ACS Applied Energy Materials
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2022
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IF 6.959
Bolei Shen,Haojing Zhang,Yingjie Wu,Hao Jiang,Yanjie Hu,Chunzhong Li
The demand for lithium compensation materials is becoming urgent as energy density requirements increase. As next-generation anodes, mixed silicon and carbon (Si–C) materials are limited by low efficiency in the first cycle owing to the formation of a solid electrolyte interphase film. However, most compensation materials are water- and oxygen-sensitive and exhibit low electrochemical activity and decomposition efficiency. In this study, water- and oxygen-stable lithium oxalate (Li2C2O4) was developed to enhance the capacity and cycle-life of the lithium-ion battery. Various metal oxides were screened to improve the electrochemical activity of Li2C2O4. Co3O4 exhibited the strongest catalytic performance, and the catalytic mechanism of Co3O4 on Li2C2O4 was studied by density functional theory. Ultrasonic atomization drying was used to combine Co3O4 quantum dots (Co3O4-QDs) with Li2C2O4 for improved efficiency. The electrochemical activity of the modified Li2C2O4 improved, and the decomposition voltage decreased from 4.65 to 4.0 V. The modified Li2C2O4 exhibits catalytic activity, and it can be used in LiFePO4, which has weak catalytic activity; the decomposition efficiency in the LiFePO4 system increased from 34.16 to 99.10%. In the Si–C//LiFePO4 full battery system, the first cycle discharge capacity increased from 80 to 160 mA h g–1; the lost capacity of the first cycle was fully compensated for. Additionally, the CO2 produced by Li2C2O4 decomposition could inhibit the decomposition of the electrolyte, further improving the cycle performance of the battery.
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
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2025
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IF 19
Yun Luo,Fanbin Hu,Le Tian,Qingfeng Liu,Yi Fan,Yingjie Zhang,Zitong Fei,Qi Meng,Peng Dong
Direct regeneration is recognized as the most promising strategy for recycling spent LiFePO 4 (SLFP) due to its economic and environmental advantages. However, challenges persist in high-temperature solid-phase regeneration, including uneven lithium compensation from particle agglomeration and conflicting timing between lithiation and carbon coating. Therefore, a regeneration strategy is proposed utilizing a molecular fence and vapor deposition mechanism. Lithiation, vapor-deposited carbon coating, and in situ nitrogen doping are achieved through the synergistic effect of creatine and lithium stearate. Lithium stearate forms a molecular fence on SLFP surfaces, enhancing particle dispersion and uniform lithium replenishment. Below 300 °C, NH 3 released from creatine decomposition drives Li + insertion into the SLFP lattice to reduce Fe 3+ , completing lithiation. Subsequently, the generated small carbon-nitrogen molecules radicals undergo structural reorganization, forming a continuous conjugated structure that forms an in situ nitrogen-doped 3D conductive carbon network with topological defects. The heterocyclic and defective structures in the carbon coating modulate electron cloud distribution, creating additional active sites for electron transport and significantly improving conductivity. The regenerated LiFePO 4 delivers a discharge capacity of 146.2 mAh g −1 at 1 C and retains 95.83% capacity after 200 cycles. This strategy offers a viable pathway for high-efficiency, high-quality SLFP recycling.
研究领域:
材料科学
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环境科学
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化学工程
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能源化学
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固态化学
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电化学
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循环利用技术
✓ 已验证
产品关联
DOI
高影响因子
Nano Energy
·
2023
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IF 17.6
Wenyi Xiang,Ruotong Ma,Xiaoye Liu,Xiangkun Kong,Shiji Shen,Limin Wang,Zongzi Jin,Zhongliang Zhan,Chusheng Chen,Chengwei Wang
Garnet type solid-state electrolytes (SSEs) possess high stability against Li metal, intrinsic safety, and wide electrochemical window. To achieve the all-solid-state batteries (ASSBs) with high gravimetric/volumetric energy density and high power density, flat thin garnet SSEs with a high ionic conductivity of > 10 −4 S/cm are required. However, the current fabrication processes are challengeable to maintain both the high ionic conductivity and the flat skeleton due to the severe Li loss during processing and the fragile nature of thin films . Herein, we introduce a rapid Li compensation (RLC) technique that combines the ultra-fast high-temperature sintering (UHS) technique with the tape casting process to produce highly ionic conductive, flat garnet SSE thin films. The freestanding Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) thin film with a thickness of 40 µm, fabricated using this technique, displays a surface roughness of 5 µm and a relative density of 95%. After a 10-seconds Li compensation, the compensated LLZTO film displays an ionic conductivity of 4.3 × 10 −4 S/cm, 2 times higher than the non-compensated one. As a proof of concept, this RLC technique proposes a new strategy for the fabrication of high-performance ceramic thin films and also lays a solid foundation for the application of ASSBs.
研究领域:
材料科学
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固态电池
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电化学
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能源材料
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陶瓷工程
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2025
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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.
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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固态电池
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界面化学
✓ 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）