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Li5FeO4
JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

Enhanced prelithiation performance of Li5FeO4 cathode additive and optimized solid electrolyte interface enabled by Mn substitution

Dezhi Wang,Jiasen Wang,Xuebao Li,Cheng Han,Hao Fei,Zhuangzhi Wu

In the pursuit of enhancing the energy density of lithium-ion batteries, cathode prelithiation emerges as a pivotal approach, introducing additional irreversible active lithium ions to augment performance. Li 5 FeO 4 (LFO) stands out as an excellent option, boasting an impressive theoretical specific capacity and the additional advantages of cost-effectiveness in raw materials and low preparation cost. However, the impact of extra lithium incorporations on compositional changes at the electrode-electrolyte interface as well as on cell stability has impeded further researches. Herein, a Mn doping strategy is proposed and predicted by first-principles calculations to synthesize partially Mn-substituted Li 5.125 Fe 0.875 Mn 0.125 O 4 (LFMO). And the prelithiation with LFMO improved the interfacial composition of LiFePO 4 (LFP) batteries compared to LFO, achieving a charging capacity of 213 mAh∙g −1 in the first cycle at 0.05 C. The subsequent treatment demonstrated superior cycling stability, maintaining a discharge specific capacity as high as 155.3 mAh∙g −1 after 100 cycles at 0.2 C, and exhibiting a higher capacity retention in the full cell. These discoveries could contribute to enhancing the regulation of battery interface during the utilization of LFO, potentially promoting the development of cathode lithium additives.

研究领域: 材料科学 · 电化学 · 电池技术
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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-13 · IF 15.7

Air-stable Li5FeO4 additive enabled by carbon coating for energy-dense lithium-ion batteries

Liu Canshang,Zhang Hao,Zhou Weiwei,Tian Xu,Zhang Tiantian,Niu Sicheng,Li Jianing,Cao Minglei,Wang Qin,Lv Fei,Peng Tangping,Tao Lijuan,Rang Xiaodong,Chen Zhicheng,Su Xin

Li 5 FeO 4 is a promising pre-lithiation additive for the positive electrode in lithium-ion batteries, offering the potential to enhance energy density. However, its susceptibility to air degradation presents a significant challenge for commercialization. In this study, we develop an effective carbon coating strategy utilizing pitch to improve the air stability of Li 5 FeO 4 . The coating process results in the formation of a compact carbon layer on the surface of Li 5 FeO 4 particles, enabling the coated Li 5 FeO 4 to retain a high specific capacity of 743.4 mAh g −1 after 72 h of exposure to air with 20% relative humidity. This retention represents 92.3% of its initial capacity and 85.7% of its theoretical maximum capacity. In contrast, uncoated Li 5 FeO 4 undergoes rapid degradation, losing most of its electrochemical activity within just 4 h under identical conditions. Beyond improving air stability, the carbon coating enhances Li 5 FeO 4 ’s specific capacity, rate capability, and cycling stability. To substantiate the practical application of carbon-coated Li 5 FeO 4 , we construct a pouch-type cell, which exhibits a 13.7% increase in energy density compared to the cell without the prelithiation additive. These findings collectively suggest that the carbon-coated Li 5 FeO 4 represents a viable strategy for advancing the commercial deployment of this material in lithium-ion batteries.

CAS / MDL: 24937-79-9 872-50-4
研究领域: 材料科学 · 电化学 · 储能
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ADVANCED FUNCTIONAL MATERIALS · 2024 ·Vol. 34 ·期 22 ·2315010 · IF 18.5

Understanding the Air-Exposure Degradation Chemistry of the Sacrificial Cathode Additive Li5FeO4 for Li-Ion Batteries

Bin Zhu,Wei Zhang,Qiyu Wang,Yanqing Lai,Jingqiang Zheng,Naifeng Wen,Zhian Zhang

Li 5 FeO 4 (LFO) is emerging as a promising prelithiation additive due to the high lithium donor capacity (>700 mAh g −1 ), cheap raw materials, good environmental adaptability, and reliable synthesis approach. However, LFO suffers from extremely poor air stability and the underlying mechanism remains elusive. Herein, LFO is subjected to different atmospheres (the main component of air) of O 2 , CO 2 , N 2, and 30% humidity air to unravel its reaction mechanism with air and the interfacial chemistry. It is found that Li + ions will escape from the LFO crystal lattice to construct Li 2 O, Li 2 CO 3, and LiOH impurity phases with an obvious change of LFO surface morphology in contact with O 2 , CO 2, and humidity air. These insulating species remarkedly inhibit Li + ion diffusion from the material and thus lead to an increment of interfacial impedance and an apparent capacity degradation. Consequently, the initial charging capacity decays rapidly from 681.5 to 169.4 mAh g −1 (under O 2 ) and to 54.8 mAh g −1 (under CO 2 ), respectively. In this regard, a facile coating strategy is proposed on the surface of LFO to effectively improve its air stability.

研究领域: 材料科学 · 电化学 · 储能技术 · 锂离子电池
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JOURNAL OF POWER SOURCES · 2026 · IF 8.4

Rational process design of cost-benefit prelithiation additive Li5FeO4 enables high-performance lithium-ion batteries

Weiwei Wang,Xueying Jia,Yuhao Zhang,Bing Qin,Ying Wang,Chenyu Yang,Qinghua Liu

Li 5 FeO 4 (LFO), an ideal cathode prelithiation additive for lithium-ion batteries, has attracted significant interest because of its extremely high capacity, suitable voltage window, and environmental friendliness. However, the solid-phase synthesis process of LFO is not clear and suffers from the exorbitant cost of Li 2 O, making finding an alternative lithium source for improving cost-effectiveness in industrial production crucial. In this study, LFO materials were synthesized via a solid-phase sintering method involving two types of lithium sources. Utilizing in-situ X-ray diffraction and X-ray absorption fine structure spectroscopy, the evolution mechanism of solid-phase synthesis was elucidated. In particular, a low-temperature plateau was determined for the synthesis process employing LiOH as the lithium source. Compared with Li 2 O-derived O-LFO, the as-obtained prelithiation additive H-LFO achieved an ∼69.7% cost reduction with satisfactory initial charge capacity, energy density and cycling stability in industrial-scale applications. This work provides a practical solution for promoting prelithiation technology and reducing the preparation cost of prelithiation additives.

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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Improved Zero-Charge Storage Performance of LiCoO2/Mesocarbon Microbead Lithium-Ion Batteries by Li5FeO4 Cathode Additive

Chunyu Liu,Guomeng Xie,Ziqin Xu,Ce Liang,Ping Xu,Hai-Tao Fang

Discharging lithium-ion batteries to zero-charge state is one of the most reliable ways to avoid the thermal runaway during their transportation and storage. However, the zero-charge state causes the degradation or even complete failure of lithium-ion batteries. Specialized solutions are required to endow lithium-ion batteries with improved zero-charge storage performance, namely, the ability to tolerate zero-charge state for a long time without unacceptable capacity loss. Here, we report that a Li5FeO4 cathode additive can improve the zero-charge storage performance of LiCoO2/mesocarbon microbead (MCMB) batteries. The irreversible charge capacity of the Li5FeO4 additive results in the downregulation of anode and cathode potentials when the battery is at zero-charge state. More importantly, the Li5FeO4 additive offers a small discharge plateau below 2.9 V versus Li/Li+, which can hold the anode potential at zero-charge battery state (APZBS) in a potential range of 2.4∼2.5 V versus Li/Li+ during storage for 10 days. Such a precise control on APZBS not only suppresses the decomposition of the solid electrolyte interface film on the MCMB anode and inhibits the dissolution of the copper current collector occurring at high potentials but also avoids the excessive decrease of the cathode potential at the zero-charge battery state and consequently protects the LiCoO2 cathode from overlithiation occurring at low potentials. As a result, the Li5FeO4 additive with a charge capacity percentage of 23% in the cathode increases the capacity recovery ratio of the LiCoO2/MCMB battery from 37.6 to 95.5% after being stored at the zero-charge state for 10 days.

研究领域: 电化学 · 能量存储与转换 · 材料科学 · 电池技术
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

Lattice Modulation on Air-Stable Fe-Based Prelithiation Materials with High Capacity via Triggering Anionic Redox Activity

Bin Zhu,Wei Zhang,Shihao Li,Naifeng Wen,Jingqiang Zheng,Chaohong Guan,Jie Li,Zhian Zhang

Li5FeO4 (LFO) is a leading candidate for cathode prelithiation due to its ability to engage in both anionic and cationic redox processes, offering substantial capacity potential. However, the practical implementation of LFO is hampered by incomplete delithiation and susceptibility to air-induced degradation, which together constrain its effectiveness in lithium compensation. In this study, we propose a lattice modulation strategy that incorporates cobalt substitution at the iron sites of LFO, resulting in the novel compound Li5.5Fe0.5Co0.5O4 (LFCO), which enhances both the anionic redox activity and the air stability of the material. We demonstrate that the incorporation of Co2+ ions facilitates the reversible oxidation of lattice oxygen species from O2– to intermediate O2n– and ultimately to O2, thereby augmenting the overall redox capacity. LFCO exhibits superior electrochemical performance with specific capacities of 860.1 mAh g–1 at 0.1C and 580.0 mAh g–1 at 1C, compared to 681.5 and 351.8 mAh g–1 for LFO. Furthermore, LFCO maintains a high capacity of 520.8 mAh g–1 after exposure to 20% relative humidity for 4 days. Integration of LFCO into graphite∥NCM811 pouch cells results in 89.6% capacity retention at 0.5C over 200 cycles, underscoring the potential of this material in developing next-generation energy-dense lithium-ion batteries.

CAS / MDL: 12057-24-8 1345-25-1
研究领域: 材料科学 · 电化学 · 储能 · 电池技术
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