In situ transmission electron microscopy for understanding materials and interfaces challenges in all-solid-state lithium batteries

Sun, Zhefei; Li, Miao; Xiao, Bo; Liu, Xiang; Lin, Haichen; Jiang, Bing; Liu, Haodong; Li, Meicheng; Peng, Dong‐Liang; Zhang, Qiaobao

doi:10.1016/j.etran.2022.100203

Cited by 44 publications

(28 citation statements)

References 121 publications

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“…Transmission electron microscopy (TEM) is an effective method to determine the structure of materials. 37 It can be seen that Ge particles were randomly tightly anchored in the carbon matrix, which is attributed to the synchronous formation of carbon (Figure 2a−d) and the Ge-132 reduction process. The interplane distance of Ge particles was 0.32 nm as measured by high-resolution TEM, corresponding to the (111) of Ge crystal planes.…”

Section: Resultsmentioning

confidence: 90%

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In Situ Synthesis of Germanium Particles Decorated in Conjugated N-doped Carbon Matrix: Boosting the Performance of the Lithium-Ion Battery

Zhang

Meng

et al. 2022

ACS Appl. Energy Mater.

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Germanium (Ge) has aroused great attention due to its high theoretical capacity, benign lithium diffusion, and low working potential. However, application of the Ge anode is hindered by volume expansion and the unstable solid electrolyte interphase (SEI) during the (de)lithiation process. Herein, Ge particles encapsulated tightly on an N-doped porous carbon matrix structure are obtained via a simple one-step in situ thermally driven reduction reaction of poly(vinylpyrrolidone) and carboxyethyl germanium sesquioxide. A protective N-doped carbon layer of suitable thickness is further rationally designed to improve the conductivity as well as enhance the transfer of lithium ions while alleviating the volume stress of Ge particles. The adsorption energy for the N-doped carbon obtained by density function theory (DFT) calculation has verified that heteroatom doping is helpful to considerable decrease the energy barrier of lithium ions and a remarkable electrochemical performance of the Ge electrode is achieved with this optimal designing. This facile easy-to-control method can further be applied for electrodes of silicon, tin, phosphorus etc., which have the volume expansion issue.

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Section: Resultsmentioning

confidence: 90%

“…Transmission electron microscopy (TEM) is an effective method to determine the structure of materials . It can be seen that Ge particles were randomly tightly anchored in the carbon matrix, which is attributed to the synchronous formation of carbon (Figure a–d) and the Ge-132 reduction process.…”

Section: Resultsmentioning

confidence: 99%

In Situ Synthesis of Germanium Particles Decorated in Conjugated N-doped Carbon Matrix: Boosting the Performance of the Lithium-Ion Battery

Zhang

Meng

et al. 2022

ACS Appl. Energy Mater.

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“…The typical cathode material for the all-solid-state Li–S battery is sulfur because of its low cost and high abundance. − However, the poor electronic and ionic conductivities of S limit the electrochemical performance of the battery utilizing S as cathode material. Li 2 S shows slightly higher electronic/ionic conductivity than that of bare S, and as a Li-containing molecular structure, it provides the possibility to combine with the Li-ion-free anode materials to fabricate SSBs. − …”

Section: Introductionmentioning

confidence: 99%

Origin of the High Conductivity of the LiI-Doped Li₃PS₄ Electrolytes for All-Solid-State Lithium–Sulfur Batteries Working in Wide Temperature Ranges

Wei

et al. 2022

Ind. Eng. Chem. Res.

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Sulfide electrolytes show great potential as solid electrolytes for all-solid-state batteries due to their high ionic conductivity and low interfacial resistance toward electrode materials. The structure of the P−S framework in the composition of sulfides plays a crucial role in the conductivity. Introducing LiI in the Li 3 PS 4 structure can tailor the P−S frameworks and thus achieve high ionic conductivities. Herein, the dopant of LiI is optimized by high-rotation milling, followed by a sintering route to achieve the highest Li-ion conductivity of 2.3 mS cm −1 for the Li 3 PS 4 -50% LiI electrolyte (also denoted as Li 7 P 2 S 8 I) among different compositions. The phase variations and structure evolution of the P−S frameworks in the LiI-doped Li 3 PS 4 electrolytes are carefully investigated in a combination of X-ray diffraction and Raman spectra. All-solid-state Li−S batteries using the prepared Li 7 P 2 S 8 I electrolyte combined with a nano Li 2 S cathode and a Li−In anode deliver a high initial discharge capacity of 739.7 mA h g −1 and sustain a discharge capacity of 517.7 mA h g −1 after 60 cycles with a capacity retention of 70.0% at 0.13 mA cm −2 at room temperature. When the operating temperature rises to 60 °C, it shows a higher discharge capacity of 862.8 mA h g −1 with fast capacity decay. However, it exhibits stable capacities and superior cycling performance under 0 °C over 70 cycles. Electrochemical impedance spectroscopy and in situ stack-pressure results find that the electrochemical performance differences of the assembled battery at different operating temperatures are associated with the interfacial resistance caused by volume changes. This work provides the strategy to obtain highly conductive sulfide electrolytes for SSBs and unravels the temperature effects on the electrochemical performance of all-solid-state Li−S batteries.

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“…Lithium (Li) metal has been pursued as the “Holy Grail” of anode materials for Li-based secondary batteries because of its high specific capacity and the lowest redox potential. − In general, during battery operations, a solid electrolyte interphase (SEI) film will be spontaneously generated on the surface of the Li metal anode due to the parasitic reactions between highly reactive Li and the electrolyte, protectively passivating the anode. − However, the SEI film formed in most electrolyte systems is unstable and suffers from repeated breakage/repair due to the volume change upon cycling. , This will lower the Coulombic efficiency (CE) by continuously consuming the active Li sources and electrolytes as well as trigger safety issues because of dendritic Li growth, severely limiting the application of Li metal anodes. , Therefore, constructing a robust artificial SEI film to improve the cyclability of Li metal anodes in practical Li metal batteries (LMBs) is of great importance. − …”

mentioning

confidence: 99%

“…4−6 However, the SEI film formed in most electrolyte systems is unstable and suffers from repeated breakage/repair due to the volume change upon cycling. 7,8 This will lower the Coulombic efficiency (CE) by continuously consuming the active Li sources and electrolytes as well as trigger safety issues because of dendritic Li growth, severely limiting the application of Li metal anodes. 9,10 Therefore, constructing a robust artificial SEI film to improve the cyclability of Li metal anodes in practical Li metal batteries (LMBs) is of great importance.…”

mentioning

confidence: 99%

Cationic Interfacial Layer toward a LiF-Enriched Interphase for Stable Li Metal Batteries

Jin

Cai

et al. 2022

ACS Energy Lett.

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Lithium (Li) metal is one of the most promising anode materials for next-generation high-energy rechargeable batteries but suffers from an unstable solid electrolyte interphase (SEI) and dendrite growth. Here, we design an interfacial layer through electrostatic integration of the cationic polymer poly(diallyldimethylammonium chloride) with commercial bamboo fibers (PBF) to precisely regulate the SEI at the molecular level. Numerous cationic sites exist on the surface of this PBF layer that adsorb electrolyte anions, which remarkably accelerates the decomposition kinetics of fluorinated salts in the electrolyte. Consequently, a LiF-enriched SEI film is developed, thus ensuring improved interfacial stability and cycling performance of the Li metal anode. The PBF-based symmetrical cell delivers a long-term cycling lifespan of more than 4800 h (∼12000 cycles) at 5 mA cm −2 . More importantly, the practical full cell with a low negative/positive capacity ratio (∼3.7) and a high-mass-loading cathode (2.7 mAh cm −2 ) exhibits enhanced cyclability of over 350 cycles.

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In situ transmission electron microscopy for understanding materials and interfaces challenges in all-solid-state lithium batteries

Cited by 44 publications

References 121 publications

In Situ Synthesis of Germanium Particles Decorated in Conjugated N-doped Carbon Matrix: Boosting the Performance of the Lithium-Ion Battery

In Situ Synthesis of Germanium Particles Decorated in Conjugated N-doped Carbon Matrix: Boosting the Performance of the Lithium-Ion Battery

Origin of the High Conductivity of the LiI-Doped Li₃PS₄ Electrolytes for All-Solid-State Lithium–Sulfur Batteries Working in Wide Temperature Ranges

Cationic Interfacial Layer toward a LiF-Enriched Interphase for Stable Li Metal Batteries

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In situ transmission electron microscopy for understanding materials and interfaces challenges in all-solid-state lithium batteries

Cited by 44 publications

References 121 publications

In Situ Synthesis of Germanium Particles Decorated in Conjugated N-doped Carbon Matrix: Boosting the Performance of the Lithium-Ion Battery

In Situ Synthesis of Germanium Particles Decorated in Conjugated N-doped Carbon Matrix: Boosting the Performance of the Lithium-Ion Battery

Origin of the High Conductivity of the LiI-Doped Li3PS4 Electrolytes for All-Solid-State Lithium–Sulfur Batteries Working in Wide Temperature Ranges

Cationic Interfacial Layer toward a LiF-Enriched Interphase for Stable Li Metal Batteries

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Origin of the High Conductivity of the LiI-Doped Li₃PS₄ Electrolytes for All-Solid-State Lithium–Sulfur Batteries Working in Wide Temperature Ranges