Journal of Energy Chemistry
·
2022
·
IF 13.599
Junbo Zhang,Haikuo Zhang,Ruhong Li,Ling Lv,Di Lu,Shuoqing Zhang,Xuezhang Xiao,Shujiang Geng,Fuhui Wang,Tao Deng,Lixin Chen,Xiulin Fan
Passivation by the inorganic-rich solid electrolyte interphase (SEI), especially the LiF-rich SEI, is highly desirable to guarantee the durable lifespan of Li metal batteries (LMBs). Here, we report a diluent with the capability to facilitate the formation of LiF-rich SEI while avoiding the excess consumption of Li salts. Dissimilar to most of reported inert diluents, heptafluoro-1-methoxypropane (HM) is firstly demonstrated to cooperate with the decomposition of anions to generate LiF-rich SEI via releasing F-containing species near Li surface. The designed electrolyte consisting of 1.8 M LiFSI in the mixture of 1,2-dimethoxyethane (DME)/HM (2:1 by vol.) achieves excellent compatibility with both Li metal anodes (Coulombic efficiency ∼ 99.8%) and high-voltage cathodes (4.4 V LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) and 4.5 V LiCoO 2 (LCO) vs Li + /Li). The 4.4 V Li (20 μm)||NMC811 (2.5 mA h cm −2 ) and 4.5 V Li (20 μm)||LCO (2.5 mA h cm −2 ) cells achieve capacity retentions of 80% over 560 cycles and 80% over 505 cycles, respectively. Meanwhile, the anode-free pouch cell delivers an energy density of ∼293 W h kg −1 initially and retains 70% of capacity after 100 deep cycles. This work highlights the critical impact of diluent on the SEI formation, and opens up a new direction for designing desirable interfacial chemistries to enable high-performance LMBs.
研究领域:
材料科学
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电化学
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DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2023
·Vol. 29
·期 64
·e202301774
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IF 4.3
Lian Li,Kaizhao Wang,Kaijun Wang,Tianyou Chen,Jing Wang,Zhongshan Deng,Qingming Chen,Weijun Zhang,Jin Hu
Graphical The amorphous titanium dioxide is used to coat eGaSn nanodroplets (eGaSn NDs) to construct the core-shell structure of eGaSn@TiO 2 nanodroplets (eGaSn@TiO 2 NDs). The amorphous TiO 2 shell forms a stable SEI film, alleviates volume expansion, and provides electron/ion transport channels. The resulting eGaSn@TiO 2 NDs exhibit high capacities of 580, 540, 515, 485, 456 and 426 mAh g −1 at 0.1, 0.2, 0.5, 1, 2 and 5 C, respectively. No obvious decay is observed in more than 500 cycles with a capacity of 455 mAh g −1 at 1 C. Gallium-based alloy liquid metal batteries currently face limitations such as volume expansion, unstable solid electrolyte interface (SEI) film and substantial capacity decay. In this study, amorphous titanium dioxide is used to coat eutectic GaSn nanodroplets (eGaSn NDs) to construct the core-shell structure of eGaSn@TiO 2 nanodroplets (eGaSn@TiO 2 NDs). The amorphous TiO 2 shell (~6.5 nm) formed a stable SEI film, alleviated the volume expansion, and provided electron/ion transport channels to achieve excellent cycling performance and high specific capacity. The resulting eGaSn@TiO 2 NDs exhibited high capacities of 580, 540, 515, 485, 456 and 426 mAh g −1 at 0.1, 0.2, 0.5, 1, 2 and 5 C, respectively. No significant decay was observed after more than 500 cycles with a capacity of 455 mAh g −1 at 1 C. In situ X-ray diffraction (in situ XRD) was used to explore the lithiation mechanism of the eGaSn negative electrode during discharge. This study elucidates the design of advanced liquid alloy-based negative electrode materials for high-performance liquid metal batteries (LMBs).
研究领域:
材料科学
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电化学
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DOI
PubMed
高影响因子
CARBON
·
2026
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IF 12.7
Junyu Lin,Yujing Xu,Peisi He,Anting Feng,Ye Han,Zongyu Mao,Zexi Li,Guobin Zhang,Yaping Wang,Xiao Yu,Shaozhong Zeng,Jing Liu,Tao Lin,Dongju Fu,Shuzhang Niu
Regenerating graphite anode materials from spent lithium-ion batteries (LIBs) is essential for improving resource utilization and reducing environmental impact. However, conventional recycling routes often require excessive energy input, incur high costs, and deliver regenerated graphite with unsatisfactory electrochemical performance. To address these limitations, we propose a low-temperature catalytic repair strategy based on an integrated carbon source, nitrogen source, and catalyst system. Chitosan serves as both the carbon precursor and the in situ nitrogen dopant, while a cobalt salt functions as both a catalyst and a pore-forming template. At a mild temperature of 600 °C, a porous nitrogen-doped graphene-like carbon (PNGC) layer is constructed on the surface of spent graphite (SG). This functional layer repairs surface defects and promotes the formation of a Li 3 N-rich solid electrolyte interphase (SEI) during cycling. Benefiting from this interfacial engineering, Li + transport kinetics are markedly accelerated, parasitic electrolyte decomposition is suppressed, and both the rate capability and cycling stability of the graphite anode are significantly improved. The regenerated graphite anode delivers an initial Coulombic efficiency of 86.73% and reversible capacities of 370.6, 336.1, and 206.9 mAh g −1 at 0.1C, 1C, and 2 C, respectively, with 90.13% capacity retention after 700 cycles at 1 C, demonstrating performance comparable to that of commercial graphite. Life cycle assessment (LCA) further confirms the environmental and economic advantages of this low-temperature catalytic process, offering a green and feasible pathway for the closed-loop high-value utilization of spent graphite. The constructed porous nitrogen-doped graphene-like carbon (PNGC) layer repairs surface defects of spent graphite, induces the formation of a Li 3 N-rich stable SEI, and provides fast Li + transport channels, synergistically enhancing the electrochemical performance of regenerated graphite. Download: Download high-res image (337KB) Download: Download full-size image
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yao Li,Biyu Jin,Keyin Wang,Lina Song,Lanhui Ren,Yang Hou,Xiang Gao,Xiaoli Zhan,Qinghua Zhang
The rational design of stable binders targeting silicon electrodes with high theoretical capacity is vital for their superior electrochemical performance. Owing to the drastic volume change of silicon electrode upon long-term cycling, unstable SEI layer accompanying with low initial Coulombic efficiency (ICE) deteriorate the battery performance severely. In this case, we propose a 3D network binder (SHA) by weaving two anionic polysaccharides (i.e., hyaluronic acid (HA) and soluble soybean polysaccharides (SSPS)) via supramolecular interactions. Driven by the distinct chain flexibility, the two polysaccharides microphase-separate into internal buffer region (hard SSPS) and external restricted region (soft HA), resulting in double-layer network of SHA. The resulted hard/soft scaffold can not only significantly confine the disintegrated Si electrodes, but also guarantee a 3D continuous ion transportation circuit. Consequently, the SHA binder effectively assists the formation of stable SEI layer and achieves an excellent ICE up to 92.67%, leading to a satisfying rate capability and stable cycling performance for 250 cycles at 2 A g −1 , with a capacity decay rate of 0.24% per cycle. This novel and facile strategy delivers a perspective binder design through alternative combination of anionic, cationic and neutral polysaccharides for high performance Si anodes.
研究领域:
材料科学
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电化学
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能源存储
·
纳米技术
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DOI
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 9
·期 9
·5606-5618
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IF 11.301
Qingping Wu,Zhenguo Yao,Aochen Du,Han Wu,Minsong Huang,Jun Xu,Fahai Cao,Chilin Li
The fragility of the natural solid electrolyte interphase (SEI) and deformability of the naked Li anode cannot meet the requirements of high coulombic efficiency (CE) and long-period cycling for Li metal batteries (LMBs). Accordingly, conductive porous anode hosts with surface decoration/defect modulation appear to be an effective solution to restrain the growth of Li dendrites. Herein, we propose an unusual oxygen-defect-rich nanoporous MgOx coating bonded with carboxyl-rich carbon wires (MgOx–C), which act as a 3D monolithic host and artificial SEI film simultaneously, to achieve dendrite-free LMBs. The enrichment of the lithiophilic (carboxyl groups) and anionphilic (oxygen defects) sites could homogenize the Li deposition process, accommodate the anode volume variation, and mitigate the depletion of the space charge. The highly defective MgOx enabled fast charge transfer, thus result in a high-rate Li plating performance. The initial nucleation and following plating behaviors of Li were significantly optimized by the conversion and alloying reactions between the Li and MgOx domains. The resultant Li@MgOx–C electrode enabled a stable Li plating/stripping process with a low overpotential and high CE, even under the high plating capacity of 10 mA h cm−2 and high current density of 15 mA cm−2.
研究领域:
材料科学
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能源存储技术
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DOI
高影响因子
Energy Storage Materials
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2022
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IF 20.831
Yunrui Zhang,Wenbo Wang,Meiling Hou,Yantao Zhang,Yaying Dou,Zehua Yang,Xiaoyang Xu,Haining Liu,Shanlin Qiao
Li metal batteries have won the fame for the enlarged cell potential and higher theoretical specific capacity. Nevertheless, the commercial implementation is still confronted with inevitable Li dendritic growth and depressed Coulombic efficiency. The Li + transfer behavior is the vital factor to ameliorate the durability of solid electrolyte interphase (SEI). Herein, a self-exfoliated TpTG covalent organic framework (COF) was developed to construct an artificial SEI film. The versatile cationic-skeleton of TpTG could spontaneously drive the formation of nano-mesh with thickness of 3∼6 nm, and facilitate uniform dispersibility on the Li metal surface. Moreover, the 7 Li solid-state nuclear magnetic resonance spectra, Fourier-transform infrared spectra, and density functional theory calculations have identified the energetic lithiophilicity and TFSI – repulsion features. The Cl – coordinated TpTG endowed with abundant lithiophilic sites can reconfigure the charge distribution and expedite the uniform Li + migration adjacent to the electrode|electrolyte interface. The uniform Li + flux distribution redounds to reversible lithium stripping/plating and tames the dendrite formation especially at high-rate protocols. The overwhelming evidences of lower polarization, prolonged lifespan, and compact Li deposition, corroborate the practicability of self-exfoliated TpTG to achieve the goal of high-energy-density Li metal batteries.
研究领域:
材料科学
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电化学
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DOI
高影响因子
Advanced Energy Materials
·
2024
·
IF 24.4
Shulan Mao,Jiahui Zhang,Jiale Mao,Zeyu Shen,Ziren Long,Shichao Zhang,Qian Wu,Hao Cheng,Yingying Lu
Silicon nanoparticles (SiNPs) show great promise as high-capacity anodes owing to their ability to mitigate mechanical failure. However, the substantial surface area of SiNPs triggers interfacial side reactions and solid electrolyte interphase (SEI) permeation during volume fluctuations. The slow kinetics at low temperatures and the degradation of SEI at high temperatures further hinder the practical application of SiNPs in real-world environments. Here, these challenges are addressed by manipulating the solvation structure through molecular space hindrance. The electrolyte enables anions to aggregate in the outer Helmholtz layer under an electric field, leading to rapid desolvation capabilities and the formation of anion-derived SEI. The resulting double-layer SEI, where inorganic nano-clusters are uniformly dispersed in the amorphous structure, completely encapsulates the particles in the first cycle. The ultra-high modulus of this structure can withstand stress accumulation, preventing electrolyte penetration during repeated expansion and contraction. As a result, SiNPs-based batteries demonstrate exceptional electrochemical performance across a wide temperature range from −20 to 60 °C. Moreover, the assembled 80 mAh SiNPs/LiFePO 4 pouch cells maintain a cycling retention of 85.6% after 150 cycles, marking a significant step forward in the practical application of silicon-based batteries.
研究领域:
材料科学
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电化学
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DOI
高影响因子
CERAMICS INTERNATIONAL
·
2019
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IF 3.45
Yaru Li,Ruyi Wang,Jiwei Zhang,Jianping Chen,Chenqiang Du,Tianhua Sun,Jian Liu,Chunhong Gong,Jianhui Guo,Laigui Yu,Jingwei Zhang
For electrospun silicon/carbon nanofiber composites, the surface precipitation of silicon nanoparticles can cause poor cycle stability. To solve this, a carbon-coated silicon/carbon nanofiber (Si/C@C) composite with a ‘sandwich’ structure is constructed by hydrothermal reaction of glucose and an electrospun silicon/carbon nanofiber, followed by high-temperature carbonization. The effects of the thickness of the carbon coating layer and calcining temperature on the electrochemical performance are studied. The results showed that carbon is uniformly and continuously coated on the surface of the composite fibers, which avoid direct exposure of precipitated silicon on the surface of the nanofibers to the electrolyte, reduce the occurrence of side reactions and is conducive to the stable formation of SEI films. At the same time, the carbon shell inhibit the volume expansion of silicon to a certain extent and improve the conductivity of the composites. Consequently, the obtained Si/C@C exhibit good rate performance and cycle stability. With the optimised carbon coating thickness and calcination temperature, the obtained electrodes deliver a reversible capacity of 1120 and 683 mA h g -1 at a current density of 0.1 and 2 A g -1 respectively, and a specific capacity of 602 mAh∙g -1 at a current density of 1 A g -1 after 100 cycles, a capacity retention rate of 80%. The facilely synthesised Si/C@C composite shows potential applications in high-capacity silicon-based anode materials .
研究领域:
材料科学
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电化学
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DOI
高影响因子
ChemSusChem
·
2023
·Vol. 16
·期 10
·e202300186
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IF 8.4
Hanxiao Zhou,Tianhui Li,Wenjing Liu,Zhihao Guo,Zihao Su,Jingjing Gao,Meizhen Qu,Gongchang Peng
Graphical Ineffable : As an additive for lithium anodes, N , O -bis(trimethylsilyl)acetamide is proposed to suppress the appearance of lithium dendrites and volume expansion. With the high-voltage (4.3 V) and high-loading (6 mg cm −2 ) NCM622 cathode, the full battery shows excellent cycling performance. It has superior properties that enable the development of lithium metal batteries in practical applications. Owing to the strong energy advantage of lithium anodes, the development of lithium-metal batteries has become an inevitable trend. However, plagued by the instability of solid-electrolyte interphase (SEI) films, lithium metal anodes face challenges such as lithium dendrite formation and volume expansion. Studies have proven that modulating the composition and structure of SEI films by using electrolyte additives is a convenient and valid method. Currently, it is widely accepted that fluoride is an effective additive but, based on the high cost of fluoride production and environmental concerns, the development of fluoride-free additives is of great significance. In this work, the bifunctional additive N , O -bis(trimethylsilyl)acetamide (BSA) is proposed, which can build up a SEI layer that is rich in SiO x and Li 3 N on the surface of the lithium anode to control the deposition behavior of lithium and clean the electrolyte of HF to protect the electrode. The experimental results indicate that BSA suppresses the generation of lithium dendrites and controls the volume expansion of lithium anodes. Moreover, compared with the commonly used carbonate electrolytes, the battery containing BSA has the best overall performance. Methodologically, the results can be extended to other additives containing Si−O functional groups to replace the same type of fluorine-containing additives.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2022
·
IF 4.598
Han He,Yue Wang,Meng Li,Jingyi Qiu,Yuehua Wen,Junhong Chen
The operation of lithium–ion batteries (LIBs) at low temperature is hampered by decreased electrical conductivity and delayed electrode reaction kinetics. Due to its positive solid electrolyte interphase (SEI) formation properties, fluoroethylene carbonate (FEC) is one of the most widely researched additives for LIBs. Herein, charge–discharge tests, electrochemical impedance spectroscopy scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X–ray photoelectron spectroscopy (XPS) were used to investigate the effect of FEC on LCO/Li cells. According to SEM, TEM and XPS results, the addition of FEC results in the formation of a thin and stable cathode–electrolyte interface (CEI) film on the surface of the LCO electrode. Charge–discharge curves show that adding FEC to the electrolyte reduces polarization while increasing the discharge capacity. At −40 °C, the discharge capacity in electrolyte with 10 wt% FEC is 75.3 % that at room temperature and only 46.8 % without FEC at 1C. LiF is the main component of the FEC electrochemistry that forms a CEI, which has a low interfacial resistance and improves the ionic conductivity of the electrolyte, thus facilitating the performance of the battery at low temperature.
研究领域:
材料科学
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电化学
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DOI
高影响因子
Small
·
2026
·
IF 11.8
Chenlu Xu,Tengtao Hu,Xiang Yan,Binyu Lu,Tiansheng Chen,Yang Xia,Jun Zhang,Xinhui Xia,Wenkui Zhang,Yongping Gan,Ruyi Fang,Min Fan,Xinping He,Xinyong Tao,Hui Huang
In situ polymerized gel polymer electrolytes (GPEs) offer a promising strategy for lithium metal batteries, as they combine high ionic conductivity of liquid electrolytes with good mechanical stability of solid electrolytes. However, the composition evolution of GPEs with the resting period and the subsequent formation of solid electrolyte interphase (SEI) remains poorly understood. Herein, the influence of the resting time on the mechanical properties, lithium-ion transport kinetics, and SEI stability of GPEs is systematically investigated. By optimizing the resting time, the premature decomposition of fluorinated additives is revealed to be suppressed, and interfacial reactions are steered toward the formation of a robust SEI rich in LiF. The as-formed GPEs exhibit a high ionic conductivity of 1.96 × 10 −3 S cm −1 and a Li + transfer number of 0.67 at 30°C. As a result, Li||Li symmetric cells achieve stable cycling for over 2600 h, while LiFePO 4 ||Li full cells retain 94.68% of initial capacity after 1000 cycles at 1 C. This work elucidates the role of the resting time in modulating electrolyte chemical composition and SEI formation, providing a practical approach from a new perspective for developing long-life quasi-solid-state lithium metal batteries.
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zhaojun Meng,Ke Wang,Haotian Bai,Lijun Han,Zhiwen Yang,Yanrong Liu
Lithium-mediated nitrogen reduction reaction (Li-NRR) is a promising reaction pathway to realize green ammonia production. However, there is a lack of clear understanding on how solid electrolyte interphase (SEI) membranes affects Li-NRR performance. The effects of different lithium salts on the SEI layer were investigated in this work. Among lithium tetrafluoroborate (LiBF 4 ), lithium perchlorate (LiClO 4 ), and lithium trifluoromethanesulfonate (LiOTf), LiOTf showed better ammonia synthesis performance. At 1 bar N 2 and −6 mA cm −2 current density, the faraday efficiency (FE) and ammonia production rate reached 16.94 ± 0.67 % and 3.51 ± 0.14 nmol s −1 cm −2 , respectively. Conversely, the LiBF 4 electrolyte has the lowest NH 3 selectivity and rate under identical operating conditions, which are only 2.41 ± 0.16 % and 0.50 ± 0.03 nmol s −1 cm −2 . Cryo-electron microscopy reveals the influence of SEI nanostructures and chemical properties on the performance of lithium-mediated electrochemical synthesis of ammonia. The results of Cryo-electron microscopy showed that the SEI membranes of LiOTf electrolyte exhibited a reticular structure, which was favorable for N 2 adsorption, while the SEIs of LiClO 4 and LiBF 4 electrolytes had a lamellar and irregular planar structure, respectively. Molecular dynamics (MD) simulations and density functional theory (DFT) results showed that the LiOTf electrolyte can more easily generate a stable SEI membrane on the electrode surface. These findings highlight the importance of SEI structure in enhancing the reaction process, and thus provide valuable suggestions for the development of artificial SEI with specific structure.
研究领域:
材料科学
·
电化学
·
环境科学
✓ 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）