Study of the formation and evolution of solid electrolyte interface via in-situ electrochemical impedance spectroscopy

Wang, Peng; Yan, Dingshun; Wang, Caiyun; Ding, Hao; Dong, Hong; Wang, Jie; Wu, Shumin; Cui, Xiaoling; Li, Chunlei; Zhao, Dongni; Li, Shiyou

doi:10.1016/j.apsusc.2022.153572

Cited by 45 publications

(32 citation statements)

References 37 publications

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“…Moreover, the EIS and physical characterization coupled strategy play a vital role in relating SEI impedance to its composition. Wang et al associated in situ EIS and DRT with XPS to study the formation and evolution of SEI, which found that the high-frequency and midfrequency semiarcs derived from the inorganic and organic components, respectively . In Figure b, the resistance of organic layer first increases and then decreases, accompanying with the increase of the resistance of inorganic layer.…”

Section: Application Of Eis To Lib’s Aging Studymentioning

confidence: 99%

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Application of Electrochemical Impedance Spectroscopy to Degradation and Aging Research of Lithium-Ion Batteries

Peng

Wei³

et al. 2023

J. Phys. Chem. C

100

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An in-depth understanding of battery degradation and aging in-Operando not only plays a vital role in the design of battery managing systems but also helps to ensure safe use and manufacturing optimization of lithium-ion batteries (LIBs) in large-scale applications. Electrochemical impedance spectroscopy (EIS) is a nondestructive method which unravels electrode kinetic processes inside the batteries in different time domains, including charge-transfer reactions, interfacial evolutions, and mass diffusions. It has become a powerful diagnosis and pre/prognosis tool in battery aging research, as it provides important insight into the changes of internal electrochemical processes by correlating the impedance evolution to degradation mechanisms. This review gives a critical overview on rapidly developing impedance techniques for degradation and aging investigation of Li-ion batteries. The EIS variations of LIBs at different aging conditions of calendar aging and accelerated aging are systematically summarized. In addition, the working principles, data validation, and modeling methods, including equivalent circuit model (ECM), distribution of relaxation times (DRT), and transmission line model (TLM), of classical EIS and dynamic EIS are elaborately concluded. Finally, the challenges and perspectives of further application of EIS in the aging research of LIBs are presented.

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Section: Application Of Eis To Lib’s Aging Studymentioning

confidence: 99%

“…The impedance and time constant of SEI could be easily obtained from EIS plot by ECM or DRT. At present, it has been commonly used to characterize SEI performance, evaluate novel electrolyte, study SEI formation, − and monitor SEI evolution …”

Section: Application Of Eis To Lib’s Aging Studymentioning

confidence: 99%

Application of Electrochemical Impedance Spectroscopy to Degradation and Aging Research of Lithium-Ion Batteries

Peng

Wei³

et al. 2023

J. Phys. Chem. C

100

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“…In a liquid electrolyte, the structure and properties of the solvents, Li salt, and additives determine which components are preferentially decomposed to form the SEI film. Furthermore, the chemical compositions and structure of the formed SEI have very important influences on the chemical and mechanical stability of the Li/electrolyte interface and Li deposition/stripping behavior. ,− Therefore, introducing additives into the electrolyte to adjust the compositions of SEI films is an effective strategy to construct a stable Li metal anode. In this work, we introduce the HCBD molecule into an ether-based electrolyte to form a LiCl-rich ionic conductive layer on the Li anode surface and thus stabilize the Li metal anode, based on the DFT calculation’s results that this molecule can preferentially react with the Li anode to generate LiCl species.…”

Section: Results and Discussionmentioning

confidence: 99%

Hexachloro-1,3-butadiene as a Functional Additive for Constructing an Efficient Solid Electrolyte Interface Layer for Long-Life Stable Li Anodes

Duan

Zhang

et al. 2022

ACS Appl. Mater. Interfaces

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Lithium (Li) metal is considered as one of the attractive anodes for next-generation high-energy-density batteries due to its ultrahigh theoretical specific capacity and low potential. However, many great challenges including uncontrolled dendrite growth and undesired side reactions during repeated cycling still seriously hinder its practical application in Li metal secondary batteries. Herein, we report the hexachloro-1,3-butadiene (HCBD) molecule as a functional additive to stabilize the Li anode by forming a stable solid electrolyte interface (SEI) layer with high Li ion conductivity via in situ surface and electrochemical reactions. Density functional theory calculations demonstrate that HCBD can preferentially react with the Li anode, which generates an ionic conducting species (LiCl) into an SEI layer. The LiCl-rich SEI layer effectively regulates Li+ deposition/stripping kinetics and then induces uniform nucleation of Li+ and reduces the side reactions between the Li anode and electrolyte. With an optimal amount of HCBD in an ether-based electrolyte, an excellent cycling lifespan (7000 h) was achieved with a low hysteresis voltage of ∼10 mV at 1.0 mA cm–2 in a Li||Li symmetrical cell. Furthermore, the LiFePO4-based cell with the additive-functionalized Li anode displays obviously improved cycling stability (with a high specific capacity of 141.1 mAh g–1 after 350 cycles at 1 C).

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“…A CHI660E electrochemical workstation (Chenhua, Shanghai, China) through a three-electrode system was used for the following tests, using a Si@Graphite@C electrode as the working electrode and lithium sheets as both the reference electrode as well as the counter electrode, respectively. Electrochemical impedance spectroscopy (EIS) measurements of cells with different electrolytes were tested after the fifth cycle and 100th cycle over the frequency range from 10 mHz to 100 kHz. − PRI-EIS was performed in the potential range of open circuit potential to 0.01 V, in the frequency range of 10 mHz–100 kHz.…”

Section: Methodsmentioning

confidence: 99%

Improving Toleration of Volume Expansion of Silicon-Based Anode by Constructing a Flexible Solid-Electrolyte Interface Film via Lithium Difluoro(bisoxalato) Phosphate Electrolyte Additive

Wang

Zhang

et al. 2022

ACS Sustainable Chem. Eng.

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The silicon (Si) anode is considered one of the most promising candidates among many novel anode materials in lithium-ion batteries owing to its high theoretical capacity and earth abundancy. Nonetheless, a large volume expansion of Si particles appears with cycling, prompting unceasing breakage/reformation of the solid-electrolyte interface (SEI) and fast capacity degradation in traditional electrolytes. For the purpose of tolerating volume expansion for the Si anode, lithium difluoro(bisoxalato) phosphate (LiDFBOP) was adopted in the standard (STD) electrolyte based on LiPF6. Density functional theory (DFT) calculations, Young’s modulus from atomic force microscopy, potential-resolved in situ electrochemical impedance spectroscopy (PRI-EIS) measurement, and other characterizations proved that the formed SEI can inhibit volume expansion of a Si@Graphite@C anode. In the STD+2% LiDFBOP electrolyte, the solvation structure of Li(EC)2(PF6)1(DFBOP)1 is more likely to be produced, and this kind of solvation structure has stronger reducibility and easily participates in SEI formation. The 2% LiDFBOP additive increases the inorganic LiF component of SEI, which yields great advantages in regulating the uniform diffusion of Li+ ions passing through the SEI. Besides, the organics containing P and F atoms are also abundant in SEI, which has greater flexibility and can tolerate volume expansion of the Si@Graphite@C anode. Therefore, the STD+2% LiDFBOP electrolyte can improve the electrochemical performances of Si@Graphite@C/Li half-cells. This work has practical implications not only for the molecular design of novel lithium salt but also for the constructions of SEI and electrolyte systems compatible with the Si@Graphite@C anode.

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Study of the formation and evolution of solid electrolyte interface via in-situ electrochemical impedance spectroscopy

Cited by 45 publications

References 37 publications

Application of Electrochemical Impedance Spectroscopy to Degradation and Aging Research of Lithium-Ion Batteries

Application of Electrochemical Impedance Spectroscopy to Degradation and Aging Research of Lithium-Ion Batteries

Hexachloro-1,3-butadiene as a Functional Additive for Constructing an Efficient Solid Electrolyte Interface Layer for Long-Life Stable Li Anodes

Improving Toleration of Volume Expansion of Silicon-Based Anode by Constructing a Flexible Solid-Electrolyte Interface Film via Lithium Difluoro(bisoxalato) Phosphate Electrolyte Additive

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