ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Lifan Wang,Pengfei Jiang,Yiheng Wu,Ruixiang Li,Min Chen,Xindong Wang,Chun Zhan,Guicheng Liu
The development of high-energy all-solid-state lithium-ion batteries (ASSLIBs) is hindered by interfacial incompatibility between Ni-rich layered oxides (LiNi 0.8 Co 0.1 Mn 0.1 O 2 , NCM811) and solid electrolytes (Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 , LATP), where co-sintering-induced Li + depletion and the subsequent oxygen release synergistically degrade electrochemical performance. Here, a dual-functional interface engineering strategy is developed through thermochemical coordination of dynamic lithium compensation and oxygen-anchoring modulation. Incorporation of 10 wt.% LiOH effectively suppresses cation interdiffusion during 700 °C co-sintering, while La 4 NiLiO 8 lithium–oxygen conductor stabilizes lattice oxygen via vacancy passivation, thus eventually protecting NCM811 from thermal decomposition (post-sintering XRD, XPS, and TEM). The optimized NCM811-LATP composite cathode achieves a high initial capacity of 217.1 mAh g −1 at 0.1 C with 80% capacity retention over 248 cycles a 143% lifespan improvement compared to baseline systems, while maintaining charge-transfer impedance below 97.8 Ω (EIS) and suppressing layered-to-spinel phase transitions (post-cycling TEM). This work establishes a universal paradigm for oxygen-interface co-stabilization in ASSLIBs, balancing thermochemical stability with interfacial ion transport to unlock ultra-stable cycling in high-energy-density solid-state systems.
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Changqi Wang,Yongjun Kang,Bingxue Liu,Daolei Lin,Guofeng Tian,Shengli Qi,Dezhen Wu
Polyimide (PI) is a promising binder material for lithium-ion batteries due to its excellent mechanical strength, high thermal stability, and outstanding chemical inertness. However, the high-temperature imidization requirement (>300 °C) of traditional PI binders is incompatible with current electrode preparation processes, severely limiting their practical applications. In this study, a low-temperature-imidized polyimide (∼150 °C) was elaborately designed and utilized as NCM811 cathode binder, which works by covalently bonding 5-aminobenzimidazole (ABZ) to the ends of the flexible 4,4′-oxidiphthalic anhydride (ODPA)/4,4′-oxidiphenylamine (ODA) poly(amic acid) (PAA) chains to realize the self-catalysis at a low temperature, followed by the assistance of dual-functional N,N′-carbonyldiimidazole (CDI) as a catalyst and dehydrating agent to accelerate the condensation and low-temperature dehydration of amic acid, yielding the imidization of the PAA precursor to give PI at 150 °C. Compared to the conventional PVDF binder, the cathode utilizing this low-temperature imidized polyimide (LTPI) binder exhibited excellent capacity retention (84.9% vs 81.7%) after 100 cycles at 0.2C, and superior rate performance (119.3 mAh·g–1 vs 95.7 mAh·g–1 at 5.0C) under a 4.3 V cutoff voltage. The CV, SEM, XRD, and XPS results demonstrate that the designed LTPI binder effectively suppresses the hexagonal (H2) to hexagonal (H3) phase transition and transition metal dissolution, maintaining the cathode’s structural integrity during charge–discharge cycles, thereby ensuring excellent long-term cycle stability. Furthermore, the NCM811 cathode with LTPI binder exhibits significantly enhanced flame-retardant performance compared with the NCM811/PVDF cathode in the combustion experiments, demonstrating the superiority of LTPI binders in improving the safety of the cathode materials. The NCM811/LTPI cathode retains the excellent structural and electrochemical stability of traditional high-temperature-imidized PI binders, providing a practical pathway to develop high-performance binder materials for high-safety and long-cycling lithium-ion batteries.
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产品关联
DOI
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
Wenjie Yuan,Jinlong Liao,Songde Huang,Dakun Song,Qinting Su,Cuihua Li,Jinhua He
Solid lithium metal batteries with solid polymer electrolytes have advantages in terms of high energy density and safety. However, their application is still hindered by unstable solid electrolyte interfaces (SEI and CEI) and uncontrolled dendrite growth. Here, a composite skeleton loaded with dielectric filler yttrium stabilized zirconia nanoparticles (YSZ) on the surface of PVDF-HFP nanofiber filaments is designed, and a novel composite solid electrolyte (CSE) is prepared by in-situ polymerization of DOL (1,3-dioxolane) on this framework to achieve safe and stable high-voltage lithium metal battery (LMB). The dual stable electrode interfaces (CEI and SEI) constructed by in-situ can effectively suppress the generation of lithium dendrites and suppress the degradation of the high-voltage NCM811 positive electrode structure and the generation of cracks in NCM811 particles, endowing the battery with extraordinary performance. The as-obtained CSE exhibits high ionic conductivity of 1.01 × 10 −3 S cm −1 at 30 °C, the enlarged electrochemical window of 6.0 V, and the Li + transference number is 0.72. The assembled Li|NCM811 battery is capable of stable cycling for 400 cycles at a cut-off voltage of 4.5 V and current density of 1C, with a capacity decay of only 0.074 % per cycle. .
研究领域:
材料科学
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电化学
·
能源存储
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DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2026
·
IF 19.9
Xiaodong Wang,Zijun Liu,Miaomiao Zhou,Ao Li,Ruiping Liu
Elemental interdiffusion and interfacial side reactions between sulfide solid-state electrolytes (SSEs) and nickel-rich layered oxide cathodes inevitably form high-impedance, ion-insulating phases at cathode/electrolyte (C/E) interface, which severely degrades the electrochemical performance of all-solid-state lithium batteries (ASSLBs). Herein, we propose a crystallinity-tailored TiNb 2 O 7 (TNO) coating strategy for LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathodes and the long-term interfacial stability of NCM811/SSE interfaces. The ion-conductive yet electron-insulating TNO coating not only guarantees rapid Li + migration across the C/E interface but also effectively suppresses the oxidative decomposition of SSEs at high voltage. More importantly, compared with the high-crystallinity TNO coating, the low-crystallinity counterpart exhibits superior structural adaptability, which can well accommodate the volume changes of NCM811 during Li + insertion/extraction. This unique structural advantage endows the TNO coating with durable protective capability for NCM811 cathodes, especially under high-current-density cycling conditions. Benefiting from the above synergistic effects, the NCM811 cathode modified with low-crystallinity TNO coating synthesized at 500°C (NCM811@T500) delivers a high specific discharge capacity of 150.9 mAh g − 1 after 100 cycles at 0.069 mA cm − 2 and 25°C. This work provides a novel crystallinity-regulation strategy for cathode surface modification, and offers valuable insights into the rational design of high-performance protective coatings for nickel-rich cathodes in sulfide-based ASSLBs.
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
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IF 3.764
Shan Zhang,Ze Feng,Ranjusha Rajagopalan,Dan Sun,Chenghuan Huang,Yougen Tang,Qunxuan Yan,Yurong Ren,Haiyan Wang
Ni-rich layered cathodes have been regarded as one of the high-priority materials, but their commercial application was limited by the highly active surfaces, poor thermal stability, and irreversible phase transition. Furthermore, when they are stored in moist air, the particles can easily form an impurity layer of Li2CO3/LiOH. This inert substance hinders the transmission of lithium ions and electrons, leading to electrochemical performance deterioration. Herein, we report a simple method, namely, metaphosphate repair, which can successfully restore the degraded LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode materials and form an in situ multifunctional hybrid repaired layer of Li3PO4-YPO4-Y(PO3)3 on the secondary particle. The repaired NCM811 delivers a discharge capacity of 171.7 mAh g–1 after 100 cycles, which is much higher than those of pristine (147.6 mAh g–1) and stored degraded (116.2 mAh g–1) samples. Moreover, the restored sample could deliver a capacity retention of 92.3% after 100 cycles at 1C along with a better initial Coulombic efficiency (CE) of 88.4%. This study provides a facile strategy to revive degraded Ni-rich cathode materials and other similar layered oxide cathodes for advanced batteries.
研究领域:
材料科学
·
能源存储与转换
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DOI
高影响因子
Small
·
2024
·Vol. 20
·期 40
·2401204
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IF 13
Siyu Fang,Chengyu Han,Shaojie Zhang,Yu Cao,Kang Ma,Yiming Zhang,Xinpeng Han,Juan Wang,Jie Sun
The demand for state-of-the-art high-energy-density lithium-ion batteries is increasing. However, the low specific capacity of electrode materials in conventional full-cell systems cannot meet the requirements. Ni-rich layered oxide cathodes such as Li(Ni 0.8 Co 0.1 Mn 0.1 )O 2 (NCM811) have a high theoretical specific capacity of 200 mAh g −1 , but it is always accompanied by side reactions on the electrode/electrolyte interface. Phosphorus anode possesses a high theoretical specific capacity of 2596 mAh g −1 , but it has a huge volume expansion (≈300%). Herein, a highly compatible and secure electrolyte is reported via introducing an additive with a narrow electrochemical window, Lithium difluoro(oxalato)borate (LiDFOB), into 1 m LiPF 6 EC/DMC with tris (2,2,2-trifluoroethyl) phosphate (TFEP) as a cosolvent. LiDFOB participates in the formation of organic/inorganic hybrid electrode/electrolyte interface layers at both the cathode and anode sides. The side reactions on the surface of the NCM811 cathode and the volume expansion of the phosphorus anode are effectively alleviated. The NCM811//RP full cell in this electrolyte shows high capacity retention of 82% after 150 cycles at a 0.5C rate. Meanwhile, the electrolyte shows non-flammability. This work highlights the importance of manipulating the electrode/electrolyte interface layers for the design of lithium-ion batteries with high energy density.
研究领域:
材料科学
·
能源技术
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DOI
高影响因子
ACS Applied Energy Materials
·
2022
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IF 6.959
Fanjue Wen,Shuai Cao,Xin Ren,Yuliang Cao,Xinping Ai,Fei Xu
Trimethyl phosphate (TMP) is the most promising safe solvent for lithium-ion battery (LIB) electrolyte because of the nonflammability, oxidation stability, and low cost, but its application is hindered by incompatibility with the graphite anode. Herein, nonflammable electrolytes with ordinary concentration (1 mol L–1) are designed for graphite/LiNi0.8Co0.1Mn0.1O2 (Gr/NCM811) LIBs with TMP/2,2,2-trifluoroethyl methyl carbonate (FEMC) binary solvents. Stable cycling of the Li/Gr half cells with high capacity is achieved via modulation of the Li+ solvation structure. A dual-salt strategy of lithium hexafluorophosphate/lithium difluoro(oxalato)borate is further used to realize the high performance of the Gr/NCM811 full cells. More significantly, the functions and relationship of Li+ solvation structure and electrode/electrolyte interphase are elucidated. Li+ solvation structure and interphase are respectively the thermodynamic and kinetic factors for the side reactions of the electrolyte occurring at the electrode/electrolyte interphase, which should be considered comprehensively in the design of electrolytes for high-energy density LIBs.
研究领域:
材料科学
·
能源化学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Lucheng Li,Meiling Liu,Peng Yang,Wenfeng Yuan,Jun Chen
Broadening the charging and discharging voltage window of high nickel cathode material NCM811 is the most expected method to improve the high specific energy density of batteries currently, yet the cathode-electrolyte interface (CEI) formed by the oxidized and decomposed products of carbonate-based electrolyte under high voltage are always so unsatisfied. Therefore, a voltage-stabilizer, TPFPB (Tris(pentafluoro)phenylborane), added into baseline electrolyte (1 M LiPF 6 in EC:EMC:DMC=1:1:1 vol%) to promote the electrochemical performance of the battery at 4.5 V. The results interpret that the TPFPB-contained NCM811-Li half-cells exhibit high specific capacity (167.10 mAh/g), excellent capacity retention rate (CRR) (75.37 %), and high rate performance (173.3 mAh/g at 5C) during 4.5 V. Meanwhile, through the analysis of the physical characterization techniques. the B- and F-rich interfacial layer, named as CEI film, existing at the interface between the cathode and the electrolyte, produced under 4.5 V, is superior, resulting in impeding the structural collapse of the cathode material and the continued dissolution of transition metal ions (TM n + ) from the cathode material, as well as, ameliorate the electrochemical polarization of the battery, ultimately, it can stabilize the electrochemical performance of the battery under high voltage. Therein, the present work elucidate a new and substantial approach to enhance the high-voltage performances of rich-Ni cathode materials.
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产品关联
DOI
PubMed
高影响因子
Frontiers in Energy Research
·
2022
·
IF 3.858
Zhang Yongquan,Zhu Baoshan,Chi Qingguo,Gao Hongchang,Zhang Changhai,Zhang Tiandong,Zhu Kai,Cao Dianxue
The transport performance of lithium ions affects the rate performance of the cathode at different current densities. The poor interface contact between a solid electrolyte and the cathode makes it difficult to transport lithium ions. Adding a solid electrolyte into the cathode material can improve lithium ion transport. In this paper, we prepared some cathodes with different doping ratios, including two common cathode materials (LiFePO4 and NCM811), and tested their rate and long cycle performance. LFP-10 has a specific discharge capacity of 79.75 mAh g−1 at 5C, and the Li+ diffusion coefficient of LFP-10 is 4.91 × 10−13 cm−2 s−1, which is about 13.4 times higher than the pure LiFePO4 sample. The rate performance of an all-solid-state battery has also been improved, and there is still more than 100 mAh g−1 capacity reserved at 60°C and 2C current density. This shows that the introduction of a PEGDA-based solid electrolyte can significantly improve the Li+ transport of the cathode, and the composite cathode also provides support for the future application of all-solid-state batteries.
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
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Qi Li,Xiaoyu Zhang,Jian Peng,Zhihao Wang,Zhixiang Rao,Yuyu Li,Zhen Li,Chun Fang,Jiantao Han,Yunhui Huang
Poly(ethylene oxide) (PEO)-based polymer electrolytes have been widely studied as a result of their flexibility, excellent interface contact, and high compatibility with a lithium metal anode. Owing to the poor oxidation resistance of ethers, however, the PEO-based electrolytes are only compatible with low-voltage cathodes, which limits their energy density. Here, a high-voltage stable solid-state interface layer based on polyfluoroalkyl acrylate was constructed via in situ solvent-free bulk electropolymerization between the LiNi0.8Mn0.1Co0.1O2 (NCM811) cathode and the PEO-based solid polymer electrolyte. The electrochemical oxidation window of the as-synthesized electrolyte was therefore expanded from 4.3 V for the PEO-based matrix electrolyte to 5.1 V, and the ionic conductivity was improved to 1.02 × 10–4 S cm–1 at ambient temperature and 4.72 × 10–4 S cm–1 at 60 °C as a result of the improved Li+ migration. This fabrication process for the interface buffer layer by an in situ electrochemical process provides an innovative and universal interface engineering strategy for high-performance and high-energy-density solid-state batteries, which has not been explicitly discussed before, paving the way toward the large-scale production of the next generation of solid-state lithium batteries.
研究领域:
材料科学
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电化学
·
能源存储
·
固态离子学
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电池技术
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高分子化学
·
界面科学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Zhen Sun,Yanqing Lai,Na lv,Yaqi Hu,Bingqin Li,Liangxing Jiang,Jiong Wang,Shuo Yin,Kui Li,Fangyang Liu
Argyrodite sulfide solid electrolytes, such as Li6PS5Cl (LPSC), have received much attention due to their high ionic conductivity (>1 mS cm–1) and success in all-solid-state batteries (long cycle performance, high energy density, etc.). Numerous efforts are spent on modifying the properties of the electrolyte itself. Here, we combine first-principles calculations with experiments to investigate O-doped argyrodite sulfide solid electrolytes (Li6PS5–xClOx,x = 0–1). It is found that Li6PS4.75ClO0.25 (LPSCO0.25) with x = 0.25 and cubic phase (F4̅3 m) shows the highest ion conductivity of 4.7 mS cm–1 (cold-pressed), higher than that of undoped Li6PS5Cl (4.2 mS cm–1). The bare LiCoO2/LPSCO0.25/Li–In all-solid-state battery exhibits an initial capacity of 131 mA h g–1 at 0.1 C and satisfactory cycling stability with 86% capacity retention after 250 cycles to the 4th cycle at 0.3 C under 25 °C. In addition, the NCM811/LPSCO0.25/Li–In cell is assembled using bare LiNi0.83Co0.06Mn0.11O2 cathode and shows an initial discharge capacity of 181 mA h g–1 at 0.1 C and 160 mA h g–1 at 0.3 C. The doping of oxygen-forming Li6PS5–xClOx also improves the stability to Li metal, proven by cyclic voltammetry and powder X-ray diffraction tests. The calculation results for the band structure reveals that LPSC has the lowest unoccupied molecular orbital than LPSCO0.25, further confirming the above conclusion.
研究领域:
材料科学
·
电化学
·
能量存储
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DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2021
·
IF 9.127
Huajun Zhao,Yunxian Qian,Guangfu Luo,Jian Chang,Chaoyang Wang,Jun Wang,Huaiyu Shao,Yonghong Deng
LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode coupling with artificial graphite (AG) is a promising tendency for high-energy-density batteries . However, realization of long-term lifespan under current realistic conditions remains a “Gordian knot” for large-scale commercialization-oriented realm owing to the aggressive and highly reactive Ni 4+ sites on the delithiated cathodes and electrolyte exhaustion. Vinylene carbonate (VC) is commonly employed as the additive for graphite anode in carbonate electrolytes. However, VC has limited protection ability for NCM811/AG, especially for high-temperature cycling, showing conspicuous gas generation and large interfacial resistance . Herein, advanced carbonate-based electrolytes containing vinylene carbonate (VC) and phosphate compounds like triallyl phosphate (TPPC2) and tripropargyl phosphate (TPPC3) as electrolyte additives are reported to improve the performance of NCM811/AG pouch cells at elevated temperature. Theoretical calculations and comprehensive characterizations reveal that these two electrolytes well regulate the electrodes interface with more robust and homogenous films. Moreover, the TPPC2 and TPPC3 additives exhibit stronger tendency to eliminate the corrosive active oxygen ( 1 O 2 ) released from NCM811. These merits mitigate the electrolyte decomposition, decrease the gas generation, inhibit the dissolution of transition metals from cathode, and protect the structure stability of NCM811. Such outstanding electrochemical performance reveals promising prospects in the commercialized application of NCM811/AG batteries .
研究领域:
电化学
·
材料科学
·
能源存储
·
锂离子电池
·
界面化学
·
电极材料
·
电解质工程
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DOI
高影响因子
危险品化学品经营许可证（带存储）