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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Interfacial fluoride engineering enabled robust LiF-rich solid electrolyte interphase to reduce active lithium loss in rechargeable lithium battery

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.

CAS / MDL: 872-50-4
研究领域: 材料科学 · 电化学
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Energy & Environmental Science · 2023 ·Vol. 17 ·期 3 ·1163-1174 · IF 32.5

Controllable long-term lithium replenishment for enhancing energy density and cycle life of lithium-ion batteries

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 · 电化学
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Energy Storage Materials · 2025 · IF 20.2

In-situ Capacity Regeneration of Degraded Lithium-ion Batteries Using Remanufacturing Remediator

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.

CAS / MDL: 2564-83-2
研究领域: 材料科学 · 能源技术 · 化学工程
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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-11 · IF 15.7

Dual-gradient metal layer for practicalizing high-energy lithium batteries

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 · 材料科学 · 能源存储 · 纳米材料 · 界面化学 · 电池技术 · 固态离子学
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