In Situ TEM Observation of Local Phase Transformation in a Rechargeable LiMn<sub>2</sub>O<sub>4</sub> Nanowire Battery

Lee, So‐Yeon; Oshima, Yoshifumi; Hosono, Eiji; Zhou, Haoshen; Kim, Kyungsu; Chang, Hansen; Kanno, Ryoji; Takayanagi, Kunio

doi:10.1021/jp409032r

Cited by 68 publications

(61 citation statements)

References 30 publications

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“…For example, extensive efforts have been made to study the SEI layer on a number of anode materials using in situ electrochemical cells coupled with an electron microscope. 13 −19 These studies reveal the growth of layers but often neglect reporting information related to the number of Coulombs of charge passed through the cells making quantitative analysis of the data difficult. [14][15][16]18 In addition, there have been numerous groups working with nuclear magnetic resonance (NMR) spectroscopy which enables chemical specificity but lacks depth resolution.…”

Section: ■ Introductionmentioning

confidence: 99%

Direct Determination of Solid-Electrolyte Interphase Thickness and Composition as a Function of State of Charge on a Silicon Anode

et al. 2015

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With the use of neutron reflectometry, we have determined the thickness and chemistry of the solid-electrolyte interphase (SEI) layer grown on a silicon anode as a function of state of charge and during cycling. We show the chemistry of this SEI layer becomes more LiF like with increasing lithiation and more Li−C−O−F like with delithiation. More importantly, the SEI layer thickness appears to increase (about 250 Å) as the electrode becomes less lithiated and thins to 180 Å with increasing Li content (Li 3.7 Si). We attribute this "breathing" to the continual consumption of electrolyte with cycling.

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Section: ■ Introductionmentioning

confidence: 99%

Direct Determination of Solid-Electrolyte Interphase Thickness and Composition as a Function of State of Charge on a Silicon Anode

et al. 2015

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“…This phase could be converted to three-layered Li 1−x CoO 2 immediately during reversible Li intercalation. [291,292] S. Lee et al [291] revealed that three phases (cubic, tetragonal and orthorhombic) took part in the phase transition of LiMn 2 O 4 through in situ TEM analysis. [280,281] The H2a appearing in the composition range of x = 0-0.5 bridged the H1 and H2.…”

Section: Stress Development Arising From the Cathode Sidementioning

confidence: 99%

Interfacial Incompatibility and Internal Stresses in All‐Solid‐State Lithium Ion Batteries

Liu

et al. 2019

Advanced Energy Materials

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The continuous depletion of fossil fuels, the increase of oil prices, and the need to decrease CO 2 emissions have stimulated intensive research on developing alternative renewable and clean energy sources. [1] Among these alternative energy sources, rechargeable Li-ion batteries (LIBs) are one of the promising candidates. To date, the LIBs basically consisting of a positive electrode (cathode), an electrolyte, and a negative electrode (anode) have widespread applications, such as portable electronic devices, pure electric vehicles (PEVs), and hybrid electric vehicles (HEVs). [2] The state-of-the-art electrolytes are usually the lithium salts (LiPF 6 , LiBF 4 , and LiCF 3 SO 3 ) dissolved in organic solvents, i.e., ethylene carbonate, propylene carbonate, polyethylene oxide, and dimethyl carbonate, [3] which exhibit excellent wetting of the electrodes and produce a fast transfer of Li + ions upon charging and discharging. However, they suffer from flammability, poor electrochemical stability, limited temperature range of operation, and low power density. [4] There is an ever-increasing demand for batteries with a higher energy and power density, although current LIBs offer volumetric and gravimetric energy densities up to 770 Wh L −1 and 260 Wh kg −1 , respectively. [5] To improve the energy/power density of LIBs, one way is to adopt high-potential cathode materials such as LiNi 0.5 Mn 1.5 O 4 (LNMO). The high-voltage plateau of LNMO (≈4.7 V vs Li/Li + ) makes its energy density 20-30% higher than the energy density of commercial LiCoO 2 and LiFePO 4 . [6] However, successful commercialization of the LNMO is restricted in high-energy LIBs due to electrolyte decomposition and side reaction of the cathodes and liquid electrolytes when operating at high voltages. [7,8] The other way to improve the energy/power density is to replace the conventional graphite anode with Li metal. The Li metal, with a low anode potential (−3.04 V vs standard hydrogen electrode) and high specific capacity (3862 mAh g −1 for the Li anode versus 372 mAh g −1 for the graphite anode), [9][10][11] has been considered as the "Holy Grail" of battery technologies. When paired with sulfur and oxygen, the theoretical energy density of Li-S (≈2567 Wh kg −1 ) and Li-O 2 (≈3505 Wh kg −1 ) batteries is far higher than the theoretical energy density of conventional LIBs (≈387 Wh kg −1 ). [12][13][14][15] When Li metal approaches the liquid electrolytes, however, unstable Li/electrolyte interface Rechargeable Li-ion batteries (LIBs) are electrochemical storage device widely applied in electric vehicles, mobile electronic devices, etc. However, traditional LIBs containing liquid electrolytes suffer from flammability, poor electrochemical stability, and limited operational temperature range. Replacement of the liquid electrolytes with inorganic solid-state electrolytes (SSEs) would solve this problem. However, several critical issues, such as poor interfacial compatibility, low ionic conductivity at ambient temperatures, etc., need to be surmounted befor...

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“…[25,[56][57][58] However, the atomic behavior of Li ion that determines LIB's performance is hardly imaged by TEM owing to its weak scattering power of electrons. ABF-STEM, in which the contrast has a low scaling rate with the atomic number, allows simultaneous imaging of light and heavy elements.…”

Section: Intercalation Reactionmentioning

confidence: 99%

“…In addition to studies of 1D channel materials, there has been some work using in situ TEM to study the electrochemical reaction dynamics of 2D and 3D transport materials . However, the atomic behavior of Li ion that determines LIB's performance is hardly imaged by TEM owing to its weak scattering power of electrons.…”

Section: Intercalation Reactionmentioning

confidence: 99%

Atomic‐Scale Monitoring of Electrode Materials in Lithium‐Ion Batteries using In Situ Transmission Electron Microscopy

Shang

Wen

Xiao

et al. 2017

Advanced Energy Materials

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Lithium‐ion batteries (LIBs) are energy storage devices that have received much attention because of their high energy density, high power capacity, and long lifetime. However, even though they are used widely in daily life, their cycling life and safety need further improvement. Understanding the reaction mechanisms and the structural degradation during the lithiation/delithiation process is a prerequisite to further improve the performance of LIBs. In situ transmission electron microscopy (TEM) allows one to monitor structural evolution at the atomic scale in real time, thus providing an unprecedented opportunity to characterize the lithiation reaction pathway in a nonequilibrium state during battery cycling. In this article, the recent advances with respect to elucidating the relationships of dynamic structural evolution, reaction kinetics, and performance of different nanostructured electrode materials at the atomic scale using in situ TEM, based on three representative reaction mechanisms, are described. Specifically, the three systems are intercalation reaction, conversion reaction, and alloying reaction. Based on the advances that have been made, it is expected that in situ TEM will play an indispensable role on future design of LIBs electrode materials.

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In Situ TEM Observation of Local Phase Transformation in a Rechargeable LiMn₂O₄ Nanowire Battery

Cited by 68 publications

References 30 publications

Direct Determination of Solid-Electrolyte Interphase Thickness and Composition as a Function of State of Charge on a Silicon Anode

Direct Determination of Solid-Electrolyte Interphase Thickness and Composition as a Function of State of Charge on a Silicon Anode

Interfacial Incompatibility and Internal Stresses in All‐Solid‐State Lithium Ion Batteries

Atomic‐Scale Monitoring of Electrode Materials in Lithium‐Ion Batteries using In Situ Transmission Electron Microscopy

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In Situ TEM Observation of Local Phase Transformation in a Rechargeable LiMn2O4 Nanowire Battery

Cited by 68 publications

References 30 publications

Direct Determination of Solid-Electrolyte Interphase Thickness and Composition as a Function of State of Charge on a Silicon Anode

Direct Determination of Solid-Electrolyte Interphase Thickness and Composition as a Function of State of Charge on a Silicon Anode

Interfacial Incompatibility and Internal Stresses in All‐Solid‐State Lithium Ion Batteries

Atomic‐Scale Monitoring of Electrode Materials in Lithium‐Ion Batteries using In Situ Transmission Electron Microscopy

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In Situ TEM Observation of Local Phase Transformation in a Rechargeable LiMn₂O₄ Nanowire Battery