Journal of Materials Chemistry A
·
2025
·
IF 9.5
Junyu Chen,Xuedong Zhang,Feixiang Wu,Long Xie,Feng Li,Nina Wu,Zixuan Cao,Jinwen Zhao,Yuxuan Zhang,Xin He,Hongxia Gu,Jianyu Huang,Qiao Huang
Integrating conversion-type cathodes (such as iron-based fluorides (IBFs)) into sulfide all-solid-state batteries (ASSBs) significantly enhances energy density but faces challenges including unstable cathode/electrolyte interfaces. To mitigate these issues, a near-amorphous Li1.26Mg0.12Zr1.86(PO4)3 (LMZP) coating technology is developed to protect nano-sized FeF2 (n-FeF2) and micro-sized FeF3 (m-FeF3) cathodes from reacting with the sulfide electrolyte for the first time. The LMZP coating approach offers simplicity, low energy consumption and scalability. With the LMZP-coated cathodes and lithium–indium (Li–In) anode, the ASSBs achieve a discharge capacity of 310 mAh g−1 after 600 cycles and a maximum areal capacity of 2 mAh cm−2 for n-FeF2, and 301 mAh g−1 after 700 cycles with a maximum areal capacity of 3.1 mAh cm−2 for m-FeF3. When using a lithium (Li) metal anode, the ASSBs maintain a discharge capacity of 310 mAh g−1 after 300 cycles for n-FeF2 and 300 mAh g−1 after 600 cycles for m-FeF3, demonstrating excellent cycling stability and capacity retention. Notably, a discharge capacity of 280 mAh g−1 is sustained after 200 cycles for n-FeF2 and 301 mAh g−1 after 180 cycles for m-FeF3, with a reduced stack pressure (10 MPa). These results are unprecedented in IBF-based ASSBs, highlighting the potential of advanced coating strategies to enable scalable, high-performance metal fluoride cathodes in ASSBs with higher energy densities.
研究领域:
储能材料
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电化学
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固态电池技术
·
表面涂层工程
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DOI
高影响因子
Journal of Energy Storage
·
2025
·
IF 9.8
Dong Chen,Jinhui Li,Lihan Zhang,Kuan Wang,Manling Sui,Pengfei Yan
Biphasic composite materials have been demonstrated to be effective in enhancing the structural stability and electrochemical performance of layered cathodes for sodium-ion batteries. Herein, based on the cationic potential methodology and co-doping strategy, we design a biphasic O3/P2 composite layered cathode (85NFMLCC, Na 0.85 Ca 0.02 Ni 0.2 Li 0.1 Fe 0.15 Co 0.05 Mn 0.5 O 2 ) and further integrate surface modification to achieve superior cycling performance, which is prepared by a simple one-pot solid state sintering method. Comprehensive structural characterizations reveal that the surface modification is realized by an inner Co-enriched layer and an outmost Ca-coating layer, which enables much improved rate capability and cycling stability simultaneously. In situ XRD confirms that biphasic design effectively suppresses the harmful phase transition during high voltage cycling, and the bilayer surface modification further enhances the cathode interfacial kinetics and robustness. The electrochemical tests demonstrated that 85NFMLCC exhibits a high specific capacity (136.7 mAhg −1 at 0.1C), superior cycling stability and rate capability at 2.0–4.3 V, 97.8 % capacity retention after 100 cycles at 0.1C and 84.5 % capacity retention after 800 cycles at 1C 2.0–4.0 V. This work demonstrates that biphasic composite with proper surface modification is a very promising design route toward high performance high voltage cathode material for sodium-ion batteries.
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DOI
高影响因子
ADVANCED MATERIALS
·
2020
·Vol. 33
·期 1
·2002325
·
IF 27.398
Shaojie Chen,Jingxuan Zhang,Lu Nie,Xiangchen Hu,Yuanqi Huang,Yi Yu,Wei Liu
Metallic lithium (Li), considered as the ultimate anode, is expected to promise high-energy rechargeable batteries. However, owing to the continuous Li consumption during the repeated Li plating/stripping cycling, excess amount of the Li metal anode is commonly utilized in lithium-metal batteries (LMBs), leading to reduced energy density and increased cost. Here, an all-solid-state lithium-metal battery (ASSLMB) based on a garnet-oxide solid electrolyte with an ultralow negative/positive electrode capacity ratio (N/P ratio) is reported. Compared with the counterpart using a liquid electrolyte at the same low N/P ratios, ASSLMBs show longer cycling life, which is attributed to the higher Coulombic efficiency maintained during cycling. The effect of the species of the interface layer on the cycling performance of ASSLMBs with low N/P ratio is also studied. Importantly, it is demonstrated that the ASSLMB using a limited Li metal anode paired with a LiFePO 4 cathode (5.9 N/P ratio) delivers a stable long-term cycling performance at room temperature. Furthermore, it is revealed that enhanced specific energies for ASSLMBs with low N/P ratios can be further achieved by the use of a high-voltage or high mass-loading cathode. This study sheds light on the practical high-energy all-solid-state batteries under the constrained condition of a limited Li metal anode.
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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电池技术
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Yang Hu,Wu Tang,Qihang Yu,Chuluo Yang,Cong Fan
The lithium-rich organic cathodes are undoubtedly important for fabricating lithium-ion (Li-ion) full batteries. Currently, very few lithium-rich organic cathodes have been reported for their O2-sensitive characteristics. In this article, we initially propose a new electrochemical method to in situ synthesize a novel lithium-rich organic cathode, namely lithium anthracene-9,10-bis[2-benzene-1,4-bis(olate)] (ABB4OLi, CT = 256 mA h g–1), from its phenol precursor of anthracene-9,10-bis(2-benzene-1,4-diol). The addition of anthracene moiety as the linking bridge is to increase the molecular weight and simultaneously enhance the electronic conductivity for the designed organic molecule (ABB4OLi). In Li-ion half cells, ABB4OLi could deliver average specific capacities of 194 mA h g–1 during 250 cycles (50 mA g–1) and 100 mA h g–1 during 400 cycles (2 A g–1). In the all-organic Li-ion full cells with the working voltage above 1 V, the ABB4OLi electrode could realize the average capacities of 70 mA h g–1cathode during 200 cycles (50 mA g–1). This work has forwarded a significant step for the development of organic Li-ion full batteries.
研究领域:
电化学
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材料科学
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能源存储
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锂离子电池
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有机功能材料
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电极材料
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DOI
高影响因子
Journal of Materials Chemistry A
·
2023
·Vol. 11
·期 6
·2979-2984
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IF 11.9
Wu Wei,Zhihong Wang,Liyun Yao,Hao Jiang,Chunzhong Li
Development of Ni-rich and Co-poor cathodes (Ni ≥ 80%, Co ≤ 5%) is indispensable for the next-generation lithium-ion batteries (LIBs) owing to the serious impact of scarce resources and fragile supply chain of cobalt, but they suffer from a more prominent lattice oxygen emission with serious Li/Ni intermixing as well as worsening crystal and interface structure. Herein, CeO2−x-coated LiNi0.9Co0.045Mn0.045Al0.01O2 has been demonstrated to stabilize lattice oxygen by the well-dispersed Al–O bonds and the reversible oxygen-storage protective layer. The in situ DEMS and ex situ spectral analyses verified the negligible O2 and CO2 emission, even charging to 4.4 V, and the formation of stable cathode–electrolyte interfacial membrane. The as-obtained cathode exhibited a reversible specific capacity as high as 223 mA h g−1 at 0.1C and 140 mA h g−1 even at 10C with 96.7% capacity retention at 1C after 100 cycles in a coin-type half-cell. About 90.1% capacity retention could still be obtained at 1C in a pouch-type full-cell after 300 cycles. This work provides a viable cathode for durable LIBs by stabilizing the lattice oxygen of Ni-rich and Co-poor cathodes.
研究领域:
电化学
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材料科学
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能源存储
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锂离子电池
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固态化学
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表面科学
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电极材料
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DOI
高影响因子
JOURNAL OF ELECTROCERAMICS
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2024
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IF 1.7
Wang Yikui,Tao Jianming,Wang Jiangjie,Chen Shaoyang,Yang Yanmin,Lin Yingbin
Serious structural irreversibility and interfacial side reactions pose major challenges for the stable operation of LiCoO 2 cathodes at high voltages. Herein, we report a polymer-based solid electrolyte (SLP) composed succinonitrile, LiTFSI and PVDF as a binder to address these issues. The SLP binder exhibits superior performance compared to traditional PVDF and PVDF binders with LiTFSI, with higher ionic conductivity (8.46 × 10 − 5 S cm − 1 at 30 ℃), lower activation energy of 0.38 eV and excellent adhesion. Even with just 3% SLP binder, LiCoO 2 cathode operating at a cutoff voltage of 4.6 V and loaded with ~ 6.0 mg cm − 2 active material demonstrates improved rate capability at higher compaction densities, delivering a discharge specific capacity of 146.5 mAh g − 1 after 100 cycles at 0.5 C-rate. The SLP binder not only enhances Li + conduction but also facilitates the formation of a stable cathode-electrolyte interphase, thus reducing the Li + diffusion barrier and interface polarization, and enhancing battery’s performance at low temperature. Furthermore, the SPL binder’s high compatibility and elasticity with the electrolyte mitigate irreversible structural changes and volume expansion in LiCoO 2 during cycling, leading to better preservation of the layered structure and lower internal stress for stable cycling under high temperatures. This strategy provides a novel interface protection idea for electroceramic cathode materials and may facilitate commercial development.
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
Nature Energy
·
2024
·
IF 49.7
Ding Feixiang,Ji Pengxiang,Han Zhen,Hou Xueyan,Yang Yang,Hu Zilin,Niu Yaoshen,Liu Yuan,Zhang Jiao,Rong Xiaohui,Lu Yaxiang,Mao Huican,Su Dong,Chen Liquan,Hu Yong-Sheng
High-entropy oxides have expanded the potential for high-performance Na-ion battery cathodes due to their vast compositional space and entropy-driven stabilization. However, a rational design approach for optimizing their composition is still lacking. Here, we develop an O3-type oxide cathode composed of all-3 d transition metals, NaNi 0.3 Cu 0.1 Fe 0.2 Mn 0.3 Ti 0.1 O 2 (NCFMT), which exhibits improved reversible specific capacity and exceptional cycling stability. Replacing Ti 4+ with Sn 4+ ions (NaNi 0.3 Cu 0.1 Fe 0.2 Mn 0.3 Sn 0.1 O 2 ; NCFMS) results in poor structural reversibility and diminished cycling stability. Our investigations suggest that the structural integrity of the layered cathode is affected by the compatibility of constituent elements within the transition metal layers (TMO 2 ). In NCFMS, planar strain induced by metal-ion displacement triggers elemental segregation and crack formation during repeated cycling. In contrast, NCFMT demonstrates a robust structural framework for stable Na + storage due to its high mechanochemical compatibility among constituent elements. This understanding provides insights for designing outstanding layered high-entropy cathode materials.
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
Small
·
2024
·
IF 13
Ruoxuan Qi,Ming Yang,Tianle Zheng,Xingchen Liu,Yonggao Xia,Ya-Jun Cheng,Peter Müller-Buschbaum
The LiCoO 2 (LCO) cathode is foreseen for extensive commercial applications owing to its high specific capacity and stability. Therefore, there is considerable interest in further enhancing its specific capacity by increasing the charging voltage. However, single-crystal LCO suffers from a significant capacity degradation when charged to 4.5 V due to the irreversible phase transition and unstable structure. Herein, an ultra-small amount (0.5% wt. in the electrode) of multi-functional PIM-1 (a polymer with intrinsic microporosity) additive is utilized to prepare a kind of binder-free electrode. PIM-1 modulates the solvation structure of LiPF 6 due to its unique structure, which helps to form a stable, robust, and inorganic-rich cathod-eelectrolyte interphase (CEI) film on the surface of LCO at a high voltage of 4.5 V. This reduces the irreversible phase transition of LCO, thereby enhancing the cyclic stability and improving the rate performance, providing new perspectives for the electrodes fabrication and improving LCO-based high-energy-density cathodes.
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
Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Zeng Weihao,Xia Fanjie,Wang Juan,Yang Jinlong,Peng Haoyang,Shu Wei,Li Quan,Wang Hong,Wang Guan,Mu Shichun,Wu Jinsong
Fast-charging, non-aqueous lithium-based batteries are desired for practical applications. In this regard, LiMn 2 O 4 is considered an appealing positive electrode active material because of its favourable ionic diffusivity due to the presence of three-dimensional Li-ion diffusion channels. However, LiMn 2 O 4 exhibits inadequate rate capabilities and rapid structural degradation at high currents. To circumvent these issues, here we introduce quintuple low-valence cations to increase the entropy of LiMn 2 O 4 . As a result, the entropy-increased LiMn 2 O 4 -based material, i.e., LiMn 1.9 Cu 0.02 Mg 0.02 Fe 0.02 Zn 0.02 Ni 0.02 O 4 , when tested in non-aqueous lithium metal coin cell configuration, enable 1000 cell cycles at 1.48 A g −1 (corresponding to a cell charging time of 4 minutes) and 25°C with a discharge capacity retention of about 80%. We demonstrate that the increased entropy in LiMn 2 O 4 leads to an increase in the disordering of dopant cations and a contracted local structure, where the enlarged LiO 4 space and enhanced Mn-O covalency improve the Li-ion transport and stabilize the diffusion channels. We also prove that stress caused by cycling at a high cell state of charge is relieved through elastic deformation via a solid-solution transition, thus avoiding structural degradation upon prolonged cycling.
研究领域:
材料科学
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电化学
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DOI
高影响因子
Materials
·
2021
·Vol. 14
·期 12
·3193
·
IF 3.623
Tu Lan,Xiaolong Guo,De Li,Yong Chen
The memory effect of lithium-ion batteries (LIBs) was first discovered in LiFePO4, but its origin and dependence are still not clear, which is essential for regulating the memory effect. In this paper, a home-made spray drying device was used to successfully synthesize LiFePO4with an average particle size of about 1 μm, and we studied the influence of spray drying temperature on the memory effect of LiFePO4in LIBs. The results showed that the increasing of spray drying temperature made the memory effect of LiFePO4strengthen from 1.3 mV to 2.9 mV, while the capacity decreased by approximately 6%. The XRD refinement and FTIR spectra indicate that the enhancement of memory effect can be attributed to the increment of Li–Fe dislocations. This work reveals the dependence of memory effect of LiFePO4on spray drying temperature, which will guide us to optimize the preparation process of electrode materials and improve the management system of LIBs.Keywords:LiFePO4;spray drying method;memory effect;cathode materials
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
Coatings
·
2022
·Vol. 12
·期 10
·1433
·
IF 3.236
Zhiyuan Pang,Hongzhou Zhang,Yue Ma,Dawei Song,Xixi Shi,Lianqi Zhang,Yong Zhou
Binders play a very important part in electrodes, as they closely bind active materials, conductive agents, and current collectors together. The application of binders is critical to the electrochemical performance of Li-S batteries. Herein, a series of studies on sulfur cathodes with different binders is carried out. Compared to traditional polyvinylidene fluoride, γ-polyglutamic acid (γ-PGA) is rich in polar functional groups (amino and carboxyl groups), and the shuttle effect of lithium polysulfide can thereby be inhibited due to the secondary bond between the functional groups and polysulfide. Furthermore, the integrity of the cathode during electrochemical processes can be maintained with a γ-PGA binder. After assembly with a Li anode, a capacity retention of 62.5% is maintained after 100 cycles, which is much higher than that of batteries with traditional binders such as polyvinylidene fluoride (53.9%), polyvinylpyrrolidone (52.8%), sodium carboxymethylcellulose (40.7%), and polyacrylonitrile (51.5%).Keywords:lithium–sulfur battery;sulfur cathode;binders;polyglutamic acid
研究领域:
材料科学
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电化学
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能源存储
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2025
·Vol. 21
·期 14
·2412647
·
IF 12.1
Hanzhou Liu,Yang Lu,Yanchen Liu,Shenghao Jing,Zongliang Zhang,Siliang Liu,Yang Liu,Yongle Chen,Kun Zhang,Shuo Yin,Fanqun Li,Fangyang Liu
All-solid-state lithium metal batteries (ASSLBs) are promising for high energy and safety. Halide-based solid-state electrolytes, characterized by high ionic conductivity and a notably wide electrochemical window exceeding 4.3 V, hold significant promise for compatibility with high-energy cathodes. However, oxygen in cathodes exhibits a strong tendency to interact with the central metal cation in halide solid-state electrolyte, forming an unstable cathode-electrolyte interface (CEI) and leading to cathodic degradations. Herein, a pre-oxidation strategy is proposed for Y based halide solid-state electrolytes, leveraging oxygen to pre-establish robust Y─O bonds within the halide electrolyte structure Li 2 YCl 2.5 Br 1.5 O 0.5 (2LO-0.5). The robust Y─O bonds in 2LO-0.5 effectively hinder uncontrolled oxygen interactions with Y 3 ⁺, which would otherwise lead to the formation of oxidizable YOCl. This stabilization promotes the formation of a thin, stable Y₂O₃-based CEI against LiNi 0.83 Co 0.11 Mn 0.06 O 2 (NCM83). Therefore, the ASSLB assembled with 2LO-0.5 and NCM83 demonstrates an initial discharge-specific capacity of 208 mAh g −1 and retained 80.6% of its capacity after 1000 cycles, attributed to stable CEI film derived from pre-oxidized strategy. This work offers new insights for regulating the non-redox reaction between halide solid-state electrolytes and oxide cathodes, promoting the rational design of high-performance halide solid-state electrolytes.
研究领域:
材料科学
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电化学
·
固态离子学
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能源存储
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电池技术
·
界面化学
✓ 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）