Extended Electrochemical Window of Solid Electrolytes via Heterogeneous Multilayered Structure for High‐Voltage Lithium Metal Batteries

Duan, Hui; Fan, Min; Chen, Wanping; Li, Jinyi; Wang, Pengfei; Wang, Wenpeng; Shi, Ji‐Lei; Yin, Ya‐Xia; Li, Wan; Guo, Yu‐Guo

doi:10.1002/adma.201807789

Cited by 365 publications

(190 citation statements)

References 47 publications

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“…which suffers from safety hazards such as leakage and combustion. [1,2,[20][21][22][23] Nevertheless, the large-scale application of SPEs in LMBs is still inevitably hindered because of the sluggish transport of Li ions and poor affinity of the Li/electrolyte interface. [24][25][26][27][28] Considering the ultrahigh reducibility of Li, serious parasitic reactions (e.g., Li reacts with poly(ethylene oxide) (PEO) to form Li 2 O, C 2 H 4 , and H 2 ) inevitably occur at the Li/PEO interface to harm the performances of batteries.…”

Section: Doi: 101002/adma202000223mentioning

confidence: 99%

In Situ Construction of a LiF‐Enriched Interface for Stable All‐Solid‐State Batteries and its Origin Revealed by Cryo‐TEM

et al. 2020

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The application of solid polymer electrolytes (SPEs) is still inherently limited by the unstable lithium (Li)/electrolyte interface, despite the advantages of security, flexibility, and workability of SPEs. Herein, the Li/electrolyte interface is modified by introducing Li2S additive to harvest stable all‐solid‐state lithium metal batteries (LMBs). Cryo‐transmission electron microscopy (cryo‐TEM) results demonstrate a mosaic interface between poly(ethylene oxide) (PEO) electrolytes and Li metal anodes, in which abundant crystalline grains of Li, Li2O, LiOH, and Li2CO3 are randomly distributed. Besides, cryo‐TEM visualization, combined with molecular dynamics simulations, reveals that the introduction of Li2S accelerates the decomposition of N(CF3SO2)2− and consequently promotes the formation of abundant LiF nanocrystals in the Li/PEO interface. The generated LiF is further verified to inhibit the breakage of CO bonds in the polymer chains and prevents the continuous interface reaction between Li and PEO. Therefore, the all‐solid‐state LMBs with the LiF‐enriched interface exhibit improved cycling capability and stability in a cell configuration with an ultralong lifespan over 1800 h. This work is believed to open up a new avenue for rational design of high‐performance all‐solid‐state LMBs.

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Section: Doi: 101002/adma202000223mentioning

confidence: 99%

In Situ Construction of a LiF‐Enriched Interface for Stable All‐Solid‐State Batteries and its Origin Revealed by Cryo‐TEM

et al. 2020

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“…In order to extend the electrochemical window of electrolytes to be compatible with highvoltage cathodes, many strategies have been proposed, including super-concentrated electrolytes, [9] dual-salt/ether electrolytes, [10] localized high-concentration electrolytes, [3] all-fluorinated electrolytes, [11] double-layer polymer electrolytes, [12] and heterogeneous multilayered solid electrolytes. [13] Although many progresses have been made in liquid electrolytes recently, broadening the electrochemical window of polymer electrolytes is still a challenge. Recently, a new type of electrolytes based on "quasi ionic liquids" (QILs) has been studied.…”

Section: Introductionmentioning

confidence: 99%

Polymer‐in‐“Quasi‐Ionic Liquid” Electrolytes for High‐Voltage Lithium Metal Batteries

Ren

et al. 2019

Advanced Energy Materials

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Due to the limited oxidation stability (< 4 V) of ether oxygen in its polymer structure, PEO-based polymer electrolytes are not compatible with high-voltage (> 4 V) cathodes, thus hindered further increase in the energy density of lithium (Li) metal batteries (LMBs). Here, we design a new type of polymer-in-"quasi ionic liquid" electrolyte (PQILE) that reduces the electron density on ethereal oxygens in PEO and ether solvent molecules, induces the formation of stable interfacial layers on both surfaces of LiNi 1/3 Mn 1/3 Co 1/3 O 2 (NMC) cathode and Li metal anode in Li||NMC batteries, and results in a capacity retention of 88.4%, 86.7% and 79.2% after 300 cycles with a charge cutoff voltage of 4.2, 4.3, and 4.4 V for the LMBs, respectively. Therefore, the use of "quasi ionic liquids" is a promising approach to design new polymer electrolytes for high-voltage and high-specific-energy LMBs. (EMSL), a national scientific user facility sponsored by the DOE's Office of Biological and Environmental Research and located at PNNL. PNNL is operated by Battelle for the DOE under Contract DE-AC05-76RLO1830. The salt LiFSI was provided by Dr. Kazuhiko Murata of Nippon Shokubai Co., Ltd.

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“…[36][37][38] Generally, commercial carbonate-based electrolytes are not suitable for Li metal batteries due to their high flammability and low coulombic efficiency during cycling. [36,[39][40][41] Therefore, the strategies that have been pursued to this end include modifying components of the liquid electrolyte, introducing new electrolyte systems such as solid and polymer electrolytes, [42][43][44][45][46][47][48] and adding particulate-based additives. [32,[49][50][51][52][53] Finally, Li metal interface modification is a practical approach that can be achieved using ex situ and in situ artificial layers.…”

Section: Introductionmentioning

confidence: 99%

Lithium Metal Interface Modification for High‐Energy Batteries: Approaches and Characterization

Lee

Song

Cho

et al. 2020

Batteries & Supercaps

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Rechargeable batteries have been a profoundly greater part of our lives than we could have ever imagined. The rechargeable Li‐ion batteries (LIBs) that have been developed for transport systems even put fossil fuels in the corner. However, state‐of‐the‐art Li‐ion batteries with graphite anodes are now approaching their theoretical specific energy limits, so they cannot meet the increasing demands of a range of portable electronics and large‐scale energy storage systems. Li metal is one of the most promising anode materials that could break through the energy density bottleneck of Li‐ion batteries due to its ultrahigh specific capacity and very low potential compared to other anode materials. Nonetheless, the direct use of Li metal in commercial battery systems has been hindered due to significant obstacles associated with it such as safety issues, corrosion from chemical reactions that occur inside the battery, or poor cycling performance. The fundamental reason for these problems is the dendritic growth of Li‐ions on the Li metal anode during cycling, as a result of the interfacial phenomena of Li metal and electrolytes. Modification of the Li metal interface with an electrolyte presents an efficient solution to solve these problems. In this review, the current challenges facing the development of Li metal anodes are presented in detail. The most recent advances in Li metal anodes using a controlled interface between the Li metal surface and an electrolyte are highlighted and an introduction on the synthesis and production methods for the application of high‐energy‐density battery systems such as Li‐oxygen (Li−O2), Li‐sulfur (Li−S), and Li metal batteries with high‐energy density cathodes is presented. Furthermore, the recent developments in the in situ/operando analysis tools adopted for the investigation of Li metal anodes such as the structural and chemical changes, dynamic properties, and solid–electrolyte interface (SEI) layer properties are described and summarized. Finally, some suggestions are given in the direction of the development of Li metal with artificial surface layers for use in future high‐energy batteries.

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Extended Electrochemical Window of Solid Electrolytes via Heterogeneous Multilayered Structure for High‐Voltage Lithium Metal Batteries

Abstract: Lithium-ion batteries (LIBs) have achieved huge success in the past few decades, due to mature technologies, low cost, and high charge-discharge efficiency. However, the development

Cited by 365 publications

References 47 publications

In Situ Construction of a LiF‐Enriched Interface for Stable All‐Solid‐State Batteries and its Origin Revealed by Cryo‐TEM

In Situ Construction of a LiF‐Enriched Interface for Stable All‐Solid‐State Batteries and its Origin Revealed by Cryo‐TEM

Polymer‐in‐“Quasi‐Ionic Liquid” Electrolytes for High‐Voltage Lithium Metal Batteries

Lithium Metal Interface Modification for High‐Energy Batteries: Approaches and Characterization

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