 C, respectively. No obvious decay is observed in more than 500 cycles with a capacity of 455 mAh g −1 at 1 C. Gallium-based alloy liquid metal batteries currently face limitations such as volume expansion, unstable solid electrolyte interface (SEI) film and substantial capacity decay. In this study, amorphous titanium dioxide is used to coat eutectic GaSn nanodroplets (eGaSn NDs) to construct the core-shell structure of eGaSn@TiO 2 nanodroplets (eGaSn@TiO 2 NDs). The amorphous TiO 2 shell (~6.5 nm) formed a stable SEI film, alleviated the volume expansion, and provided electron/ion transport channels to achieve excellent cycling performance and high specific capacity. The resulting eGaSn@TiO 2 NDs exhibited high capacities of 580, 540, 515, 485, 456 and 426 mAh g −1 at 0.1, 0.2, 0.5, 1, 2 and 5 C, respectively. No significant decay was observed after more than 500 cycles with a capacity of 455 mAh g −1 at 1 C. In situ X-ray diffraction (in situ XRD) was used to explore the lithiation mechanism of the eGaSn negative electrode during discharge. This study elucidates the design of advanced liquid alloy-based negative electrode materials for high-performance liquid metal batteries (LMBs).

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

Self-exfoliated covalent organic framework nano-mesh enabled regular charge distribution for highly stable lithium metal battery

Yunrui Zhang,Wenbo Wang,Meiling Hou,Yantao Zhang,Yaying Dou,Zehua Yang,Xiaoyang Xu,Haining Liu,Shanlin Qiao

Li metal batteries have won the fame for the enlarged cell potential and higher theoretical specific capacity. Nevertheless, the commercial implementation is still confronted with inevitable Li dendritic growth and depressed Coulombic efficiency. The Li + transfer behavior is the vital factor to ameliorate the durability of solid electrolyte interphase (SEI). Herein, a self-exfoliated TpTG covalent organic framework (COF) was developed to construct an artificial SEI film. The versatile cationic-skeleton of TpTG could spontaneously drive the formation of nano-mesh with thickness of 3∼6 nm, and facilitate uniform dispersibility on the Li metal surface. Moreover, the 7 Li solid-state nuclear magnetic resonance spectra, Fourier-transform infrared spectra, and density functional theory calculations have identified the energetic lithiophilicity and TFSI – repulsion features. The Cl – coordinated TpTG endowed with abundant lithiophilic sites can reconfigure the charge distribution and expedite the uniform Li + migration adjacent to the electrode|electrolyte interface. The uniform Li + flux distribution redounds to reversible lithium stripping/plating and tames the dendrite formation especially at high-rate protocols. The overwhelming evidences of lower polarization, prolonged lifespan, and compact Li deposition, corroborate the practicability of self-exfoliated TpTG to achieve the goal of high-energy-density Li metal batteries.

研究领域: 材料科学 · 电化学
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CERAMICS INTERNATIONAL · 2019 · IF 3.45

Sandwich structure of carbon-coated silicon/carbon nanofiber anodes for lithium-ion batteries

Yaru Li,Ruyi Wang,Jiwei Zhang,Jianping Chen,Chenqiang Du,Tianhua Sun,Jian Liu,Chunhong Gong,Jianhui Guo,Laigui Yu,Jingwei Zhang

For electrospun silicon/carbon nanofiber composites, the surface precipitation of silicon nanoparticles can cause poor cycle stability. To solve this, a carbon-coated silicon/carbon nanofiber (Si/C@C) composite with a ‘sandwich’ structure is constructed by hydrothermal reaction of glucose and an electrospun silicon/carbon nanofiber, followed by high-temperature carbonization. The effects of the thickness of the carbon coating layer and calcining temperature on the electrochemical performance are studied. The results showed that carbon is uniformly and continuously coated on the surface of the composite fibers, which avoid direct exposure of precipitated silicon on the surface of the nanofibers to the electrolyte, reduce the occurrence of side reactions and is conducive to the stable formation of SEI films. At the same time, the carbon shell inhibit the volume expansion of silicon to a certain extent and improve the conductivity of the composites. Consequently, the obtained Si/C@C exhibit good rate performance and cycle stability. With the optimised carbon coating thickness and calcination temperature, the obtained electrodes deliver a reversible capacity of 1120 and 683 mA h g -1 at a current density of 0.1 and 2 A g -1 respectively, and a specific capacity of 602 mAh∙g -1 at a current density of 1 A g -1 after 100 cycles, a capacity retention rate of 80%. The facilely synthesised Si/C@C composite shows potential applications in high-capacity silicon-based anode materials .

CAS / MDL: 25249-54-1 9003-39-8
研究领域: 材料科学 · 电化学
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