Inorganics
·
2025
·Vol. 13
·期 4
·115
·
IF 3
Yinan Liu,Wei Jiang,Congcong Zhang,Pingshan Jia,Zhiyuan Zhang,Yun Zheng,Kunye Yan,Jun Wang,Yunxian Qian,Junpo Guo,Rong Chen,Yike Huang,Yingying Shen,Lifen Long,Bang Zheng,Huaiyu Shao
Pre-lithiation using Li–Si alloy-type additives is a promising technical approach to address the drawbacks of Si-based anodes, such as a low initial Coulombic efficiency (ICE) and inevitable capacity decay during cycling. However, its commercial application is limited by the air sensitivity of the highly reactive Li–Si alloys, which demands improved environmental stability. In this work, a protective membrane is constructed on Li13Si4alloys using low-surface-energy paraffin and highly conductive carbon nanotubes through liquid-phase deposition, exhibiting enhanced hydrophobicity and improved Li+/e−conductivity. The Li13Si4@Paraffin/carbon nanotubes (Li13Si4@P-CNTs) composite achieves a high pre-lithiation capacity of 970 mAh g−1and superb environmental stability, retaining 92.2% capacity after exposure to ambient air with 45% relative humidity. DFT calculations and in situ XRD measurements reveal that the paraffin-dominated coating membrane, featuring weak dipole–dipole interactions with water molecules, effectively reduces the moisture-induced oxidation kinetics of Li13Si4@P-CNTs in air. Electrochemical kinetic analysis and XPS depth profiling reveal the enhancement in charge transfer dynamics and surface Li+transport kinetics (SEI rich in inorganic lithium salts) in P-SiO@C pre-lithiated by Li13Si4@P-CNTs pre-lithiation additives. Benefitting from pre-lithiation via Li13Si4@P-CNTs, the pre-lithiated SiO@C(P-SiO@C) delivers high ICE (103.7%), stable cycling performance (981 mAh g−1at 200 cycles) and superior rate performance (474.5 mAh g−1at 3C) in a half-cell system. The LFP||P-Gr pouch-type full cell exhibits a capacity retention of 83.2% (2500 cycles) and an energy density of 381 Wh kg−1after 2500 cycles. The Li13Si4@P-CNTs additives provide valuable design concepts for the development of pre-lithiation materials.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Xiang Li,Li Wang,Zhengguo Gu,Xuanhao Wu,Feiyue Tu,Naiwen Liang,Xiaofan Liu,Wenqing Ma,Zhongchang Wang,Lezhi Yang,Lishan Yang
The prelithiated SiO x anode showcases markedly improved Li-storage capabilities compared to its unlithiated counterparts, yet it faces hurdles such as slurry gassing, electrolyte deterioration, and capacity fade attributed to residual alkali and an unstable electrolyte/anode interface. To tackle these challenges, we propose a strategic utilization of residual alkali by creating an in-situ γ -LiAlO 2 functional layer on the prelithiated SiO x @C anode material. This is accomplished by incorporating a minor amount of Al 2 O 3 into the SiO x @C/LiH precursor mixture before the solid-phase prelithiation process. The resulting modified prelithiated SiO x @C anode with in-situ formed electrolyte-isolating γ -LiAlO 2 layer exhibits no discernible slurry gas generation within 7 days and substantially mitigates side reactions with the electrolyte, thereby boosting the initial coulombic efficiency and cycling stability of the SiO x @C anode. In half-cell evaluations, the prelithiated SiO x @C anode demonstrates a high Li-storage capacity of 1323 mAh g −1 and an impressive initial coulombic efficiency of 91.09%. When assessed in a 3.2 Ah 18650 cylindrical battery, the prelithiated SiO x @C anode showcases exceptional cyclability, retaining 81% of its capacity after 1000 cycles, underscoring its potential for practical applications. This study introduces a scalable and cost-effective prelithiation technique that propels the development and practical deployment of Si-based anodes by resolving persistent scientific challenges with the use of inexpensive additives.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Liewu Li,Xiaoyu Gong,Chufang Chen,Zhencheng Huang,Weibin Chen,Qianqian Jiang,Jing Chen,Jionghui Wang,Liqing He,Tengfei Cheng,Hongbin Wang,Shenghua Ye,Xuming Yang,Xiangzhong Ren,Xiaoping Ouyang,Jianhong Liu,Qianling Zhang,Jiangtao Hu
The high specific capacity and safety nature of silicon (Si) anode has garnered significant attention and investment for its application in high-energy-density lithium-ion batteries (LIBs). However, the Si anode exhibits low initial Coulombic Efficiency (CE) and compromised cycle stability due to interfacial side reactions and the volume expansion of Si particles. Here, a straightforward strategy is proposed to prelithiate Si anodes and enhance the cycle stability by utilizing a lithium carbide (LiC 6 ) coated separator. By incorporating a LiC 6 prelithiation agent-coated PP/PE separator (PP/PE@LiC 6 ), a robust interaction between PP/PE@LiC 6 and Si anode forms during cycling, which significantly reduces subsequent contact between the electrolyte and Si particles, thereby minimizing excessive electrolyte decomposition during cycling, and facilitates the compact expansion of the Si electrode. In Si|PP/PE@LiC 6 |Li cell, the initial CE reaches 108.51%, showcasing enhanced electrochemical stability (77.93% after 100 cycles). Moreover, the Si|PP/PE@LiC 6 |LiFePO 4 cell also exhibits exceptional initial CE of ≈93.02% and improved electrochemical stability (100.94% after 100 cycles at 0.33C). This study introduces a secure and readily attainable prelithiation method for industrial applications of high-energy density Si-based batteries.
研究领域:
材料科学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Miao Bai,Liyan Yang,Qiurong Jia,Xiaoyu Tang,Yujie Liu,Helin Wang,Min Zhang,Runchen Guo,Yue Ma
Si anodes suffer from poor cycling efficiency because of the pulverization induced by volume expansion, lithium trapping in Li–Si alloys, and unfavorable interfacial side reactions with the electrolyte; the comprehensive consideration of the Si anode design is required for their practical deployment. In this article, we develop a cabbage-inspired graphite scaffold to accommodate the volume expansion of silicon particles in interplanar spacing. With further interfacial modification and prelithiation processing, the Si@G/C anode with an areal capacity of 4.4 mA h cm–2 delivers highly reversible cycling at 0.5 C (Coulombic efficiency of 99.9%) and a mitigated volume expansion of 23%. Furthermore, we scale up the synthetic strategy by producing 10 kg of the Si@G/C composite in the pilot line and pair this anode with a LiNi0.8Co0.1Mn0.1O2 cathode in a 1 A h pouch-type cell. The full-cell prototype realizes a robust cyclability over 500 cycles (88% capacity retention) and an energy density of 301.3 W h kg–1 at 0.5 C. Considering the scalable fabrication protocol, holistic electrode formulation design, and harmony integration of key metrics evaluated both in half-cell and full-cell tests, the reversible cycling of the prelithiated silicon species in the graphite scaffold of the composite could enable feasible use of the composite anode in high-energy density lithium batteries.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2024
·Vol. 35
·期 14
·1-13
·
IF 2.8
Hou Chunping,Yue Zeyu,Sun Hehang,Zhai Lidong,Xie Haidong,Tian Hui,Qu Yuqing,Wang Xinwei,Hou Jiao
Silicon oxide (SiO x ) anode materials have gained significant attention in lithium-ion batteries due to their high theoretical specific capacity (above 1965 mAh g −1 ), relatively stable cycling performance, and lower production costs. However, SiO x anode materials tend to form a solid electrolyte interphase (SEI) film and generate inert substances like Li 2 O and Li 4 SiO 4 during the initial charge and discharge processes, leading to the consumption of active lithium ions and low initial coulombic efficiency. To address these issues effectively, prelithiation of SiO x anode materials is explored in this study. A lithium powder suspension is prepared by dispersing lithium powder and carbon nanotubes (CNTs) in the electrolyte, served as the prelithiation agent. The SiO/G@C@A anode material is then prelithiated with this agent. The lithium powder suspension prelithiation agent enables effective prelithiation of the anode material. The SiO@C@A-1 anode exhibits improved electrochemical performances. At a current density of 0.1 A g −1 , the initial specific capacity reaches 981.3 mAh g −1 with an initial coulombic efficiency of 95.65%, which is approximately 25% higher than that of the untreated sample. After 100 cycles and at a current density of 0.5 A g −1 , the prelithiated sample retains a discharge specific capacity of 648 mAh g −1 , with a capacity retention rate of 83.27%, around 10% higher than that of the untreated sample, demonstrating excellent cycling performances.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
Cuilian Liu,Hongzhang Zhang,Tianyu Li,Wei Liu,Chao Qu,Xiaofei Yang,Xianfeng Li
Prelithiation is a highly attractive technique to offset the irreversible lithium loss caused by the formation of the SEI film during the first charging cycle in lithium-ion batteries. Li 3 N is an ideal prelithiation reagent due to its high theoretical specific capacity, proper decomposing potential and no residues after decomposition. However, the chemical instability of Li 3 N inevitably limits its large-scale use as prelithiation additives. Here we successfully developed a facile surface passivation method to improve the stability of Li 3 N by immersing Li 3 N in both fluoroethylene carbonate (FEC) and Vinylenecarbonate (VC) to in situ generate a coating layer on the Li 3 N surface via the spontaneous decomposition of the solvents. The coating composed of LiF, Li 2 CO 3 and lithium carbonate organics enables excellent stability of Li 3 N in the ambient environment. Remarkably, surface-passivated Li 3 N display a high prelithiation capacity of 1799 mAh/g and maintain a high capacity of 1612 mAh/g (almost 90 % of initial capacity) after exposed to humid air with 12 % relative humidity for 26 h. The effect of the compensation of lost active lithium is verified via a LiFePO 4 @ex-Li 3 N-coated//HC full cell, which exhibits not only a high capacity but also a stable cycling performance. The specific energy of LiFePO 4 @ex-Li 3 N-coated//HC full cell shows a remarkable increase compared to the LiFePO 4 //HC full cell, exhibiting ~29 % more specific energy after the 1st cycle, even Li 3 N-coated have been exposed to air with 12 % relative humidity for 26 h before use.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
NATURE
·
2024
·Vol. 628
·期 8007
·313-319
·
IF 50.5
Zhang Liangzhu,Yang Zixuan,Feng Shun,Guo Zhuobin,Jia Qingchao,Zeng Huidan,Ding Yajun,Das Pratteek,Bi Zhihong,Ma Jiaxin,Fu Yunqi,Wang Sen,Mi Jinxing,Zheng Shuanghao,Li Mingrun,Sun Dong-Ming,Kang Ning,Wu Zhong-Shuai,Cheng Hui-Ming
Transition metal tellurides (TMTs) have been ideal materials for exploring exotic properties in condensed-matter physics, chemistry and materials science 1 , 2 , 3 . Although TMT nanosheets have been produced by top-down exfoliation, their scale is below the gram level and requires a long processing time, restricting their effective application from laboratory to market 4 , 5 , 6 , 7 , 8 . We report the fast and scalable synthesis of a wide variety of MTe 2 (M = Nb, Mo, W, Ta, Ti) nanosheets by the solid lithiation of bulk MTe 2 within 10 min and their subsequent hydrolysis within seconds. Using NbTe 2 as a representative, we produced more than a hundred grams (108 g) of NbTe 2 nanosheets with 3.2 nm mean thickness, 6.2 µm mean lateral size and a high yield (>80%). Several interesting quantum phenomena, such as quantum oscillations and giant magnetoresistance, were observed that are generally restricted to highly crystalline MTe 2 nanosheets. The TMT nanosheets also perform well as electrocatalysts for lithium–oxygen batteries and electrodes for microsupercapacitors (MSCs). Moreover, this synthesis method is efficient for preparing alloyed telluride, selenide and sulfide nanosheets. Our work opens new opportunities for the universal and scalable synthesis of TMT nanosheets for exploring new quantum phenomena, potential applications and commercialization.
研究领域:
材料科学
·
凝聚态物理
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2020
·Vol. 138
·期 10
·49950
·
IF 2.52
Shuling Liu,Lingzhi Zhang
Partially lithiated ternary graft copolymers were synthesized through free radical graft polymerization of acrylic acid (AA), lithium acrylate (LiAA) and hydroxyethyl acrylate (HEA) onto polyvinyl alcohol (PVA). With optimized feeding molar ratio of AA/LiAA/HEA (2:1:2), the ternary graft copolymer with partial lithiation shows the best flexibility, elasticity and adhesion strength comparing to PVA-g-PAA and PVA-g-P(AA-HEA) when used as aqueous binder for Si anode. The Si anode using PVA-g-P(AA-LiAA-HEA) with the optimized molar ratio of AA-LiAA-HEA exhibits better cycling stability and rate performance, delivering a capacity of 2265 mAh g −1 with a capacity retention of 82.4% after 200 cycles at 1A g −1 . Even at a high current of 10 A g −1 , the Si electrode still obtained a high capacity of 1300 mAh g −1 .
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Qiyuan Zhou,Hongfeng Zhan,Bo Chen,Hai Li,Zhendong Huang,Yanwen Ma,Hua Zhang,Shaozhou Li,Xiao Huang,Wei Huang
Although ultrahigh theoretical capacity has long been predicted for boron-based lithium-ion battery anodes, experimentally, boron has exhibited only limited performance and its lithiation process remains elusive. The two-dimensional (2D) form of boron is believed to be an ideal model system to investigate the lithiation behavior of boron; however, unfortunately, most reported 2D boron structures are prone to oxidation under ambient conditions. In this contribution, through a simultaneous etching and in situ functionalization process, we synthesized for the first time methyl-functionalized boron nanosheets, which remain stable up to 250 °C. Combining experiments and theoretical calculations, we found that lithiation of boron is realized through the formation of alloys such as LiB3 and Li3B14, while alloys with higher Li content such as Li5B are thermodynamically less favored. In addition, detailed electrochemical analysis reveals that side reactions on the boron surface may also contribute to the unsatisfactory performance of boron-based electrodes. Our findings suggest that reducing the enthalpy of formation of high Li content alloys and the choice of a less nucleophilic electrolyte are key to developing high-performance anodes based on novel boron materials. Our demonstration of stable 2D boron structures also paves the way for their fundamental study and practical applications.
研究领域:
材料科学
·
电化学
·
理论计算
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Xingxin Niu,Chengdeng Wang,Wenyuan Zhang,Donghua Wang,Haofeng Shi,Lu Yu,Chong Wang,Zhihao Xiong,Zhen Ji,Yan Gao,Xiaoqin Yan
The application of silicon-based anode remains a serious challenge due to its intrinsic volumetric expansion effect and low conductivity. In our work, a novel CNT-interspersed hierarchical carbon shell structure (denoted as PDA@CoZn-NC@Si) is synthesized by wrapping Si uniformly in the bimetallic zeolite imidazolate frameworks (ZIFs) and then encapsulated with a dopamine-derived carbon shell. The PDA@CoZn-NC@Si anode delivers better cycle stability of 814 mAh/g at 0.5C for 400 cycles (only −0.14% capacity reduction per cycle) and possesses excellent rate capability, which benefits from the inner porous buffer spaces, interspersed CNT, and solid heterogeneous carbon shells. In addition, the full cell is assembled by pairing a solution-based chemically prelithiated PDA@CoZn-NC@Si anode with a Li(Ni 1/3 Co 1/3 Mn 1/3 )O 2 (NCM111) cathode, and it presents an improved initial coulombic efficiency (88.3%) and a high energy density (419.8 Wh/kg). This study provides effective guidance for optimizing the microstructure design and prelithium of Si-based anodes.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Heyang Zhou,Li Ting Gao,Yimeng Li,Yuhang Lyu,Zhan-Sheng Guo
Thick electrodes whose active materials have high areal density may improve the energy densities of lithium-ion batteries. However, the weakened rate abilities and cycle lifetimes of such electrodes significantly limit their practical applications. In this study, a modified two-dimensional model was built to evaluate the influence of the electrode structure on the lithiation process. Gradient electrodes with different particle sizes along the thickness direction are designed and fabricated via a two-layer coating process . The gradient design in the thickness direction is confirmed by three-dimensional digital microscopy , energy-dispersive spectroscopy, X-ray diffraction, and scanning electron microscopy . Galvanostatic charge/discharge cycling tests and electrochemical impedance spectroscopy are performed to investigate the electrochemical properties of the fabricated gradient electrodes. The simulation results indicate that the gradient electrode structure can enhance the utilization of electrode particles on the current collector side and alleviate the nonuniformity of the solid-phase Li concentration along the thickness direction. High electrochemical performance and long-term cycling stability of the designed gradient electrodes are verified by electrochemical test. The gradient structure fabricated via multi-layer coating processes can be used to improve the electrochemical performance of thick electrodes.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Guoqiang Zhao,Changwei Luo,Bin Wu,Mengyang Zhang,Haoqi Wang,Qingsong Hua
Unexpected interface resistance and lithium dendrite puncture hinder the application of garnet-type solid-state electrolytes in high-energy-density systems. Different from the previous high-temperature (>180 °C) molten lithium that promotes the alloying reaction between the coating layer and Li to enhance the interface contact, herein, we introduce liquid-metal-like SbCl3 to construct a three-dimensional Li+ directional-selection interlayer by in situ low-temperature lithiation (80 °C). An interlayer with a more negative interface energy composed of SbLi3 and LiCl exhibits a superior affinity with Li and LGLZO, which reduces the interface resistance and suppresses the growth of Li dendrites by an insulated electron. The introduction of the SbCl3 modification layer into Li/Li symmetric cells enables charge/discharge at a current density of 6.0 mA cm–2 and operation for more than 1000 h under 2.0 mA cm–2 at room temperature. The full cells with the LiFePO4 cathode exhibit a high residual capacity of 144.8 mAh g–1 at 0.5 C after 1000 cycles and excellent cycling stability with a retention ratio of 94.7% at 1 C after 600 cycles. The low-temperature lithiation method based on an energy-saving perspective should be applied to other types of solid-state electrolyte modification strategies.
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）