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
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Yangchenyi Wu,Shanyu Wang,Yang Wu,Fuzhong Wu,Jie Tang
Silicon (Si) is living with severe pulverization of active materials, continuous breakage of structure in electrode, and turbulent solid electrolyte interphase (SEI) because of huge volume variation during (dis)charging. Herein, from the view of the active material and electrode structure, the innovative dual modification that combines carbon coating and Ti 3 C 2 T x as conductive agents is adopted, generating more than simply pooling their efforts together. The resultant Si@C-M electrodes exhibit an excellent rate capacity of 1538.1 mA h g −1 at 5 A g −1 and maintain capacity retention of 80.5 % with 1084.8 mA h g −1 after 300 cycles at 1 A g −1 . The sterling performance is thanks to the stable electrode provided by the coating-carbon and Ti 3 C 2 T x which not only reduces interface impedance, and enhances Li-ion diffusion, but suppresses the volume variation of electrodes as well effectively as verified by in situ and ex situ characterization. Moreover, utilizing the Ti 3 C 2 T x as the conductive agent is beneficial to forming benign SEI rich in LiF and Li 2 O. This work provides a potential strategy and exploits new routes for the practical utilization of high-energy-density lithium-ion batteries (LiBs).
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
RARE METALS
·
2025
·
IF 11
Liu Lang,Zhang Qian,Han Guangrui,Zhang Mengjie,Song Xinyu,Xiao Hong,Hou Linrui,Jiang Ruiyu,Yuan Changzhou
Si, as the most promising anode with high theoretical capacity for next-generation lithium-ion batteries (LIBs), is hampered in commercial application by its poor electrical conductivity and significant volume expansion. Herein, the core-shell Si@SiO x /C@C-Ar (SSC-A) or Si@SiO x /C@C-H 2 /Ar (SSC-H) composites are purposefully designed by in situ introduction of inorganic SiO x in pure Ar or H 2 /Ar atmosphere to realize a Si-based anode for LIBs. By introducing different atmospheres, the valence states of SiO x are regulated. The inorganic transition layer formed by the combination of SiO x with higher average valence and asphalt-derived carbon demonstrates better performance in both stabilizing the core-shell structure and inhibiting the agglomeration of Si particles. Given these advantages, the SSC-A electrode exhibits excellent electrochemical performance (1163 mAh g −1 after 400 cycles at 1 A g −1 ), and the commercial blended graphite-SSC-A electrode reaches a specific capacity of 442 mAh g −1 with 74.8% capacity retention under the same conditions. Even the SSC-A electrode without Super P maintains an ultrahigh discharge specific capacity of 803 mAh g −1 with 60.6% after cycling. Importantly, the full batteries based on SSC-A without Super P achieve a discharge specific capacity of 126 mAh g −1 with 28.2% capacity decay after 200 cycles, demonstrating the superior commercial application potential.
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
ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Qiang Zhang,Yuxiu Yu,Haojie Li,Fengying Zhang,Yaodong Liu
Binders are expected to play important role in silicon-based anode materials, but have not been well explored. In this work, a serial of silicon containing polyimides and polyamides have been synthesized and used as the binder of high content (80wt%) silicon anode. Systematic characterizations have been done on the chemical structures, physical properties of the binders, and the electrochemical performances of silicon-based anode. It was found that the swelling ratio, adhesion strength, and hardness plays important roles on the initial Coulombic efficiency (ICE) and capacity retention of silicon-based anode, and these parameters highly depend on the types and properties of binders. After optimizing the chemical structures and physical properties of the binders, a high specific capacity of 2941 mAh g −1 , relatively high initial Coulombic efficiency (ICE) of 83%, and good capacity retention of 85% (after 200 cycles) have been obtained. These results would help researchers to design new types of binders for silicon-based anode to improve its ICE and capacity stability.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xiaorui Wang,Hao Li,Wenhui Fu,Qiushi Chen,Xuzhong Gong,Zhi Wang,Junhao Liu
Binders provide a straightforward and efficient strategy to mitigate the significant challenge of volume expansion in silicon anodes for lithium-ion batteries. To improve the cycle life of silicon anodes, a cross-linked binder carboxymethyl cellulose–phytic acid–pyrrole (CMC-DP) is designed and synthesized using carboxymethyl cellulose, phytic acid, and pyrrole. The numerous hydroxyl groups in phytic acid provide abundant binding sites for the formation of hydrogen and ester bonds. The formation of hydrogen bonds and covalent bonds enhances the mechanical properties of the adhesive. The amino groups in the binder form N Si O covalent bonds with silicon particles, while the hydroxyl and carboxyl groups form (COO) 2 Cu and (OH) 2 Cu coordination bonds with the copper foil, enhancing interfacial adhesion. When the CMC-DP10 (10 µL pyrrole) binder is applied to silicon nanoparticles (∼30 nm), the specific capacity of the electrode can be maintained at around 1700 mAh/g after 500, whereas the CMC binder achieves only ∼100 mAh/g under the same conditions. This work demonstrates that the CMC-DP binder exhibits strong adhesion to both silicon nanoparticles and copper foil.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Small Methods
·
2022
·Vol. 6
·期 5
·2101591
·
IF 15.367
Zhibo Song,Taohang Zhang,Lu Wang,Yan Zhao,Zikun Li,Meng Zhang,Ke Wang,Shida Xue,Jianjun Fang,Yuchen Ji,Feng Pan,Luyi Yang
Due to the severe volume variations during electrochemical processes, Si-based anodes suffer from poor cycling performance as the result of a collapsed conductive network. In this regard, a key strategy for fully exploiting the capacity potential of Si-based anodes is to construct a robust conductive network through rational binder design. In this work, a bio-inspired conductive binder (PFPQDA) is designed by introducing dopamine-functionalized fluorene structure units (DA) into a conductivity enhanced polyfluorene-typed copolymer (PFPQ) to enhance its mechanical properties. Through constructing hierarchical binding networks and resilient electron transportations within both nano-sized Si and micro-sized SiO x electrodes via interweaved interactions, the PFPQDA successfully suppresses the electrode expansion and maintains the integrity of conductive pathways. Consequently, owing to the favorable properties of PFPQDA, Si-based anodes exhibit improved cycling performance and rate capability with an areal capacity over 2.5 mAh cm –2 .
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
PubMed
高影响因子
Scientific Reports
·
2019
·Vol. 9
·期 1
·1-16
·
IF 4.011
An Fuqiang,Zhao Hongliang,Zhou Weinan,Ma Yonghong,Li Ping
Recently, high-energy density cells containing nickel-rich cathodes and silicon-based anodes have become a practical solution for increasing the driving range of electric vehicles. However, their long-term durability and storage performance is comparatively poor because of the unstable cathode-electrolyte-interphase (CEI) of the high-reactivity cathode and the continuous solid-electrolyte-interphase (SEI) growth. In this work, we study several electrolyte systems consisting of various additives, such as S-containing (1,3,2-dioxathiolane 2,2-dioxide (DTD), DTD + prop-1-ene-1,3-sultone (PES), methylene methanedisulfonate (MMDS)) and Si-containing (tris(trimethylsilyl) phosphate (TTSP) and tris(trimethylsilyl) borate (TMSB)) compounds, in comparison to the baseline electrolyte (BL = 1.0 M LiPF 6 + 3:5:2 w-w:w EC: EMC: DEC + 0.5 wt% lithium difluoro(oxalato)borate (LiDFOB) + 2 wt% lithium bis(fluorosulfonyl)imide (LiFSI) + 2 wt% fluoroethylene carbonate (FEC) + 1 wt% 1,3-propane sultone (PS)). Generally, electrolytes with Si-containing additives, particularly BL + 0.5% TTSP, show a lower impedance increase in the full cell, better beginning-of-life (BOL) performance, less reversible capacity loss through long-term cycles and better storage at elevated temperatures than do electrolytes with S-containing additives. On the contrary, electrolytes with S-containing additives exhibit the advantage of low SEI impedance but yield a worse performance in the full cell than do those with Si-containing additives. The difference between two types of additives is attributed to the distinct function of the electrodes, which is characterized by cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS) and X-ray photoelectron spectroscopy (XPS), which was performed on full cells and half cells with fresh and harvested electrodes.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
Coatings
·
2024
·Vol. 14
·期 9
·1210
·
IF 2.9
Songjia Kong,Chenguang Liu,Jiawei Ren,Tianchang Wang,Xianwei Geng,Yudan Yuan,Chun Zhao,Cezhou Zhao,Li Yang
Silicon is a promising anode material for high-performance lithium-ion batteries (LIBs), but its rapid capacity degradation has significantly hindered its large-scale application. In this study, we propose an in situ self-assembly polymerization method to fabricate a stable silicon-based anode by leveraging electrostatic self-assembly technology, in situ esterification, and amidation reactions. The incorporation of a cross-linked polymer, combined with the synergistic effects of electrostatic interactions between negatively charged MXene and positively charged silane-coupling-agent-modified silicon, offers a novel strategy for enhancing the electrochemical performance of LIBs. Notably, annealed electrodes with a 65 wt% nmSi-NH2/MXene ratio demonstrate outstanding electrochemical performance, achieving a capacity of 929.5 mAh g⁻¹ at a current density of 1 A g⁻¹ after 100 charge/discharge cycles. These findings suggest that the integration of cross-linked polymers and electrostatic self-assembly can significantly improve the intercalation and overall electrochemical performance of silicon anodes in lithium-ion batteries.
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
Materials Today Energy
·
2024
·
IF 9
Yuhui Weng,Jun Cao,Jianhong Gao,Wei Cao,Jiale Chen,Waqar Ahmad,Min Ling,Dongxu Yu,Jun Chen,Chengdu Liang
Currently, silicon-based anode is one of the most promising anode materials which can be applied in next-generation lithium-ion batteries. However, the high activity of electrode-electrolyte interface and low electronic conductivity of Si anode during the cycling process greatly limits its large-scale application. Al is the metallic current collector known to promote electronic conductivity and lithium-ion transfer with low cost. However, to our knowledge, scalable interface engineering incorporating Al with carbonized polymer has not been reported. Herein, a polyacrylonitrile (PAN) and aluminum metal dual functionalization interconnected network is achieved via a simple sol-gel method followed by high-temperature calcination to obtain a stable solid electrolyte interphase (SEI) while allowing fast Li + transmission. The calculated diffusion energy barrier for lithium ions in Al is 0.2198 eV, significantly lower than that in Cu and Fe. Benefiting from the enhanced interfacial protection and kinetics of Si with polyacrylonitrile/Al, the prepared Si@Al@CPAN anode exhibits high lithium storage capacity (2034.90 mAh·g -1 after 150 cycles at 0.84 A·g -1 ). At the same time, the prepared Si@Al@CPAN anode outperforms the pure Si anode in rate performance at 12.6 A g -1 (1116.75 mAh·g -1 vs. 2.84 mAh·g -1 ). The present work delivers new design ideas for high-performance Si anode with the multi-functionalization interface.
研究领域:
材料科学
·
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
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
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
危险品化学品经营许可证（带存储）