Silica gel solid nanocomposite electrolytes with interfacial conductivity promotion exceeding the bulk Li-ion conductivity of the ionic liquid electrolyte filler

Chen, Xubin; Put, Brecht; Sagara, A.; Gandrud, Knut Bjarne; Murata, Mitsuhiro; Steele, Julian A.; Yabe, Hiroki; Hantschel, Thomas; Roeffaers, Maarten B. J.; Tomiyama, Morio; Arase, Hidekazu; Kaneko, Yukihiro; Shimada, Mikinari; Mees, Maarten; Vereecken, Philippe M.

doi:10.1126/sciadv.aav3400

Cited by 61 publications

(99 citation statements)

References 40 publications

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“…[7,8] Moreover, ionogel electrolytes provide high ionic conductivity, favorable interfacial contact with electrodes, and wide processing compatibility, which address the key issues confronting inorganic and polymer solid-state electrolytes. [9][10][11][12] The electrochemical stability windows of ionogel electrolytes primarily depend on the ionic liquids. Since the anodic and cathodic stability of ionic liquids can be manipulated by altering the constituent anions and cations, a wide range of ionic liquids with different electrochemical windows have been explored for lithium-ion batteries.…”

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confidence: 99%

Layered Heterostructure Ionogel Electrolytes for High‐Performance Solid‐State Lithium‐Ion Batteries

et al. 2021

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Ionogel electrolytes based on ionic liquids and gelling matrices offer several advantages for solid‐state lithium‐ion batteries, including nonflammability, wide processing compatibility, and favorable electrochemical and thermal properties. However, the absence of ionic liquids that are concurrently stable at low and high potentials constrains the electrochemical windows of ionogel electrolytes and thus their high‐energy‐density applications. Here, ionogel electrolytes with a layered heterostructure are introduced, combining high‐potential (anodic stability: >5 V vs Li/Li+) and low‐potential (cathodic stability: <0 V vs Li/Li+) imidazolium ionic liquids in a hexagonal boron nitride nanoplatelet matrix. These layered heterostructure ionogel electrolytes lead to extended electrochemical windows, while preserving high ionic conductivity (>1 mS cm−1 at room temperature). Using the layered heterostructure ionogel electrolytes, full‐cell solid‐state lithium‐ion batteries with a nickel manganese cobalt oxide cathode and a graphite anode are demonstrated, exhibiting voltages that are unachievable with either the high‐potential or low‐potential ionic liquid alone. Compared to ionogel electrolytes based on mixed ionic liquids, the layered heterostructure ionogel electrolytes enable higher stability operation of full‐cell lithium‐ion batteries, resulting in significantly enhanced cycling performance.

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confidence: 99%

Layered Heterostructure Ionogel Electrolytes for High‐Performance Solid‐State Lithium‐Ion Batteries

et al. 2021

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“…A new concept has been recently proposed by Chen et al [ 138 ] who explained the electrolytic conductance is highly affected by the layers of chemical water (immobile ice layer) adsorbed on OH-terminated SiO 2 surface. They proposed the immobilization of 1-butyl-1-methylpyrrolidinium-bis TFSI (BMP TFSI) IL molecules extends the formation of ice layer on the SiO 2 surface ( Figure 17 ).…”

Section: Mechanism Of LI + Transport On the Intmentioning

confidence: 99%

Inorganic Fillers in Composite Gel Polymer Electrolytes for High-Performance Lithium and Non-Lithium Polymer Batteries

Huy

Hur

2021

Nanomaterials

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Among the various types of polymer electrolytes, gel polymer electrolytes have been considered as promising electrolytes for high-performance lithium and non-lithium batteries. The introduction of inorganic fillers into the polymer-salt system of gel polymer electrolytes has emerged as an effective strategy to achieve high ionic conductivity and excellent interfacial contact with the electrode. In this review, the detailed roles of inorganic fillers in composite gel polymer electrolytes are presented based on their physical and electrochemical properties in lithium and non-lithium polymer batteries. First, we summarize the historical developments of gel polymer electrolytes. Then, a list of detailed fillers applied in gel polymer electrolytes is presented. Possible mechanisms of conductivity enhancement by the addition of inorganic fillers are discussed for each inorganic filler. Subsequently, inorganic filler/polymer composite electrolytes studied for use in various battery systems, including Li-, Na-, Mg-, and Zn-ion batteries, are discussed. Finally, the future perspectives and requirements of the current composite gel polymer electrolyte technologies are highlighted.

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“…[22] Moreover, NIEs based on SiO 2 and 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide (BMP-TFSI)/LiTFSI have shown 200% higher ionic conductivity than the IL electrolyte alone by introducing a functional ice layer to the SiO 2 matrix. [6]…”

Section: Ionic Conductivitymentioning

confidence: 99%

“…Herein, we discuss recent developments surrounding nanocomposite ionogel electrolytes (NIEs) in the context of solidstate rechargeable batteries. Diverse nanoscale matrix materials are considered including oxides, [6][7][8][9][10][11] boron nitride (BN), [12,13] metal-organic frameworks (MOFs), [14] and garnets. [15] Section 2 describes the relationships between nanoscale material structure and ionogel properties, including ionic conductivity, mechanical moduli, thermal properties, and electrochemical stability.…”

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confidence: 99%

Nanocomposite Ionogel Electrolytes for Solid‐State Rechargeable Batteries

Hyun

Thomas

Hersam

2020

Advanced Energy Materials

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Ionogels composed of ionic liquids and gelling solid matrices offer several advantages as solid‐state electrolytes for rechargeable batteries, including safety under diverse operating conditions, favorable electrochemical and thermal properties, and wide processing compatibility. Among gelling solid matrices, nanoscale materials have shown particular promise due to their ability to concurrently enhance ionogel mechanical properties, thermal stability, ionic conductivity, and electrochemical stability. These beneficial attributes suggest that ionogel electrolytes are not only of interest for incumbent lithium‐ion batteries but also for next‐generation rechargeable battery technologies. Herein, recent advances in nanocomposite ionogel electrolytes are discussed to highlight their advantages as solid‐state electrolytes for rechargeable batteries. By exploring a range of different nanoscale gelling solid matrices, relationships between nanoscale material structure and ionogel properties are developed. Furthermore, key research challenges are delineated to help guide and accelerate the incorporation of nanocomposite ionogel electrolytes in high‐performance solid‐state rechargeable batteries.

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Silica gel solid nanocomposite electrolytes with interfacial conductivity promotion exceeding the bulk Li-ion conductivity of the ionic liquid electrolyte filler

Cited by 61 publications

References 40 publications

Layered Heterostructure Ionogel Electrolytes for High‐Performance Solid‐State Lithium‐Ion Batteries

Layered Heterostructure Ionogel Electrolytes for High‐Performance Solid‐State Lithium‐Ion Batteries

Inorganic Fillers in Composite Gel Polymer Electrolytes for High-Performance Lithium and Non-Lithium Polymer Batteries

Nanocomposite Ionogel Electrolytes for Solid‐State Rechargeable Batteries

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