CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Tianqi Jia,Geng Zhong,Sirong Lu,Xiaolong Ren,Yao Lv,Nanrui Li,Rui Yin,Guohuang Kang,Kangning Cai,Feiyu Kang,Yidan Cao
Active lithium loss, which is caused by parasitic reactions due to the instability of solid electrolyte interphase (SEI) on the anodes, results in fast capacity fade of batteries. Constructing robust SEI layer is an effective way to reduce active lithium loss. Herein, we propose a AgF-coated separator (AgF-CS) to facilitate robust LiF-rich SEI on the anode during initial cycle. Electrochemical analysis and microstructure investigations confirm the formation of the LiF-rich SEI on the anode induced by the fluoride-containing coating layer. The fluoride-containing interfacial layer not only effectively enhances the reversible capacity of the SiO anode even under lean electrolyte (14 μL mAh −1 ) condition, but also prolongs the cycling life of lithium metal batteries by reducing the consumption of electrolyte and active lithium. The initial Coulombic efficiency (ICE) of LiFePO 4 ||SiO full cell is increased from 43.68 % to 84.18 % with pretreatment by AgF-CS. As a result, the reversible capacity of LiFePO 4 ||SiO full cell is increased by ∼124 % in contrast with that of the unmodified one. The strategy proposed here, benefiting from the simple manufacture, provides a feasible way to alleviate active lithium loss and elevate energy density of rechargeable lithium batteries.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2024
·Vol. 35
·期 9
·1-13
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IF 2.8
Gong Zonggui,Wang Nanlan,Guo Haoxuan,Zhu Peishu,Wang Qijing,Yu Hang,Zhang Yu,Gao Min,Zheng Xinghua
Due to the increasingly urgent safety and energy density concerns of lithium-ion batteries, more and more attention has been attracted by the Li 7 La 3 Zr 2 O 12 (LLZO)-based solid electrolytes with high ion conductivity and chemical stability against Li-metal. However, to prepare the high-quality LLZO ceramic electrolyte with high-ion conductivity and density, there is still a big challenge of the serious “Li-loss” and the abnormal grain growth during the long-time high-temperature sintering process. A novel covered sintering method is put forward to prepare the high-quality Mo-doped LLZO (LLZMO) ceramic electrolyte. The sintering strategy effectively suppresses the Li-loss to obtain the LLZMO dense ceramics with cubic garnet phase and tight grain boundaries. The LLZMO ceramics sintered at lower temperature of 1050 °C for 2 h via the novel covered sintering exhibit high density ( ρ r = 92.3%) and high-ionic conductivity of 6.08 × 10 –4 S cm −1 at 25 °C, which are close to those of LLZO-based ceramics prepared by hot pressing sintering, ultrafast high-temperature sintering (UHS). The novel covered sintering provides an energy-saving, low-cost and high-efficient strategy to prepare the high-quality LLZO-based ceramics electrolyte.
研究领域:
材料科学
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固态电解质研究
✓ 已验证
DOI
高影响因子
Energy & Environmental Science
·
2023
·Vol. 17
·期 3
·1163-1174
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IF 32.5
Ganxiong Liu,Wang Wan,Quan Nie,Can Zhang,Xinlong Chen,Weihuang Lin,Xuezhe Wei,Yunhui Huang,Ju Li,Chao Wang
A persistent challenge plaguing lithium-ion batteries (LIBs) is the consumption of active lithium with the formation of SEI. This leads to an irreversible lithium loss in the initial cycle and a gradual further exhaustion of active lithium in subsequent cycles. While prelithiation has been proven effective in compensating for this loss by introducing additional active lithium into batteries, prior studies have predominantly concentrated on offsetting the initial lithium loss, often overlooking the continuous lithium consumption that occurs throughout cycling. To address this challenge, we employed a sustained in situ lithium replenishment strategy that involves the systematic release of additional lithium inventory through precise capacity control during long-term cycling. Our method utilizes a lithium replenishment separator (LRS) coated with dilithium squarate-carbon nanotube (Li2C4O4–CNT) as the lithium compensation reagent. Placing Li2C4O4 on the separator rather than within the cathode significantly reduces disruptions in conduction pathways and inhibits catalytic reactions with LiFePO4, preventing the formation of carbon residues. When implemented in the LiFePO4||graphite battery system, our approach resulted in an impressive 12.9% capacity improvement in the initial cycle and a remarkable 97.2% capacity retention over 700 cycles, surpassing the comparison group, which exhibited 80% capacity retention after 426 cycles.
研究领域:
材料科学
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电化学
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
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2025
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IF 5.5
Minghua Li,Deli Xu,Guoxian Wu,Sheng Wang,Hao Cheng,Jianshu He,Kangzhe Yu,Zhihan Liu,Yaqing Zhou,Bingbing Tian
All-solid-state lithium batteries (ASSLBs) have attracted significant attention due to their advantages of high energy density, enhanced safety profile, and potential for cost-effective manufacturing. At the same time, a superior anode that matches the ASSLBs is particularly important. In this work, we demonstrated chemically prelithiated MoS2 as an anode material for ASSLBs, which embeds lithium ions into a MoS2 matrix (LixMoS2) in advance to counteract lithium loss during the cycling. By a combination of LixMoS2, Li6PS5Cl (LPSC), and Li–In alloy, an all-solid-state lithium battery with superior long-term cycling and rate capability has been achieved. The cells exhibited a capacity retention rates of 93.4 and 90.8% after 100 cycles at both 0.2 and 1C, alongside a high specific discharge capacity of 480 mAh g–1 at 1C. Furthermore, when paired with a LiCoO2 (LCO) cathode, the full cell maintained a capacity retention rate of 95% over 300 cycles at 1C, with an average capacity loss of only 0.013 mAh g–1 per cycle. This work offers a feasible strategy for optimizing anode materials within sulfide-based ASSLBs, providing valuable insights for the development of high-performance ASSLBs for practical applications.
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
Energy Storage Materials
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2025
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IF 20.2
Yuhang Gao,Han-Ming Zhang,Jinfeng Sun
With the increasing application and production of lithium-ion batteries, the environmentally friendly and low-cost recycling of degraded lithium-ion batteries has become an urgent issue. Based on the battery degradation theory of active lithium loss, this work proposes a strategy for in-situ remanufacturing of degraded batteries through the injection of the 2,2,6,6-tetramethylpiperidine N-oxide (TEMPO) remediator to replenish the active lithium loss. The mechanism of TEMPO remediator initiated in-situ remanufacturing (TRIISR) strategy is sustainable activation of the inactive Li 0 (lithium dendrites and dead lithium) to recover the degraded capacity. Moreover, TEMPO induces the LiF-rich solid electrolyte interphase (SEI) formation, further enhancing the dynamics and cycling stability of remanufactured batteries. Multiple characterizations and electrochemical tests corroborate the underlying mechanism of TRIISR according to the corresponding evolutions of structure and electrochemical performances of button cells. Based on this TRIISR strategy, the in-situ remanufactured commercial pouch cell exhibits a satisfactory capacity recovery of 5.89% and a lifespan extension by 70%. This work presents the simplicity TRIISR strategy with pro-environment, low-capacity loss rate, great techno-economic benefits due to the internal Li replenishment without damaging the cells. The insightful TRIISR strategy facilitates the secondary utilization of degraded batteries.
研究领域:
材料科学
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能源技术
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Science China-Materials
·
2022
·Vol. 66
·期 3
·903-912
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IF 8.64
Zhong Wei,Zhang Ce,Li Siwu,Zhang Wei,Zeng Ziqi,Cheng Shijie,Xie Jia
Irreversible lithium loss in the initial cycles appreciably reduces the energy density of lithium-ion batteries. Prelithiation is an effective way to compensate for such lithium loss, but current methods suffer from either the instability or low capacity of prelithiation reagents. Lithium oxalate (Li 2 C 2 O 4 ) has shown great potential as a lithium-compensation material because of its high theoretical capacity (equivalent to lithium metal), low cost, and air stability. However, the practical applications of Li 2 C 2 O 4 are limited by its low electrochemical activity and high critical decomposition voltage. In this study, we performed the prelithiation of a low-voltage cathode by using Mo 2 C catalysis and nano-Li 2 C 2 O 4 . Results show that the Mo 2 C catalyst changes the electron cloud distribution around Li 2 C 2 O 4 and greatly reduces the activation energy, thereby significantly accelerating the lithium release from Li 2 C 2 O 4 . The nano-Li 2 C 2 O 4 prepared by freeze-drying shows accelerated ionic and electronic conduction as well as close contact with Mo 2 C. Benefiting from the synergistic effect, the decomposition potential of Li 2 C 2 O 4 is decreased by 0.5 V with an efficiency close to 100%. The LiCoO 2 ∥SiO full cell empowered with the nano-Li 2 C 2 O 4 /Mo 2 C prelithiation composite demonstrates 46.9% higher capacity than the control and thus has great potential for practical applications.
研究领域:
储能
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材料科学
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电化学
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纳米技术
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Xiaojuan Lu,Feng Zhang,Jing Li
Perovskite-type lithium-ion conductor Li 0.33 La 0.56 TiO 3 was prepared via microwave sintering. The influence of lithium sources on the properties of the samples prepared and the compensation of lithium loss were investigated. XRD patterns, exhibiting a mixture of tetragonal and cubic phase, were all similar for the samples made with different lithium sources. The total conductivity of the sample made with Li 2 CO 3 achieved 0.51 × 10 −4 S/cm, which was the highest among all the samples made with different sources. The highest total conductivity of the sample made with Li 2 CO 3 was attributed to the largest grains, which would result in a smaller concentration of less-conductive grain boundaries. The total conductivity of the sample compensated with 5% Li 2 O was 38% higher than the sample made stoichiometrically. Given that grain sizes were similar for the samples compensated with a varied amount of Li 2 O and the relative density of the sample compensated with 5% Li 2 O was even the lowest among these samples, the highest total conductivity was rooted in the highest ratio of cubic phase. These results indicated that lithium sources could influence the properties of the LLTO samples greatly by resulting in a variation on crystalline phase, grain size, and relative density, which collectively determine the migration of lithium ions in polycrystalline Li 0.33 La 0.56 TiO 3 .
研究领域:
材料科学
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固体化学
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电化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Wei Weng,Bin Liu,Weiwei Lin,Fanyou Zeng,Rui Mei,Feng Yan,Xinghua Zheng
As a promising candidate for solid-state electrolytes, garnet solid electrolyte Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) with high ionic conductivity and excellent electrochemical performance has attracted more and more attention due to the increasingly urgent safety and energy density concerns of lithium-ion batteries. However, there is still a big challenge to prepare the high-quality LLZTO ceramic electrolyte with fine grains, high ion conductivity and high density because of the serious Li-loss, porous microstructure and the abnormal grain growth during the long-time high-temperature conventional sintering process. Herein, Fe 2 O 3 as a sintering aid has been introduced to prepare the high-quality LLZTO ceramic electrolyte by low temperature sintering, which is an effective strategy to obtain high density and inhibit Li-loss. The densification behavior, phase composition, microstructure and electrochemical performance have been systematically investigated for LLZTO ceramics with different amount of Fe 2 O 3 additive. High density (ρ r = 94.7 %), high ionic conductivity of 6.82 × 10 −4 S cm −1 and low electronic conductivity of 9.09 × 10 −9 S cm −1 at 25 °C are achieved for the LLZTO-5 mol% Fe 2 O 3 ceramics sintered at the lower temperature of 1075 °C for 3 h. Meantime, the garnet electrolyte exhibits excellent electrochemical performance. Li/LLZTO-5 mol% Fe 2 O 3 /Li symmetric cell exhibits good stability after cycling more than 800 h at a current density of 0.1 mA·cm −2 . The LiFePO 4 /LLZTO-5 mol% Fe 2 O 3 /Li full cell delivers an initial discharge capacity of 115.2 mAh·g⁻¹ and retains a good capacity of 88 % after 80 charge-discharge cycles at 0.2 C. This suggests that the introduction of Fe 2 O 3 as a sintering aid provides a promising strategy of energy-saving, low-cost and high-efficient to achieve high-quality LLZTO-based solid electrolytes for advanced energy storage systems.
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-11
·
IF 15.7
Tian Mengyu,Qiao Ronghan,Cen Guanjun,Tian Li,Ben Liubin,Yu Hailong,De Volder Michael,Zhao Chenglong,Wang Qidi,Huang Xuejie
Pairing high-energy nickel-rich cathodes with current collectors as anodes presents a compelling strategy to significantly boost the specific energy of rechargeable lithium-ion batteries, driving progress toward a transportation revolution. However, the limited active lithium inventory sourced by the cathodes tend to be rapidly consumed by irreversible Li plating/stripping and interfacial side reactions. To address these limitations, we propose a dual-gradient metal layer as an innovative solution to mitigate active Li loss by promoting uniform Li deposition and in situ formation of a stable solid electrolyte interphase. The operation of these batteries is investigated using a combination of electrochemical and chemical techniques to differentiate dead Li and interphase-bound Li inventory loss as well as material characterization methods to analyse the plated Li and interfacial composition and morphology. The developed dual gradient metal layer-based 600 mAh LiNi 0.9 Co 0.05 Mn 0.05 O 2 | |Cu pouch cells achieve an areal capacity of 7.25 mAh cm −2 and deliver an 80% capacity retention over 160 cycles. We show that the proposed approach is compatible with a range of different metal materials, offering a promising path toward next generation long-lasting, high-energy, initially active material-free anode based Li metal 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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纳米材料
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界面化学
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电池技术
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固态离子学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
·
IF 16.6
Jin Chengbin,Huang Yiyu,Li Lanhang,Wei Guoying,Li Hongyan,Shang Qiyao,Ju Zhijin,Lu Gongxun,Zheng Jiale,Sheng Ouwei,Tao Xinyong
Reactive negative electrodes like lithium (Li) suffer serious chemical and electrochemical corrosion by electrolytes during battery storage and operation, resulting in rapidly deteriorated cyclability and short lifespans of batteries. Li corrosion supposedly relates to the features of solid-electrolyte-interphase (SEI). Herein, we quantitatively monitor the Li corrosion and SEI progression (e.g., dissolution, reformation) in typical electrolytes through devised electrochemical tools and cryo-electron microscopy. The continuous Li corrosion is validated to be positively correlated with SEI dissolution. More importantly, an anti-corrosion and interface-stabilizing artificial passivation layer comprising low-solubility polymer and metal fluoride is designed. Prolonged operations of Li symmetric cells and Li | |LiFePO 4 cells with reduced Li corrosion by ~74% are achieved (0.66 versus 2.5 μAh h −1 ). The success can further be extended to ampere-hour-scale pouch cells. This work uncovers the SEI dissolution and its correlation with Li corrosion, enabling the durable operation of Li metal batteries by reducing the Li loss.
研究领域:
材料科学
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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）