Construction of a LiF-Rich and Stable SEI Film by Designing a Binary, Ion-, and Electron-Conducting Buffer Interface on the Si Surface

Lv, Linze; Wang, Yan; Huang, Weibo; Li, Yuchen; Shi, Qiang; Zheng, Honghe

doi:10.1021/acsami.2c08019

Cited by 21 publications

(5 citation statements)

References 53 publications

(78 reference statements)

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“…This implies that the SEI layer formed on the surface of the Si anode is composed of organic species at the outer compartment and inorganic species close to Si, as generally observed for other Si-based anodes. 44,45 Interestingly, the oxygen (O) content is obviously lower for the SE-based cell, particularly after sputtering, e.g., 36.3% (SE) vs 46.1% (RE) before sputtering and 38% (SE) vs 54.8% (RE) after sputtering for 240 s. This indicates that the decompositions of the carbonate solvent are significantly suppressed by the addition of elemental sulfur, considering that other components (e.g., LiPF 6 and Si) are free from oxygen-related moieties. Furthermore, the fluorine (F) content is significantly higher for the SE electrolyte [e.g., 47.3% (SE) vs 35.1% (RE) before sputtering], suggesting the presence of fluorine-rich components (e.g., LiF; cf.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Domino Reactions Enabling Sulfur-Mediated Gradient Interphases for High-Energy Lithium Batteries

Tian,

Jin,

Song

et al. 2023

J. Am. Chem. Soc.

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Silicon (Si)-based anodes are currently considered a feasible solution to improve the energy density of lithium-ion batteries owing to their sufficient specific capacity and natural abundance. However, Si-based anodes exhibit low electric conductivities and large volume changes during cycling, which could easily trigger continuous breakdown/reparation of the as-formed solid-electrolyte-interphase (SEI) layer, seriously hampering their practical application in current battery technology. To control the chemoelectrochemical instability of the conventional SEI layer, we herein propose the introduction of elemental sulfur into nonaqueous electrolytes, aiming to build a sulfur-mediated gradient interphase (SMGI) layer on Si-based anodes. The SMGI layer is generated through the domino reactions (i.e., electrochemical cascade reactions) involving the electrochemical reductions of elemental sulfur followed by nucleophilic substitutions of fluoroethylene carbonate, which endows the corresponding SEI layer with strong elasticity and chemomechanical stability and enables rapid transportation of Li+ ions. Consequently, the prototype Si||LiNi0.8Co0.1Mn0.1O2 cells attain a high-energy density of 622.2 W h kg–1 and a capacity retention of 88.8% after 100 cycles. Unlike previous attempts based on sophisticated chemical modifications of electrolyte components, this study opens a new avenue in interphase design for long-lived and high-energy rechargeable batteries.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Domino Reactions Enabling Sulfur-Mediated Gradient Interphases for High-Energy Lithium Batteries

Tian,

Jin,

Song

et al. 2023

J. Am. Chem. Soc.

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“…Notably, this exchange reaction does not require thermal activation and can occur once the electrolyte preparation is completed. The reduction reaction mechanism of the P(BTMSB)F 4 1– monoanion involves single electron transfer to accept electron and combine Li + to form inorganic lithium salt (LiF), which is beneficial to the stabilization of the SEI film. , Moreover, the inorganic components within the SEI film possess superior properties in terms of Li + transport compared to organic components. This can be attributed to the tendency of the inorganic SEI substance to bond Li + in ionic bonds that facilitates hopping-type transport mechanisms .…”

Section: Resultsmentioning

confidence: 99%

Solid Electrolyte Interface Film-Forming and Surface-Stabilizing Bifunctional 1,2-Bis((trimethylsilyl)oxy) Benzene as Novel Electrolyte Additive for Silicon-Based Lithium-Ion Batteries

Cheng,

Li,

Liu

et al. 2023

ACS Appl. Mater. Interfaces

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The application of Si-based anodes in lithium-ion batteries (LIBs) has garnered significant attention due to their high theoretical specific capacity yet is still challenged by the substantial volume expansion of silicon particles during the lithiation process, resulting in the instability of the electrode–electrolyte interphase and deteriorative battery performance. Herein, an ortho(trimethylsilyl)oxybenzene electrolyte additive, 1,2-bis((trimethylsilyl)oxy) benzene (referred to as BTMSB), has been investigated as a bifunctional electrolyte additive for Si-based LIBs. The BTMSB can form a uniform and robust LiF-rich solid electrolyte interphase (SEI) on the surface of Si-based material particles, adapting the huge volume expansion of the Si-based electrode and facilitating lithium-ion transport. Additionally, the BTMSB demonstrates the ability to scavenge hydrofluoric acid (HF) to stabilize the electrode–electrolyte interphase. The SiO x /C∥Li batteries with 2% BTMSB exhibit improved cycle performance and current–rate capabilities, of which the capacity retention retains 69% after 400 cycles. Furthermore, Si-based anode cells with higher theoretical specific capacities (1C = 550 mAh g–1) and NCM523∥SiO x /C pouch cells are constructed and evaluated, displaying superior cycle performance. This work provides valuable insights for the development of effective electrolyte additives and the commercialization of high energy density LIBs with Si-based anodes.

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“…Various studies have reported the effect of adding Ag nanoparticles (NPs) or AgNWs to improve charge carrier mobility and conductivity with a Si based anode. To date, porous Si/AgNPs/C, SiO 2 mixed with AgNPs, carbon paper coated with AgNPs, Si@SiOx/AgNP composite electrode, Si electrode mixed with nitrogen-doped carbon and Ps, Si particles with a buffer layer, and AgNPs in a core–shell form have been used as anode materials. By applying wire-type Cu and Ag, electron conduction can be induced in line contact with carbon in point contact, which creates a more effective conductive network than other alternatives.…”

Section: Introductionmentioning

confidence: 99%

Tailored Silver Nanowires for Amplified Lithium-Ion Battery Performance and Inhibition of Lithium Dendrites in Silicon–Graphite–Silver Nanowire Composite Electrodes

Jeong,

Wang,

Nersisyan

et al. 2023

ACS Appl. Energy Mater.

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In Li ion batteries using Si-based anodes, silver nanowires (AgNWs) are centrifugally mixed to prevent the loss of an electron conduction path due to the expansion of Si. In this study, a robust conductive network is created by modifying AgNWs to a width of 50 nm and length of 25 μm, considering the constituents of the electrode microstructure and adjusting the concentration of polyvinylpyrolidine used as a binder. The variations in the electrode microstructure and the effect of AgNWs on Li behavior are examined. Distinct phase transformations and thermodynamically stable phases are estimated using density functional theory calculations based on a Li− Si−Ag ternary system. The incorporation of the AgNWs network into Si anodes offers multiple benefits including ultrafast electron transport, reduced charge and capacitance resistance, improved adhesion to the current collector, and suppressed Li dendrite formation. It enhances the specific capacity (15−18%) and adhesion force (86%). In particular, the 50 nm Si@Gr/C/AgNWs electrode exhibits the best performance (∼460 mAh g −1 ) and capacity retention characteristics (96%) at a current density of 0.1 A g −1 , with enhanced rate capability and charge efficiency, particularly at 1.6 A g −1 . The proposed AgNWs network will benefit highperformance and stable Si-based electrodes for advanced energy storage systems.

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Construction of a LiF-Rich and Stable SEI Film by Designing a Binary, Ion-, and Electron-Conducting Buffer Interface on the Si Surface

Cited by 21 publications

References 53 publications

Domino Reactions Enabling Sulfur-Mediated Gradient Interphases for High-Energy Lithium Batteries

Domino Reactions Enabling Sulfur-Mediated Gradient Interphases for High-Energy Lithium Batteries

Solid Electrolyte Interface Film-Forming and Surface-Stabilizing Bifunctional 1,2-Bis((trimethylsilyl)oxy) Benzene as Novel Electrolyte Additive for Silicon-Based Lithium-Ion Batteries

Tailored Silver Nanowires for Amplified Lithium-Ion Battery Performance and Inhibition of Lithium Dendrites in Silicon–Graphite–Silver Nanowire Composite Electrodes

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