APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Yali Liu,Fanglongwen Xu,Chen Wang,Xiaofei Cao,Jiarui Cheng,Zilong Zeng,Hao Yao,Youlong Xu
The application of lithium-metal batteries (LMBs) has been hindered by dendritic deposition, low coulomb efficiency (CE) and significant volume changes during repeated plating/stripping process. Herein, we developed an elastomeric quasi-solid electrolyte (QSE) through in-situ polymerization method with a tailored composition. The incorporation of difluoro(oxalato)borate (LiDFOB) facilitated the generation of a uniform lithium deposition morphology and significantly enhanced the CE of LMB. Remarkably, the Li/Cu cell exhibited a high CE of 98.33 % compared to the battery without LiDFOB (97.09 %). Moreover, the Li/Li symmetric cell demonstrated long-term cycling stability about 600 h at 0.3 mA cm −2 for 0.3 mAh cm −2 . The Li/LiFePO 4 (LFP) cell displayed an initial discharge capacity of 144.2 mAh g −1 at 1 C, with a capacity retention of 98.54 % after 400 cycles. Additionally, the average CE over 400 cycles was improved to 99.93 %. Density functional theory (DFT) calculations revealed that Slab-DFOB − -Li + has a lower binding energy, enabling LiDFOB to preferentially absorb and react on the lithium metal surface, thereby facilitating smooth and dendrite-free lithium deposition. The incorporation of functional LiDFOB into elastomeric QSE effectively enhances the electrochemical performance of LMBs. The compatible modification strategy provides a new perspective for improving the performance of elastomeric electrolytes.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
IONICS
·
2024
·
IF 2.4
Liu Liyang,Zhao Xufan,Qi Jiaxing,Abdussalam Abubakar,Zhang Wei,Wang Hongyu,Xu Guobao
Since the concept of hybrid Li/Na-ion batteries (HLNIBs) was proposed, many cathode materials with excellent performance and low cost have been studied. However, in HLNIBs, mixed cationic electrolyte is formed as Na + is extracted from the cathode, resulting in relatively complicated and unstable electrochemical performance, especially for the half-cell test with lithium metal as the anode. It is necessary to consider the tolerance of lithium metal counter electrode to sodium contamination in half-cell test with hybrid-ion electrolyte containing different cations. In this work, we have found that lithium metal electrodes in hybrid-ion electrolyte are unstable and Na + causes significant polarization. The polarization influences over potential and complex interface properties and thus reduces the accuracy of half-cell tests. To solve the problem, lithium difluoro(oxalato)borate (LiDFOB) with excellent film-forming properties was utilized as an additive of symmetrical batteries to form solid electrolyte interface (SEI) film. The adverse effect of Na + on the kinetics of hybrid-ion electrolyte was confirmed by regulating the SEI film on lithium metal electrode. The SEI film exhibits a selective effect on Li + and Na + and inhibits the interfacial transport of Na + , which significantly reduces the overpotential of the batteries and the interface migration impedance and also improves the stability of lithium counter electrode. Lithium metal with stable interfacial properties in the presence of LiDFOB is a reliable counter electrode that resists sodium contamination in half-cell test. Graphical abstract
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·Vol. 30
·期 39
·e202400803
·
IF 3.9
Kang Wang,Song Gao,Li Li,Liying Wang,Xijia Yang,Xuesong Li,Wei Lü
To meet the demand for higher energy density in lithium-ion batteries and expand their application range, coupling lithium metal anodes with high-voltage cathodes is an ideal solution. However, the compatibility between lithium metal batteries and electrolytes affects their applicability. In this study, proposes a locally concentrated electrolyte based on ethyl acetate (EA) as the solvent, lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) as the lithium salt, and lithium difluorooxoborate (LiDFOB) as a sacrificial agent to enhance the low-temperature and high-voltage endurance of Li//Lithium cobalt oxide (LCO) batteries. The Li//LCO battery can operate within the voltage range of 3 to 4.5 V, with an initial discharge specific capacity of 174.5 mAh g −1 at 20 °C. At −40 °C, after 200 cycles, the capacity retention rate is 87.7 %. It can operate under extreme conditions of −70 °C, with a discharge specific capacity of 112.6 mAh g −1 . Additionally, LCO//HC batteries using this electrolyte demonstrate excellent performance. Present work provides a new perspective for the optimization of electrolytes for low-temperature lithium-ion batteries. Graphical Adjusting the solvent structure and reducing the desolvation energy enables the electrolyte to withstand high voltages and low temperatures. Li//LCO and HC//LCO batteries using this electrolyte can still operate within the voltage range of 3.0 to 4.5 V at −40 °C, exhibiting high discharge specific capacities and long cycling performance.
研究领域:
电化学
·
储能
·
材料科学
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电池技术
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 15
·8308-8319
·
IF 11.9
Yali Liu,Youlong Xu,Jing Wang,Yao Niu,Xiangdong Ding
Elastomeric electrolytes exhibit attractive benefits in lithium-metal batteries due to the accommodation of volume changes during the lithium metal plating and stripping processes. However, their narrow oxidation potential restricts their application in high-energy batteries. Herein, an improved high-voltage elastomeric quasi-solid electrolyte (QSE) was fabricated through in situ polymerization by incorporating lithium difluoro(oxalate)borate (LiDFOB). LiDFOB could preferentially react at the cathode side to form an enhanced LiF-rich cathode electrolyte interphase (CEI) before the decomposition of the bulk electrolyte. Moreover, the crosslinked oligomeric borates (B–O), LiF and B–F-containing solid electrolyte interphase (SEI) possibly guide the formation of a uniform morphology after lithium deposition. Benefitting from the dual-stabilized effect of LiDFOB, the as-designed QSE exhibited a significantly improved electrochemical window of 5.36 V compared with the initial 4.6 V, as revealed by the linear sweep voltammetry (LSV) results. In particular, the Li/LiVPO4F cell with a high cut-off voltage of 4.7 V displayed a discharge capacity of 121.5 mA h g−1 with a capacity retention of ∼84.03% after 100 cycles. Density functional theory (DFT) calculations further reveal that LiDFOB is critical to fabricating LiF-rich CEI and uniform lithium deposition. The compatible modification strategy employed in this work for the in situ formed elastomeric QSE gives new insights into improving the performance of elastomeric electrolytes.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Energy Storage Materials
·
2022
·
IF 20.831
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
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2019
·
IF 0
Qingyu Dong,Feng Guo,Zhenjie Cheng,Yayun Mao,Rong Huang,Fangsen Li,Houcai Dong,Qingyong Zhang,Wei Li,Hui Chen,Zhaojun Luo,Yanbin Shen,Xiaodong Wu,Liwei Chen
Ni-rich layered oxides (LiNixMnyCozO2, x ≥ 0.6, x + y + z = 1) are promising positive electrode materials for high energy density lithium-ion batteries thanks to their high specific capacity. However, large-scale application of Ni-rich layered oxides is hindered by its poor structural and interfacial stability, especially during cycling at a high cutoff potential (i.e., ≥ 4.3 V, versus Li+/Li). Herein, we demonstrate that lithium difluoro(oxalato)borate (LiDFOB) as a film-forming additive plays a dual role on the electrode|electrolyte interphase formation in a LiNi0.83Mn0.05Co0.12O2||graphite cell, meaning that it can not only be reduced on the graphite negative electrode but also oxidized on the nickel-rich oxide LiNi0.83Mn0.05Co0.12O2 positive electrode cycled at a high cutoff potential (4.4 V, versus Li+/Li) prior to typical carbonate-based electrolyte constituents. As a result, the addition of 1.5 wt % LiDFOB greatly reduces the polarization and improves the cycling stability of the LiNi0.83Mn0.05Co0.12O2||graphite cell, which shows a high discharge capacity of 198 mA h g–1, and more than 83.1% of the initial capacity was retained after 200 cycles at C/3 (the capacity retention obtained at the same cycling condition is only 59.9% for the cell without LiDFOB additive). Furthermore, the employ of LiDFOB additive also significantly suppresses the self-discharge of the LiNi0.83Mn0.05Co0.12O2||Li cell during high-temperature and long-term room-temperature storage at 4.4 V. These electrochemical performance enhancements could be attributed to the participation of LiDFOB in forming a stable and Li+ transfer favorable protective layer that is rich in inorganic boron, fluorine, and carbonate compounds on both the surface of the LiNi0.83Mn0.05Co0.12O2 positive electrode and the graphite negative electrode, thus suppressing the electrolyte decomposition on the positive electrode and negative electrode surfaces and decreasing the dissolution of transition-metal ions from the positive electrode bulk.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Qiujun Wang,Nana Bai,Yelun Xin,Xiaomeng Fan,Di Zhang,Zhaojin Li,Qujiang Sun,Huilan Sun,Bo Wang,Guoxu Wang,Li-Zhen Fan
LiCoO 2 (LCO) is a prominent high-voltage cathode material due to its exceptional energy density and impressive theoretical specific capacity of 274 mAh g −1 . However, challenges such as irreversible structural phase transitions, loss of reactive oxygen, and cobalt dissolution can lead to unstable interfaces between the electrolyte and the LCO cathode. In this study, sulfolane (SUL)-based composite polymer electrolytes (CPEs) were synthesized through in-situ polymerization, and the LCO cathode was modified using vinylidene carbonate (VC) and lithium difluoro(oxalato)borate (LiDFOB). The synergistic effects of SUL and VC/LiDFOB facilitated the formation of a more stable cathode-electrolyte interface (CEI) layer. Consequently, the Li/EFHTL-15 %SUL/LCO-VC-LiDFOB cell demonstrated excellent reversible cycling performance, achieving 86.36 % capacity retention after 300 cycles at 0.5C within a voltage range of 2.8–4.4 V at 25 ℃. This work provides a viable approach for enhancing the interface stability of the LCO cathode in CPEs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
Chen Jia,Yong-Feng Shen,Miao Wang,Wen-cui Li
The cathodic pre-lithiation process, currently considered the most feasible resolution to address the irreversible depletion of Li + in dual carbon-based lithium-ion capacitors (LICs), encounters obstacles in widespread adoption due to its substantial dosage requirement, rising decomposition potential and the damage related to its decomposition residues. Hence, in this study, the successful utilization of Li 2 NiO 2 for LIC pre-lithiation is accomplished, leveraging the synergistic effect between Li 2 NiO 2 and lithium difluoro oxalate borate (LiDFOB). It's noteworthy that the full capacitor, entirely composed of commercial materials (activated carbon/hard carbon) and supplemented with 20 wt% LNO +2 wt% LiDFOB, exhibits remarkable energy densities of 98.53 Wh kg −1 at a power density of 31 W kg −1 and 19 Wh kg −1 at a power density of 4.65 kW kg −1 . Moreover, the full capacitor displays commendable performance, demonstrating superior capacitive behavior and excellent high-current cycling proficiency. Besides, electrochemical evaluations and structural analyses unveil that LiDFOB, via solid electrolyte interface (SEI) modification, enhances the utilization of Li + sourced from Li 2 NiO 2 thus avoiding the abuse of pre-lithiation reagents, while the LNO decomposition products contribute substantially to additional capacitance. The synergistic effect of pre-lithiation reagent and SEI modification underpin the outstanding performance witnessed in the full capacitor.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·Vol. 34
·期 19
·2313146
·
IF 18.5
Fengchun Li,Xin Gu,Akang Cui,Yang Li,Sijin Dong,Shuang Wu,Zhenjie Cheng,Qian Yao,Jian Yang,Mingbo Wu
Manganese-based layered oxide cathodes, particularly K x MnO 2 (KMO), have shown great potential in potassium-ion batteries (PIBs) due to their low cost, high theoretical capacities, and excellent thermal stability. However, Jahn-Teller distortion, manganese dissolution, and interface instability of electrode/electrolyte lead to structural instability and performance decay. Here, lithium difluoro(oxalate) borate (LiDFOB) is introduced as an electrolyte additive to improve the electrochemical performance of P3-type KMO. LiDFOB creates a uniform, thin, and robust cathode-electrolyte interphase layer on the cathode surface, enhancing reaction kinetics, preventing manganese dissolution, and stabilizing the structure. The P3-KMO cathode with LiDFOB in the basic electrolyte exhibits significantly improved electrochemical performance, such as a remarkable Coulombic efficiency of ≈99.5% and high capacity retention of 78.6% after 300 cycles at 100 mA g −1 . Moreover, the full cell of P3-KMO||soft carbon demonstrates satisfactory specific capacity and energy density. This study emphasizes the importance of interface chemistry for PIBs.
研究领域:
电化学
·
储能
·
材料科学
·
电池技术
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yongquan Zhang,Jingrun Hu,Jingshun Wang,Sen Wang,Cheng Wan,Yue Zhang,Tiandong Zhang,Changhai Zhang,Qingguo Chi
Solid-state electrolytes face significant challenges in concurrently optimizing mechanical strength and ionic conductivity. To address this issue, a two-step synthesis strategy was employed to construct a hierarchical mesh-interpenetrating network composite electrolyte. The electrolyte contained self-crosslinking networks formed by the reaction of epoxy resin polyethylene glycol diglycidyl ether (PEGDE) catalyzed by lithium difluoro(oxalato)borate (LiDFOB), embedded within a rigid layered skeleton induced by 365 nm ultraviolet light in the liquid crystal compound 1,4-bis[4-(6-acryloyloxyhexanoyloxy)benzoyloxy]-2-methylbenzene (C6M). The independent formation and spatial interpenetration of the two network systems resulted in significant synergistic effects. The resulting PEGDE-LC composite electrolyte (designated as PLE) exhibited a room-temperature ionic conductivity of 2.61 × 10 −4 S·cm −1 , an electrochemical stability window of 4.79 V vs. Li + /Li, and a tensile strength of 4.7 MPa for the optimized PLE-3 formulation. The LFP/Li battery delivered an initial discharge capacity of 153.8 mAh·g −1 at room temperature under a 1C rate, with a capacity retention of 89.6 % (137.9 mAh·g -1) after 300 cycles. This interpenetrating network structure, based on material composite synergy, provides a novel material design strategy to overcome the trade-off between mechanical and electrochemical properties in solid-state electrolytes.
研究领域:
材料科学
·
储能技术
·
电化学
·
高分子化学
·
锂离子电池
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Ran He,Kuirong Deng,Tianyu Guan,Fuhui Liang,Xiaoqiong Zheng,Maosheng Li,Daize Mo,Kai Yang,Haijiao Xie
In-situ preparation of polymer electrolytes (PEs) can enhance electrolyte/electrode interface contact and accommodate the current large-scale production line of lithium-ion batteries (LIBs). However, reactive initiators of in-situ PEs may lead to low capacity, increased impedance and poor cycling performance. Flammable and volatile monomers and plasticizers of in-situ PEs are potential safety risks for the batteries. Herein, we adopt lithium difluoro(oxalate)borate (LiDFOB)-initiated in-situ polymerization of solid-state non-volatile monomer 1,3,5-trioxane (TXE) to fabricate PEs (In-situ PTXE). Fluoroethylene carbonate (FEC) and methyl 2,2,2-trifluoroethyl carbonate (FEMC) with good fire retardance, high flash point, wide electrochemical window and high dielectric constant were introduced as plasticizers to improve ionic conductivity and flame retardant property of In-situ PTXE. Compared with previously reported in-situ PEs, In-situ PTXE exhibits distinct merits, including free of initiators, non-volatile precursors, high ionic conductivity of 3.76 × 10 −3 S cm −1 , high lithium-ion transference number of 0.76, wide electrochemical stability window (ESW) of 6.06 V, excellent electrolyte/electrode interface stability and effectively inhibition of Li dendrite growth on the lithium metal anode. The fabricated LiFePO 4 (LFP)/Li batteries with In-situ PTXE achieve significantly boosted cycle stability (capacity retention rate of 90.4% after 560 cycles) and outstanding rate capability (discharge capacity of 111.7 mAh g −1 at 3C rate).
研究领域:
材料科学
·
电化学
·
电池技术
·
聚合物化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）