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ACS Nano · 2022 · IF 18.027

Tailoring Electrolyte Solvation for LiF-Rich Solid Electrolyte Interphase toward a Stable Li Anode

Haifeng Tu,Linge Li,Zhicheng Wang,Jian Wang,Hongzhen Lin,Mingchao Wang,Cheng Yan,Meinan Liu

A solid electrolyte interphase (SEI) with robust mechanical property and high ionic conductivity is imperative for high-performance lithium metal batteries since it can efficiently impede the growth of notorious lithium dendrites. However, it is difficult to form such a SEI directly from an electrolyte. In this work, a crowding dilutant modified ionic liquid electrolyte (M-ILE) has been developed for this purpose. Simulations and experiments indicate that the 1,2-difluorobenzene (1,2-dfBen) dilutant not only creates a crowded electrolyte environment to promote the interaction of Li+–FSI–, leading to abundant aggregate ion pairs (AGGs), but also participates in the reduction to construct a robust and high ionic-conductive SEI. With this M-ILE, Li/LiFePO4 cells achieve a capacity retention of 96% over 250 cycles with 9.5 mg cm–2 mass loading, and Li/LiNi0.5Co0.2Mn0.3O2 cells also deliver a discharge capacity of 132 mAh g–1 with a high retention of 88% after 100 cycles. Therefore, the use of a crowding diluent is considered to be an efficient way to construct an advanced SEI for a Li anode.

研究领域: 电化学 · 储能技术 · 材料科学 · 锂离子电池
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Nano Energy · 2017 · IF 12.343

Stabilizing Li/electrolyte interface with a transplantable protective layer based on nanoscale LiF domains

Zhe Peng,Ning Zhao,Zhenggang Zhang,Hao Wan,Huan Lin,Meng Liu,Cai Shen,Haiyong He,Xiangxin Guo,Ji-Guang Zhang,Deyu Wang

Although Li metal has been regarded as one of the most promising anode materials , an unstable Li/electrolyte interface during the cycling process seriously limits its practical application in rechargeable batteries. Herein, we report a transplantable LiF-rich layer (TLL) that can suppress the side reactions between electrolyte and lithium metal. This peelable layer cross-linked by nanoscale LiF domains is obtained by electrochemically reducing NiF 2 electrodes and could be used to protect Li metal anodes . Cu-Li cells using the TLL protection can operate for more than 300 cycles with a Coulombic efficiency as high as ~ 98% in carbonate-based electrolytes. In Li-LiFePO 4 cells, lithium metal with a TLL still looks shiny after 1000 cycles (~ 6 months) in contrast to the black surface of bare lithium foil after ~ 500 cycles (~ 3 months). These results clearly demonstrate that the TLL could greatly limit the side reactions between lithium metal and the carbonate-based electrolytes, and may enable long-term stable operation of Li metal batteries .

研究领域: 材料科学 · 电化学 · 储能技术 · 锂金属电池
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ACS Nano · 2025 · IF 16

Stabilizing Halide Electrolytes against Lithium Metal with a Self-Limiting Layer for All-Solid-State Lithium Metal Batteries

Guangwen Zhang,Deyuan Li,Dongfang Yu,Ao Du,Zihui Chen,Huilin Ge,Weiqi Hou,Yizhou Zhu,Chunpeng Yang

Halide solid-state electrolytes (SSEs) with high ionic conductivity and high-voltage stability have attracted significant interest for application in all-solid-state batteries. However, they are not chemically stable against the lithium (Li) metal anode due to continuous side reduction reactions, hindering the application of halide SSEs in high-energy-density all-solid-state Li metal batteries (ASSLMBs). Here, we report a self-limiting layer (SLL) composed of InF3 and Li2ZrCl6 (LZC) to stabilize the halide SSEs and Li metal anode interface, where the in situ generated LiF-rich layer serves as a passivation layer to suppress ensuing reactions and kinetically stabilize the interface between LZC and Li metal anode. As a result, Li metal symmetric cells with LZC protected by the SLL exhibit excellent cycling performance for over 3000 h. The ASSLMBs with SLL achieve 99.2% capacity retention over 100 cycles at 0.5 C and 83.5% capacity retention after 250 cycles at 2 C. Density functional theory-computed thermodynamic data and postcycling experimental characterizations confirm the forming of a LiF-rich passivation layer between the SLL and the Li anode, which effectively prevents continuous side reactions. This self-limiting interface protection offers a feasible kinetical passivation strategy for halide SSEs and the Li metal anode toward high-performance ASSLMBs.

CAS / MDL: 10026-11-6 7447-41-8
研究领域: 材料科学 · 电化学 · 能源存储
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CERAMICS INTERNATIONAL · 2024 · IF 5.1

Enhanced microwave dielectric properties in one-step cold sintered LiF ceramics via pre-calcination treatment

Jia Peng Yuan,Nuo Chen,Cheng Chao Hu,Bing Liu,Kai Xin Song

Cold sintering has proven effective in densifying microwave dielectric ceramics , but the resulting properties are significantly influenced by the crystallinity of the raw powder. In this study, lithium fluoride (LiF) raw powder underwent pre-calcination at temperatures ranging from 650 °C to 800 °C for 3 h to enhance grain crystallinity. The calcined powder was then mixed with 10 wt% deionized water and cold-sintered at 150 °C under 900 MPa for 1 h to achieve dense LiF ceramics. XRD results confirmed the preservation of LiF phase composition throughout both processes. Increasing calcination temperature exhibited a positive correlation with enhanced relative density in cold-sintered ceramics, reaching up to 98.6 % at 800 °C. SEM images revealed controlled grain growth with higher calcination temperatures. ε r increased with temperature, corresponding to the variation in relative density. Significantly, Qf value experienced substantial enhancement with increasing calcination temperature, ultimately achieving optimal microwave dielectric properties ( ε r  = 8.80, Qf  = 33,300 GHz, and τ f  = −138 ppm/°C) through cold sintering of LiF powder pre-calcinated at 800 °C.

CAS / MDL: 7789-24-4
研究领域: 材料科学 · 陶瓷工程
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY · 2024 · IF 5.8

Sintering behavior, structural evolution, and dielectric properties of Li3Mg3NbO7 + x wt% LiF microwave dielectric ceramics

Chaoyang Cai,Jiawei Xie,Jingjing Ma,Hao Li,Wenming Guo,Hang Qin,Pengzhao Gao,Hanning Xiao

In this paper, x wt% LiF (1 ≤ x ≤ 10) is utilized to decrease sintering temperature, improve microstructure and enhance Q × f of Li 3 Mg 3 NbO 7 ceramics. Remarkably, the appropriate addition of LiF leads to the dramatic reduction in sintering temperature (reduced by 300 °C) and the significant improvement in Q × f (increase ratio: 26 %). The addition of LiF causes the generation of cubic oxyfluoride solid solution, which is confirmed by XRD, SEM and TEM. When x ≤ 8, both orthorhombic oxide and cubic oxyfluoride solid solution exist in ceramics. When x = 10, the ceramic is composed of cubic oxyfluoride solid solution and LiF. It is confirmed that the maximum mass percentage of LiF required to fully form a cubic solid solution is between 8 wt% and 10 wt%. The significant improvement in Q × f is mainly attributed to increase in relative density and orthorhombic-cubic phase transition. In this system, Li 3 Mg 3 NbO 7 + 8 wt% LiF ceramics sintered at 900 °C possess the optimal dielectric properties: ε r = 14.10, Q × f = 152,510 GHz and τ f = −43.5 ppm/°C. The Li 3 Mg 3 NbO 7 + 8 wt% LiF ceramics show an outstanding combination of low ε r , high Q × f and low sintering temperature, surpassing the performance of most low-temperature dielectric materials. The excellent chemical compatibility with Ag electrodes suggests that the Li 3 Mg 3 NbO 7 + 8 wt% LiF ceramics are particularly promising for LTCC applications.

CAS / MDL: 7789-24-4 1313-96-8
研究领域: 材料科学 · 电子工程
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2026 · IF 9.6

Lean-catalyst LiF/Co heterointerface: Unlocking efficient prelithiation for high-energy-density lithium-ion batteries

Xiaoxuan Wang,Jiangdong Sun,Kuikui Xiao,Dong Cai,Shuo Yang,Huagui Nie,Zhi Yang

Developing high-capacity cathode prelithiation agents remains challenging due to severe kinetic limitations, high operational voltages, or insufficient stability in conventional materials. To address this, we report a cobalt-decorated lithium fluoride composite (S-LiF/Co, with a Co content of 15.76 wt% by ICP-OES) synthesized via a scalable solid-state route. The in situ formed LiF/Co heterointerface serves as a catalytic center, which, as evidenced by theoretical calculations, effectively weakens Li F bonds and significantly lowers the energy barriers for both Li + migration and LiF decomposition. This enables S-LiF/Co to deliver a high initial charge capacity of 886.23 mAh g −1 . When incorporated into NCM811 cathodes, it substantially promotes a stable, LiF-rich cathode electrolyte interphase (CEI). In NCM811||Si/C full cells, this additive effectively compensates for irreversible lithium loss, yielding a high initial energy density of 484.01 Wh kg −1 and superior cycling stability with 80.42% capacity retention after 170 cycles. This work provides an effective interface-engineering strategy to overcome the intrinsic barriers of LiF-based materials, offering a promising prelithiation solution for next-generation high-energy-density batteries.

✓ 已验证 DOI PubMed 高影响因子
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PHYSICA B-CONDENSED MATTER · 2026 · IF 3.2

Enhanced luminous performance of perovskite light-emitting diodes with PEDOT:PSS/LiF composite hole transport layer

Xingyue Zhang,Zhixing Chen,Yiting Wang,Xi Wang,Sheng Li,Fei Mei,Yuanming Zhou

Perovskite light-emitting diodes (PeLEDs), characterized by their excellent optoelectronic properties, including high color purity, flexibly tunable emission wavelengths, and relatively high photoluminescent quantum yields, make them suitable for next-generation display technologies. This study investigates and demonstrates that PeLEDs using a PEDOT:PSS/LiF composite hole transport layer (HTL) can achieve enhanced device performance. When 1.0 mg mL −1 of LiF is added, the device attains a maximum luminance of 8317 cd m −2 and a maximum current efficiency of 8.09 cd A −1 , representing improvements of 163% and 92% respectively compared to the reference device. Analysis reveals that the introduction of LiF can optimize the morphology of the perovskite film and passivate defects within it. Additionally, it helps modulate the work function of PEDOT:PSS and enhance its electrical conductivity, thereby improving hole injection efficiency and further boosting the performance of the PeLEDs. The findings presented in this study can provide a reference for the optimization of PeLEDs.

CAS / MDL: 141-78-6 7789-24-4
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Energy Storage Materials · 2023 · IF 20.4

Superior lithium-metal all-solid-state batteries with in-situ formed Li3N-LiF-rich interphase

Qifa Gao,Dengxu Wu,Zhixuan Wang,Pushun Lu,Xiang Zhu,Tenghuan Ma,Ming Yang,Liquan Chen,Hong Li,Fan Wu

Lithium dendrite growth in solid electrolytes (SEs) is one of the most serious challenges to the commercialization of all-solid-state lithium-metal batteries(ASSLMBs) with SEs. Herein , we propose an electrochemical strategy to realize an in-situ modified solid electrolyte interphase (SEI) that can simultaneously resolve both interfacial and dendrite issues. By controlling the current and deposition time in electrochemical treatment, ordered reaction between lithium metal and Si 3 N 4 particles are realized to effectively produce a Li 3 N-LiF-rich multifunctional composit including Li−Si alloys. The consequent symmetric cells demonstrated a remarkably high critical current density up to 3.3mA cm −2 at room temperature and stable plating/stripping process over 1200h at a current density of 0.5mA cm −2 . Moreover, LiCoO 2 /Li 6 PS 5 Cl/Li ASSLMBs delivered a high safety and long life of more than 500 cycles at 1.0mA cm −2 with a steady coulombic efficiency.

研究领域: 材料科学 · 能源技术
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2024 · IF 11.2

Crystal structure, sintering behavior, and microwave dielectric properties of LiF-tailored high entropy Li2Mg6ZnTi6O20 ceramics

Qianbiao Du,Linzhao Ma,Jianhong Duan,Longxiang Jiang,Hao Li,Hanning Xiao

This study designs and synthesizes highly dense Li 2 Mg 6 ZnTi 6 O 20 microwave dielectric ceramics based on a high-entropy strategy, focusing on achieving stable structures, low sintering temperatures, and excellent comprehensive performance. The ceramics exhibit a predominant face-centered cubic disordered phase ( Fd -3 m) sintered at 1200–1280 °C, alongside an increased presence of the second phase MgTiO 3 at higher temperatures. Remarkably, these ceramics demonstrate excellent microwave dielectric properties ( ε r = 16.69, Q × f = 88,230 GHz, and τ f = −36.5 ppm/°C). Additionally, we have explored the addition of x wt% LiF (1 ≤ x ≤ 5) to the Li 2 Mg 6 ZnTi 6 O 20 ceramics to enhance their applicability. The ceramics feature a spinel structure for LiF contents up to 3 wt%, while higher LiF concentrations induce the formation of a secondary phase, LiTiO 2 , characterized by a rock salt structure. Notably, the lattice distortion induced by LiF leads to a constant decrease in ε r . A moderate degree of lattice distortion serves to enhance the lattice stability of ceramics, which is reflected in increased lattice energy. Excellent microwave dielectric properties ( ε r = 16.23, Q × f = 89,728 GHz, τ f = −43.5 ppm/°C) were obtained for x = 3 ceramic sintered at 1140 °C. Even at x = 5, the ceramic retains excellent microwave dielectric properties ( ε r = 16.02, Q × f = 63,079 GHz, τ f = −26 ppm/°C) at a low sintering temperature of 900 °C. This work realizes the multiple effects of LiF and confirms good chemical compatibility with silver for LTCC (low-temperature co-fired ceramics) applications.

研究领域: 材料科学 · 陶瓷工程 · 电子材料
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Materials Today Energy · 2026 · IF 8.6

Stable LiF-rich solid electrolyte interphase via self-polymerizing gel electrolytes boosts silicon anode cycling

Yingqi Li,Dan Zhao,Mengling Zhao,Peiao Lu,Jiakun Luo,Kui-Qing Peng

Silicon is regarded as the most promising candidate for replacing graphite anodes due to its high theoretical capacity (3579 mAh g −1 ) and favorable operating potential (0.3 V vs. Li + /Li), compatible with practical lithium-ion battery applications. However, the inability of liquid electrolytes to accommodate the severe volume changes of microsized silicon (μSi) particles leads to continuous mechanical stress and unstable solid electrolyte interphase (SEI) formation, resulting in rapid electrode fracture. Herein, we design a self-poymerizing gel electrolyte that utilizes the thermal decomposition of LiPF 6 to simultaneously construct a durable, LiF-rich SEI and initiate ring-opening polymerization of tetrahydrofuran (THF) into a polytetrahydrofuran (PTHF) network. Dynamic cross-linking of the PTHF matrix via reversible hydrogen bonding and coordination interactions provides structural adaptability and introduces a solvent nanoconfinement effect. The optimized μSi||Li half-cell delivers a high capacity of 2936.3 mAh g −1 at 0.1 C and maintains a high capacity of 1171.6 mAh g −1 after 600 cycles at 2 C (where 1 C = 3579 mAh g −1 ), outperforming its countertparts employing liquid electrolytes. This work successfully integrates microsized silicon anodes with adaptive gel electrolytes, offering a promising avenue toward high-performance lithium-ion batteries.

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Journal of Energy Chemistry · 2025 · IF 14.9

Nitrogen functionalization of natural hydroxyl cellulose induces a LiF-rich interphase for lithium metal batteries

Jie Deng,Ningxin Chen,Sida Xie,Shan Liu,Zichan Yuan,Shuaiming He,Shi Chen,Zhaohui Wang

Cellulose, the most abundant and renewable biopolymer, offers a sustainable and cost-effective solution for regulating lithium electrodeposition toward safer lithium metal batteries, thanks to its high nanofibrous structure and intrinsic lithiophilic property. In this work, we introduce interface-engineered cellulose-based separators by converting intrinsic hydroxyl groups on cellulose nanofibers (CNFs) to nitrogen functionalities through a trace conducting polymer coating. Both experimental and theoretical results reveal that the nitrogen moieties disrupt the compact hydrogen bond network within hydroxyl cellulose, enabling multiple nitrogen-lithium interactions that enhance lithium ion transport. In addition to an extraordinary Li + transference number of 0.86 and a high ionic conductivity of 1.1 mS cm −1 , the nitrogen-functionalized CNF contributes to a uniform electric field and Li + concentration distribution across the lithium metal surface. This facilitates the formation of a LiF-rich solid electrolyte interface and suppresses Li dendrite growth. Consequently, Li||Li cells demonstrate stable plating/stripping cycles for approximately 3000 h at a current density of 1 mA cm −2 with a fixed capacity of 1 mAh cm −2 , while maintaining a low overpotential of 15 mV. Our work provides valuable insights into the surface functionalization of natural biomass for advancing sustainable energy storage technologies.

CAS / MDL: 109-97-7 64-17-5
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