Building a rigid-soft coupling interphase by a reduction–oxidation collaborative approach with lithium difluorobis(oxalato) phosphate additives

Wang, Peng; Wu, Shumin; Li, Jingni; Cui, Xiaoling; Li, Chunlei; Zhao, Dongni; Li, Shiyou

doi:10.1039/d2ta08386h

Cited by 4 publications

(3 citation statements)

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“…As reported, a stable SEI is established as a prerequisite for realizing the practical application of silicon-based anode cells. − Thus, various types of electrolyte additives which are usually able to preferentially form stable SEI on the anode surface before the decomposition of electrolyte body are used in Si-based LIBs. , It is reported that additives of fluoroethylene carbonate (FEC), vinyl carbonate (VC), (pentafluorophenyl)borane (TPFPB), lithium bis(oxalate)borate (LiBOB), and lithium difluorobisoxalate phosphate (LiDFBOP) have shown positive effects on improving the cycle life of Si-based anodes. − FEC has once been considered as the most promising additive because its reduction products are mainly composed of polyolefins and LiF, and its derived SEI has characteristics of flexibility and high ionic conductivity. However, FEC will decompose at high temperature to generate gaseous products, especially HF, which is very destructive to cycling and safety performances .…”

Section: Introductionmentioning

confidence: 99%

Building a Flexible and Highly Ionic Conductive Solid Electrolyte Interphase on the Surface of Si@C Anodes by Binary Electrolyte Additives

Song,

Li,

Wang

et al. 2023

ACS Appl. Mater. Interfaces

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Si@C as a high specific capacity anode material for lithium batteries (LIBs) has attracted a lot of attention. However, the severe volume change during lithium de-embedding causes repeated rupture/reconstruction of the solid electrolyte interphase (SEI), resulting in poor cycling stability of the Si-based battery system and thus hindering its application in commercial batteries. Using electrolyte additives to form an excellent SEI is considered to be a cost-effective method to meet this challenge. Here, the classical film-forming additive vinyl carbonate (VC), and the newly emerging lithium salt additive lithium difluorophosphate (LiDFP), are chosen as synergistic additives to improve the electrode–electrolyte interface properties. Final results show that the VC additive generates flexible polycarbonate components at the electrode/electrolyte interface, preventing the fragmentation of Si particles. However, the organic components show high impedance, inhibiting the fast transport of Li+. This defect can be supplemented from the decomposition substances of the LiDFP additive. The derived inorganic products, such as LiF and Li3PO4, can strengthen the reaction kinetics of the electrode, reduce the interfacial impedance, and promote the Li+ transport. Thus, the synergistic effect of VC and LiDFP additives builds an effective SEI with good flexibility and high ionic conductivity and then significantly improves the cycling and rate stability of Si@C anodes. The experimental results show that the utilization of LiDFP and VC additives to modify the Si@C anode interface enhances the capacity retention of the Si@C/Li half-cell after 100 cycles from 68.2% to 85.1%. Besides, the possible mechanism of action between VC and LiDFP is proposed by using the spectral characterization technique and density functional theory (DFT) calculations. This research opens up a new possibility for improvement of SEI, and provides a simple way to achieve high-performance Si-based LIBs.

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Section: Introductionmentioning

confidence: 99%

Building a Flexible and Highly Ionic Conductive Solid Electrolyte Interphase on the Surface of Si@C Anodes by Binary Electrolyte Additives

Song,

Li,

Wang

et al. 2023

ACS Appl. Mater. Interfaces

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“…To further validate the benefits of the RF method, leakage current testing provides evidence of the performance advantages associated with the interface film formed via the RF method in terms of Li + conductivity. As shown in Figure c, the leakage current through RF (0.02481 mA) is lower than that through NF (0.03333 mA), indicating that the interface film generated using the RF method can mitigate the occurrence of side reactions on the electrode surface . The evolution of the CEI layer is further elucidated through EIS.…”

Section: Resultsmentioning

confidence: 94%

“…As shown in Figure 3c, the leakage current through RF (0.02481 mA) is lower than that through NF (0.03333 mA), indicating that the interface film generated using the RF method can mitigate the occurrence of side reactions on the electrode surface. 42 The evolution of the CEI layer is further elucidated through EIS. An LNMC622||Li battery was used to investigate the influence of different film-forming voltage scopes on the positive electrode interface, as shown in Figure 3d.…”

Section: Electrochemical Performances Of Lnmc622||limentioning

confidence: 99%

Precycling Strategy in Suitable Voltage to Improve the Stability of Interfacial Film and Suppress the Decline of LiNi_0.6Mn_0.2Co_0.2O₂ Cathode at Elevated Temperatures

Li,

Yang,

Quan

et al. 2024

ACS Appl. Mater. Interfaces

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Layered ternary oxide LiNi x Mn y Co1–x–y O2 is a promising cathode candidate for high-energy lithium-ion batteries (LIBs). However, the capacity of LIBs is significantly restricted by several factors, including the repeated dissolution-regeneration of the interfacial film at high temperatures, the dissolution of transition metals, and the increase of impedance. Herein, a new precycling strategy in suitable voltage scope at room temperature is proposed to construct a uniform, thermally stable, and insoluble cathode-electrolyte interface (CEI), which helps to maintain stable cycling performances at high temperatures. Specifically, after 5 precycles in the range of 3.85–4.3 V at room temperature, a CEI layer containing numerous inorganic components and oligomers is formed on the surface of LiNi0.6Mn0.2Co0.2O2. Subsequently, the harmful side reactions are effectively suppressed, endowing the cell with an excellent capacity retention of 84.67% after 50 cycles at 0.5C and 55 °C, much higher than that of 65.61% under the conventional film-forming process conditions. This work emphasizes the crucial role of the precycling strategy in regulating the characteristics of CEI layer on the surface of cathode electrode, opening up a new avenue for the high-temperature application of positive electrodes of LIBs.

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Mitigating volume expansion of silicon-based anode through interfacial engineering based on intermittent discharge strategy

Li,

Zhu,

Quan

et al. 2024

Journal of Energy Chemistry

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Building a rigid-soft coupling interphase by a reduction–oxidation collaborative approach with lithium difluorobis(oxalato) phosphate additives

Abstract: Optimizing the properties of solid electrolyte interphase (SEI) layers on graphite electrodes is a crucial method for influencing the performance of cells. However, most studies ignore any potential synergistic effects...

Cited by 4 publications

References 42 publications

Building a Flexible and Highly Ionic Conductive Solid Electrolyte Interphase on the Surface of Si@C Anodes by Binary Electrolyte Additives

Building a Flexible and Highly Ionic Conductive Solid Electrolyte Interphase on the Surface of Si@C Anodes by Binary Electrolyte Additives

Precycling Strategy in Suitable Voltage to Improve the Stability of Interfacial Film and Suppress the Decline of LiNi_0.6Mn_0.2Co_0.2O₂ Cathode at Elevated Temperatures

Mitigating volume expansion of silicon-based anode through interfacial engineering based on intermittent discharge strategy

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Building a rigid-soft coupling interphase by a reduction–oxidation collaborative approach with lithium difluorobis(oxalato) phosphate additives

Abstract: Optimizing the properties of solid electrolyte interphase (SEI) layers on graphite electrodes is a crucial method for influencing the performance of cells. However, most studies ignore any potential synergistic effects...

Cited by 4 publications

References 42 publications

Building a Flexible and Highly Ionic Conductive Solid Electrolyte Interphase on the Surface of Si@C Anodes by Binary Electrolyte Additives

Building a Flexible and Highly Ionic Conductive Solid Electrolyte Interphase on the Surface of Si@C Anodes by Binary Electrolyte Additives

Precycling Strategy in Suitable Voltage to Improve the Stability of Interfacial Film and Suppress the Decline of LiNi0.6Mn0.2Co0.2O2 Cathode at Elevated Temperatures

Mitigating volume expansion of silicon-based anode through interfacial engineering based on intermittent discharge strategy

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Precycling Strategy in Suitable Voltage to Improve the Stability of Interfacial Film and Suppress the Decline of LiNi_0.6Mn_0.2Co_0.2O₂ Cathode at Elevated Temperatures