CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Bin Fan,Weikun Chen,Qian He,Bigui Zhou,Zhiyun Xu,Wei Liu,Qingya Wei,Yingping Zou
To achieve the practical application of high energy density lithium–sulfur (Li–S) batteries, it is essential not only to enhance lithium-ion (Li + ) transport but also to effectively suppress the lithium polysulfides (LiPSs) shuttle effect, which remains challenge for the conventional commercial separators. In this study, a fluorinated covalent organic framework (Tp-TFAB COF) material with high selective permeability was employed to modify separators for Li–S batteries. The fluorinated Tp-TFAB COF layer can effectively enhance Li + conduction while providing electrostatic shielding against LiPSs, which were also confirmed by density functional theory calculations. As a result, Li–S batteries with Tp-TFAB/PP-modified separators retained 79.4 % of their initial capacity after 800 cycles at a 0.5C rate, with a low capacity decay of 0.026 % per cycle. Even at a high sulfur loading (7.3 mg cm −2 ), the batteries exhibited an impressive areal capacity of 5.83 mAh cm −2 . This work highlights the selective functionality of the fluorinated COFs nanoscopic channels, demonstrating its potential for applications in energy storage and beyond.
研究领域:
材料科学
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电化学
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能源存储
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DOI
高影响因子
ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Tao Huang,Yongwei Chen,Xiangzhen Zheng,Ying Pan,Maoxiang Wu
Layered lithium-rich oxides(LRO) materials have garnered significant attention due to their high reversible capacity and broad operating voltage range. However, the practical application of LRO materials is still restricted by the serious interfacial instability and surface structure reconstruction during long-term cyclic test. In this study, we use 2-(Trimethoxysilyl)ethyl methacrylate (TSM) as a multifunctional electrolyte additive to enhance the electrochemical performance of the Li/LRO cell. The capacity retention of the Li/LRO cell improves significantly from 67.2 % to 85.8 % after 100 cycles at 0.5C (1C = 300 mAh g -1 ) between 2.0 and 4.8 V with the addition of 2 % TSM. Under harsh conditions (with the addition of 1000 ppm H 2 O to the electrolytes), Li/LRO cell with TSM additives maintains the capacity retention of 82.5 % after 100 cycles, which is significantly higher than the cell without additives (38.0 %). Both theoretical calculations and experiments results demonstrate that TSM exhibits higher oxidation activity than the solvents, forming a uniform cathode electrolyte interphase (CEI) on the LRO surface. The TSM-derived CEI layer effectively mitigates the interfacial parasitic reactions and prevents structural degradation of LRO. Furthermore, theoretical calculations and nuclear magnetic resonance (NMR) results confirm that TSM effectively eliminates water (H 2 O) and hydrofluoric acid (HF), mitigating their adverse effects.
研究领域:
材料科学
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电化学
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能量存储
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纳米技术
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表面化学
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DOI
高影响因子
ChemSusChem
·
2024
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IF 7.5
Dan Li,Qian Chen,Rui Li,Yaolin Hou,Yulong Liu,Haiming Xie,Jia Liu,Jiefang Zhu
Graphical The incorporation of the polyionic liquid additive [PBVIm]-TFSI in LiI-mediated Li-O 2 batteries enables the in situ formation of a protective layer on the Li anode. [PBVIm] + cations migrate to the Li anode, forming a cationic shield that promotes uniform Li + deposition. A [PBVIm][TFSI]-containing cell demonstrates a considerable reversibility and cycling stability. Redox mediators (RMs) have shown promise in enhancing Li-O 2 battery cycling stability by reducing overpotential. However, their application is hindered by the shuttle effect, leading to RM loss and Li anode corrosion. Here, we introduce a polyionic liquid, poly (1-Butyl-3-vinylimidazolium bis(trifluoromethanesulfonylimine)) ([PBVIm]-TFSI) as an additive, showcasing a novel Li anode protection strategy for LiI-mediated Li-O 2 batteries. [PBVIm] + cations migrate to the Li anode, forming a protective cationic shield that promotes uniform Li + deposition. The addition of [PBVIm]-TFSI enhances the cycling stability, achieving 105 cycles at 200 mA⋅g −1 , compared to the cell with LiI which exhibited 38 cycles under the same conditions. Synchrotron X-ray tomography reveals the evolution of this protective layer, providing insights into its formation mechanism, in conjunction with XPS analysis. Our findings offer a new approach to Li anode protection in Li-O 2 batteries, emphasizing the critical role of interfacial engineering for battery performance.
研究领域:
材料科学
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电化学
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能源存储
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产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2024
·Vol. 48
·期 27
·12199-12208
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IF 2.7
Shaowei Wang,Zesen Gao,Futing Sun,Yan Yang,Lang Tao,Yunluo Wang,Zhiqian Yu,Jianghua Wu,Jingshan Hou,Zhanqiang Liu,Hucheng Song,Haijie Chen
Safety concerns associated with lithium batteries suggest the development of solid-state batteries as a promising variant. In this work, we doped a lithium boracite (Li4B7O12Cl) with Mg2+ to modify the Li+ sites and observed significant improvement in ionic conductivity by two orders of magnitude (from 3.03 × 10−7 S cm−1 to 2.81 × 10−5 S cm−1 at room temperature). We attribute the enhanced ion conductivity to the artificially induced Li vacancies resulting from Mg doping. The as-fabricated symmetrical battery (Li|Li3.6Mg0.2B7O12Cl|Li) exhibited good cycling performance with a stable voltage output even after 60 hours of cycling. The battery showed a coulombic efficiency retention of ∼99.7% after the cycling test. Our work demonstrates that Li4B7O12Cl is a superior solid electrolyte for solid-state batteries and the introduction of Li vacancies can be an efficient approach to greatly improve the ionic conductivity of other electrolytes.
研究领域:
材料科学
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电化学
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电池技术
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Jiahui Zhou,Man Xie,Feng Wu,Guangling Wei,Yang Mei,Ruling Huang,Guoqiang Tan,Li Li,Renjie Chen
Great efforts have been made to optimize Li metal anodes to improve energy density and cycle life. However, challenges remain in achieving uniform Li plating/stripping while maintaining stable interphase chemistry. Here, an engineered graphene aerogel with uniformly oriented microscale channels, and normalized lithiophilic binding sites as hosted Li anodes is reported. Vertically aligned graphene with oriented channels are constructed using a freeze-drying mechanism, and highly lithiophilic binding sites are optimized by adjusting functional oxygen anions on graphene. Based on the in-situ optical microscopy visualization and first-principles calculations, this graphene host design presents homogeneous Li-ion nucleation owing to its straight transport channels with ultrahigh lithiophilicity, resulting in greatly improved cycling stability. Also, the flat and compatible electrode–electrolyte interphase facilitates smooth Li growth, thereby suppressing the formation of dendrites. Notably, the symmetric cells using the new composite anodes exhibit superior electrochemical reversibility over 500 cycles, with the patternable LiFePO 4 //Li@graphene pouch cells displaying outstanding cycling performance. This graphene-hosted Li anode thus demonstrates great potential for Li batteries.
研究领域:
材料科学
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电化学
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能源存储
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DOI
高影响因子
Nature Energy
·
2018
·Vol. 3
·期 8
·674-681
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IF 46.859
Zeng Ziqi,Murugesan Vijayakumar,Han Kee Sung,Jiang Xiaoyu,Cao Yuliang,Xiao Lifen,Ai Xinping,Yang Hanxi,Zhang Ji-Guang,Sushko Maria L.,Liu Jun
Non-flammable electrolytes could intrinsically eliminate fire hazards and improve battery safety, but their compatibility with electrode materials, especially graphite anodes, remains an obstacle owing to the strong catalytic activity of the anode surfaces. Here, we report an approach that improves the stability of non-flammable phosphate electrolytes by adjusting the molar ratio of Li salt to solvent. At a high Li salt-to-solvent molar ratio (~1:2), the phosphate solvent molecules are mostly coordinated with the Li + cations, and the undesired reactivity of the solvent molecules toward the graphite anode can be effectively suppressed. High cycling Coulombic efficiency (99.7%), good cycle life and safe operation of commercial 18650 Li-ion cells with these electrolytes are demonstrated. In addition, these non-flammable electrolytes show reduced reactivity toward Li-metal electrodes. Non-dendritic Li-metal plating and stripping in Li–Cu half-cells are demonstrated with high Coulombic efficiency (>99%) and good stability.
研究领域:
材料科学
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电化学
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电池技术
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产品关联
DOI
高影响因子
ACS Applied Energy Materials
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2019
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IF 0
Tiancun Liu,Jiulin Hu,Chilin Li,Yong Wang
Li metal anode is deemed the most promising candidate anode for high-energy battery systems such as Li-sulfur and Li-fluoride batteries. However, some severe challenges, for example, facile formation and growth of Li dendrites, large volume evolution of hostless Li ,and low Coulombic efficiency of Li plating/stripping, still hinder the commercialization of Li-metal batteries (LMBs). Herein, a free-standing and highly flexible 3D current collector made of carbon nanofibers (CNFs) conformally coated by continuous Sn layer is synthesized by electrospinning method. Sn layer enables a lithiophilic and alloyable carbon skeleton surface and provides uniform and continuous Li nucleation sites, leading to unusual conformal Li plating behavior and effective inhibition of Li dendrites. The spatial confinement of Li plating mitigates the volume expansion and network distortion of CNFs. The electric contact reinforced by Sn interlayer achieves highly reversible Li stripping for more than 850 h for CNF-Sn@Li symmetric cell. The small nucleation overpotential (28 mV) and potential polarization (14 mV for symmetric cell) benefit from the low energy barrier of Li–Sn alloying and following Li nucleation on Li–Sn layer. For CNF-Sn@Li-LiFePO4 full cell, the capacity retention ratio is as high as 92.2% after 150 cycles at 0. 5C and the reversible capacities are maintained at 134.3 and 106.7 mAh g–1 at 2C and 5C respectively. The design of 3D lithiophilic current collector instead of planar Cu is a potential solution to highly safe LMBs.
研究领域:
材料科学
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能源存储
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产品关联
DOI
ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Lei Fu,Chao Zou,Yun Huang,Xinyan Xiang,Jie Xiao,Wenping Zeng,Xing Li,Mingshan Wang,Bingshu Guo,Yuanhua Lin
Multifunctional modified separators have the potential to effectively regulate Li ion deposition, suppress the growth of dendrite and improve the safety of lithium metal batteries (LMBs). Here, we designed a separator, constructed by co-deposition of polydopamine (PDA) and polyethyleneimine (PEI) on PP separator. Due to the introduction of polar functional groups such as amine groups, PDA/PEI-3 modified separator exhibits better electrolyte wettability, higher Li ion migration number (0.9), lower energy barrier and faster ion transfer kinetics. Electrochemical tests prove that PDA/PEI-3 modified separator has achieved better cycling stability at different current density in Li//Li symmetric cells and higher CE in Li//Cu cells. Meanwhile, the Li/LFP full cells show more excellent rate performance and long cycle performance (80%). SEM and XPS also prove that modified separator has achieved homogenized Li ions flux and more uniform LiF-rich SEI layer. This work provides a simple and effective strategy for functional separator to protect Li metal anode and improve safety performance of LMBs.
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DOI
高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 37
·20174-20186
·
IF 11.9
Guoqiang Zhao,Changwei Luo,Qingsong Hua
Battery systems based on garnet-type solid electrolytes and Li metal anodes coupled with high-specific-capacity cathodes are expected to be the most promising high-energy density solid-state lithium-ion batteries. However, the low critical current density of garnet-type solid electrolytes and their high interface resistance have been the main challenges facing these materials in the application of solid-state batteries. Herein, a low-melting-point metal chloride coating combined with in situ lithiation addresses the key issues of interface contact and growth of Li dendrites. BiCl3 with fluid properties can serve as an “aqueous” interlayer, in situ constructing a 3D cross-linked Li+ selective transport network for Li+ transfer (BiLi3) and electron blockage (LiCl) via thermal lithiation. Consequently, Li/Li symmetric cells can charge/discharge dendrite-free at a high current density of 10.0 mA cm−2 and stably cycle at 2.5 mA cm−2 for over 1000 h at room temperature. The Li metal full cells with coated garnet solid electrolyte and LiFePO4 cathode exhibit a 105.5 mA h g−1 residual capacity at a rate of 4C and 138.8 mA h g−1 reversible capacity at 1C after 600 cycles. This innovative modification strategy laid the groundwork for future commercial applications of garnet-type solid electrolytes.
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产品关联
DOI
高影响因子
Materials Today Physics
·
2021
·
IF 9.298
Y. Wu,D. Lei,C. Wang
Lithium metal has been regarded as an ideal anode to meet the rapidly growing requirements on high energy density batteries , owing to their highest gravimetric capacity and their lowest redox potential . However, lithium metal batteries persistently suffer from serious issues, such as the unstable solid electrolyte layer and uncontrolled dendrite growth during plating/stripping, especially under high current density . Herein, we developed an innovative method to prepare dense LiAl 5 O 8 nanowires membrane and designed a LiAl 5 O 8 nanowires membrane/poly (vinylidene fluoride-co-hexafluoropropylene)-based gel polymer composite electrolyte (LPH-GPE) to address these issues. On the interface of LPH-GPE and lithium anode, uniformly dispersed aluminum is in situ generated by reducing LiAl 5 O 8 nanowires, which brings both superlithiophilic sites and uniform lithium ion flux, and thus enables the lithium ion depositing in plates rather than forming sharp lithium dendrites . The solid-state lithium/lithium symmetric cells with LPH-GPE exhibit significantly improved lifespan at 0.5 mA cm − 2 and short-circuit does not occur even at current density up to 4 mA cm − 2 .
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Xiyuan Tao,Li Yang,Jiali Liu,Zihao Zang,Peng Zeng,Changfei Zou,Lingguang Yi,Xiaoyi Chen,Xiaolin Liu,Xianyou Wang
Garnet-type Li 7 La 3 Zr 2 O 12 (LLZO) is a promising solid-state electrolyte (SSE) for next generation lithium batteries due to its high Li + conductivity and stability against lithium metal, especially the Li 7−3x Ga x La 3 Zr 2 O 12 (Ga-LLZO) is most valuable because of its high ionic conductivity (> 1 ×10 −3 S cm −1 ). However, it is difficult to prepare high-quality Ga-LLZO by the traditional air ambient sintering. Herein, we develop a simple and efficient rapid ultra-high-temperature sintering (RUHTS) method to prepare high-conductivity Ga-LLZO ceramic SSE. It has been found that the as-prepared Ga-LLZO ceramic SSE with the composition of Li 6.25 Ga 0.25 La 3 Zr 2 O 12 exhibits high relative density of 99%, good ionic conductivity of 1.48 × 10 −3 S cm −1 and large critical current density of 0.5 mA cm −2 after sintering at 1200 °C for 2 min. In addition, the Ga-LLZO SSE shows good electrochemical stability and interfacial compatibility against Li metal. The assembled Li-Li symmetric cell represents a small interfacial impedance of 37 Ω cm 2 . In the same time, the Li/Ga-LLZO/LE+LMNCO full battery has a total impedance of 205 Ω cm 2 , and can deliver a first discharge capacity of 235.1 mAh g −1 at 0.5 C, and the capacity retention rate is 88.3% after 100 cycles. This indicates that the as-prepared Ga-LLZO has good application prospect in the Li-metal solid-state batteries (LMSSBs). Moreover, this method does not require the use of mother powder during preparation process, which will effectively reduce the waste of raw materials, save manufacture costs and be beneficial to quantity production of Ga-LLZO ceramic electrolyte.
研究领域:
材料科学
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电化学
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电池技术
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DOI
高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 19
·12214-12224
·
IF 10.733
Yuanzhou Yao,Xiaohui Zhao,Amir Abdul Razzaq,Yuting Gu,Xietao Yuan,Rahim Shah,Yuebin Lian,Jinxuan Lei,Qiaoqiao Mu,Yong Ma,Yang Peng,Zhao Deng,Zhongfan Liu
The passivation of lithium metal anodes to mitigate an unstable solid electrolyte interface and parasitic dendrite growth is the key premise for their successful implementation in lithium metal batteries. Herein, aiming to simultaneously reduce the interfacial resistance and to suppress lithium dendrites, we coated lithium metal anodes with two-dimensional (2D) rGO layers prepared via a solvent-evaporation-assisted self-assembly. Upon lithiation/delithiation, the rGO coating cracked into mosaic-like flakes, in between which the interconnected gaps served as the passage for uniform lithium plating/stripping. Half cells composed of a sandwich Cu/Li/rGO electrode vs. Cu foils revealed much improved Li usage and coulombic efficiencies. Through ex situ SEM imaging and XPS depth profiling, a comprehensive view of Li intercalation, deposition, and dendrite suppression on the rGO coating was obtained. As a result of the improved kinetics of Li transportation, excellent electrochemical performances were demonstrated in symmetric gLi‖gLi cells with a stabilized overpotential of only 87.9 mV at 5 mA cm−2 over 600 cycles, and in Li–S batteries with a stabilized capacity of 1200 mA h g−1 at 1C near 1000 cycles.
研究领域:
材料科学
·
电化学
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电池技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）