ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Zongzhe Liu,Shaobo Ma,Xue Mu,Renlong Li,Geping Yin,Pengjian Zuo
A silicon anode with ultra-high specific capacity has motivated tremendous exploration for high-energy-density lithium ion batteries while it still faces serious issues of irreversible lithium loss, unstable electrode electrolyte interface (SEI), and huge volume expansion. Prelithiation is a crucial technology to alleviate the harm of active lithium loss of silicon-based full-cell systems. Herein, we reported a cathode prelithiation method using Li2S-PAN as a lithium “donor”, which was synthesized via chemical reaction between sulfurized polyacrylonitrile and Li-biphenyl complex. The Li2S-PAN with an initial charging capacity of 668 mAh g–1 (2.5–4.0 V) is loaded on the LiFePO4 electrode, and the LiFePO4/Li2S-PAN composite electrode displays a high initial charge capacity of 206 mAh g–1, which is 22.3% higher than the pristine LiFePO4. With a silicon/graphite/carbon (Si/G/C) composite anode, the Si/G/C||LiFePO4/Li2S-PAN full cell exhibits a reversible capacity of 123 and 107 mAh g–1 in the 1st and 10th cycle, which is 15.5 and 24.5% higher than the Si/G/C||LiFePO4 battery, respectively. The SEI layer of the silicon anode in the Si/G/C||LiFePO4/Li2S-PAN cell contains abundant conductive LiF species, which can enhance the interfacial stability and reaction kinetics of the cells. The proposed cathode prelithiation process is compatible with the industrial roll-to-roll electrode preparation process, exhibiting a promising application prospect.
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
Science China-Chemistry
·
2025
·
IF 9.7
Liang Haoyue,Zhong Xingguo,Huang Guxin,Liu Wenpan,Liu Yao,Wang Shuhao,Wang Deyu,Liu Hao,Wang Hao,Zhai Tianyou,Li Huiqiao
Li 3 VO 4 has been a promising insertion anode material for Li-ion batteries, which has high theoretical capacity (up to ∼600 mAh g −1 ) and safe Li insertion voltage (0.5–1 V vs. Li/Li + ). However, the low initial Coulombic efficiency (ICE) has always been the bottleneck limiting its commercialisation. Here, we propose a facile pre-lithiation method to controllably elevate the ICE by the post-treatment of the prepared Li 3 VO 4 composite electrode based on an immersion reaction. In this process, the whole electrode was immersed in the liquid Li source, via which the ICE of the Li 3 VO 4 electrode can be controllably elevated from 80% to over 100% within 5 min of pre-lithiation. Rather than the traditional powder treatment for pre-lithiation, this process we proposed minimizes the impact of pre-lithiation on the battery assembly process. Moreover, we further investigated the effect of this pre-lithiation process on the functional components in the electrode. For the first time the ICE of Li 3 VO 4 electrode was elevated to 100%. As a result, the initial reversible capacity of LiFePO 4 ∥Li 3 VO 4 full cell was improved from 44.0 to 146.3 mAh g −1 , demonstrating the feasibility and great potential of the process.
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
LANGMUIR
·
2025
·
IF 3.9
Ling Lin,Shuang Yuan,Huahui Chen,Peng Xu,Tao Zhu,Long Li,Jiaojing Shao
The cobalt-free, high-voltage spinel-type cathode LiNi0.5Mn1.5O4 (LNMO) exhibits high energy and power densities, rendering it a promising candidate for incorporation into next-generation lithium-ion batteries (LIBs). However, its high operating voltage of 4.7 V can lead to electrolyte decomposition, causing structural damage. In addition, the irreversible loss of active lithium in the early cycles reduces capacity performance, hindering its commercial application. To take full advantage of the catalytic effect of LNMO and the prelithiation of sacrificial salt, this work involved blending sacrificial salts (Li2C2O4, Li2CO3, and CH3COOLi) with LNMO to form prelithiated electrodes (LNMO-Sac) and investigating the influence of different sacrificial salts on the performance of LIBs. The results demonstrate that LNMO could efficiently catalyze the decomposition of sacrificial salts and promote the formation of a more stable electrode–electrolyte interface after cycling to mitigate structure destruction of electrodes caused by electrolyte decomposition. Compared with other sacrificial salts, Li2C2O4 provided a highly efficient supplement of active lithium and improved the electrochemical performance of the battery. Thus, LNMO-Li2C2O4 achieved an excellent discharge capacity of 137.9 mAh g–1 at 1C, and capacity retention of 85.9% after 500 cycles, superior to that of LNMO without prelithiation. Moreover, the LNMO-LO/Gr full cell presented an initial capacity of 117.9 mAh g–1 and retained 79.4 mAh g–1 after 300 cycles. This work demonstrates the feasibility of a sacrificial salt as a lithium replenishment strategy for LNMO in practical applications.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Small
·
2023
·Vol. 20
·期 2
·2305639
·
IF 13.3
Shiwei Xu,Qiu Fang,Jipeng Wu,Suting Weng,Xiaoyun Li,Qiuyan Liu,Qiyu Wang,Xiqian Yu,Liquan Chen,Yejing Li,Zhaoxiang Wang,Xuefeng Wang
Prelithiation is an essential technology to compensate for the initial lithium loss of lithium-ion batteries due to the formation of solid electrolyte interphase (SEI) and irreversible structure change. However, the prelithiated materials/electrodes become more reactive with air and electrolyte resulting in unwanted side reactions and contaminations, which makes it difficult for the practical application of prelithiation technology. To address this problem, herein, interphase engineering through a simple solution treatment after chemical prelithiation is proposed to protect the prelithiated electrode. The used solutions are carefully selected, and the composition and nanostructure of the as-formed artificial SEIs are revealed by cryogenic electron microscopy and X-ray photoelectron spectroscopy. The electrochemical evaluation demonstrates the unique merits of this artificial SEI, especially for the fluorinated interphase, which not only enhances the interfacial ion transport but also increases the tolerance of the prelithiated electrode to the air. The treated graphite electrode shows an initial Coulombic efficiency of 129.4%, a high capacity of 170 mAh g −1 at 3 C, and negligible capacity decay after 200 cycles at 1 C. These findings not only provide a facile, universal, and controllable method to construct an artificial SEI but also enlighten the upgrade of battery fabrication and the alternative use of advanced electrolytes.
研究领域:
材料科学
·
电化学
·
电池技术
✓ 已验证
DOI
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Jusheng Zheng,Kui Liang,Kaiyue Shi,Yechao Qiu
The irreversible capacity loss in the first cycle significantly reduces the specific capacity of lithium ion batteries. Cathode prelithiation is a common method to alleviate this problem. Here, Fe/Li2O were successfully prepared by in situ solid phase reaction method. Fe/Li2O as a cathode prelithiation additive has a high prelithiation specific capacity of 447.3 mAh g -1 during charging, and the first charge capacity of LiNi0.6Co0.2Mn0.2O2 with 7.5% Fe/Li2O additive could be enhanced by 9.1% and its cycling stability was improved from 86.9% to 90.2% after 70 cycles. The cathode prelithiation additive remarkably enhanced the content of active lithium during the initial delithiation process, contributing the formation of solid electrolyte interphase on the anode surface and better cycling stability. This easy-operating cathode prelithiation method could obtain evident effect of prelithiation and had good compatibility with existing lithium ion batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
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
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
危险品化学品经营许可证（带存储）