Abstract The safe operation of rechargeable batteries is crucial because of numerous instances of fire and explosion mishaps. However, battery chemistry involving metallic lithium (Li) as the anode is prone to thermal runaway in flammable organic electrolytes under abusive conditions. Herein, an in situ encapsulation strategy is proposed to construct nonflammable quasi‐solid electrolytes through the radical polymerization of a hexafluorobutyl acrylate (HFBA) monomer and a pentaerythritol tetraacrylate (PETEA) crosslinker. The quasi‐solid system eliminates the inherent flammability of ether electrolytes with zero self‐extinguishing time owing to the gas‐phase radical capturing ability of HFBA. Additionally, the graphitized carbon layer generated during the decomposition of PETEA at high temperatures obstructs the heat and oxygen required for combustion. When coupled with Au‐modified reduced graphene oxide anodic current collectors and lithium sulfide cathodes, the assembled anode‐free Li‐metal cell based on the quasi‐solid electrolyte exhibits no signs of cell expansion or gas generation during cycling, and thermal runaway is eliminated under multiple mechanical, electrical, and thermal abuse scenarios and even rigorous strikes. This nonflammable quasi‐solid configuration with gas‐ and condensed‐phase flame‐retardant mechanisms can drive a technological leap in anode‐free Li‐metal pouch cells and secure the practical applications necessary to power this society in a safe manner. 

Nonflammable Polyfluorides‐Anchored Quasi‐Solid Electrolytes for Ultra‐Safe Anode‐Free Lithium Pouch Cells without Thermal Runaway

The poor compatibility with Li metal and electrolyte oxidation stability preclude the utilization of commercial ester-based electrolytes for high-voltage lithium metal batteries. This work proposes a quasi-localized high-concentration electrolyte (q-LHCE) by partially replacing solvents in conventional LiPF6 based carbonated electrolyte with fluorinated analogs (fluoroethylene carbonate (FEC), 2,2,2-trifluoroethyl methyl carbonate (FEMC)) with weakly-solvating ability. The q-LHCE enables the formation of an anion-rich solvation sheath, which functions like LHCE but differs in the partial participation of weakly-solvating cosolvent in the solvation structure. With this optimized electrolyte, inorganic-dominated solid electrolyte interphases are achieved on both the cathode and anode, leading to uniform Li deposition, suppressed electrolyte decomposition and cathode deterioration. Consequently, q-LHCE supports stable cycling of Li | LiCoO2 (≈3.5 mAh cm−2) cells at 4.5 V under the whole climate range (from −20 to 45 °C) with limited Li consumption. A practical ampere-hour level graphite | LiCoO2 pouch cell at 4.5 V and aggressive Li | LiNi0.5Mn1.5O4 cell at 5.0 V with excellent capacity retention further reveals the effectiveness of q-LHCE. The refinement of old-fashioned carbonate electrolytes provides new perspectives toward practical high-voltage battery systems. 

Quasi‐Localized High‐Concentration Electrolytes for High‐Voltage Lithium Metal Batteries

Lithium metal batteries (LMBs) coupled with a high-voltage Ni-rich cathode are promising for meeting the increasing demand for high energy density. However, aggressive electrode chemistry imposes ultimate requirements on the electrolytes used. Among the various optimized electrolytes investigated, localized high-concentration electrolytes (LHCEs) have excellent reversibility against a lithium metal anode. However, because they consist of thermally and electrochemically unstable solvents, they have inferior stability at elevated temperatures and high cutoff voltages. Here we report a semisolvated sole-solvent electrolyte to construct a typical LHCE solvation structure but with significantly improved stability using one bifunctional solvent. The designed electrolyte exhibits exceptional stability against both electrodes with suppressed lithium dendrite growth, phase transition, microcracking, and transition metal dissolution. A Li||Ni0.8Co0.1Mn0.1O2 cell with this electrolyte operates stably over a wide temperature range from -20 to 60 °C and has a high capacity retention of 95.6% after the 100th cycle at 4.7 V, and ∼80% of the initial capacity is retained even after 180 cycles. This new electrolyte indicates a new path toward future electrolyte engineering and safe high-voltage LMBs.

A Semisolvated Sole-Solvent Electrolyte for High-Voltage Lithium Metal Batteries.

Lithium batteries play a dominant role in the power source market of electric vehicles and portable electronic devices. The electrolyte is critical to determining the performance of lithium batteries. Conventional electrolytes cannot meet the ever-growing demands of fast-charging, wide-temperature operation, and safety properties of lithium batteries. Despite the great success of (localized) high-concentration electrolytes, they still suffer from disadvantages like low ionic conductivity and high cost. The emerging weakly solvating electrolytes, also known as low-solvating electrolytes, offer another solution to these challenges and have attracted intensive research interests in recent years. This contribution reviews the working mechanisms, design principles, and recent advances in developing weakly solvating electrolytes. A summary and perspective about future research directions in this field is also provided. The insights will benefit both academic and industrial communities in designing safe and high-performance next-generation Li batteries. 

Weakly solvating electrolytes for next-generation lithium batteries: design principles and recent advances

High degrees of freedom (DOF) for K+ movement in the electrolytes is desirable, because the resulting high ionic conductivity helps improve potassium-ion batteries, yet requiring support from highly free and flammable organic solvent molecules, seriously affecting battery safety. Here, we develop a K+ flux rectifier to trim K ion's DOF to 1 and improve electrochemical properties. Although the ionic conductivity is compromised in the K+ flux rectifier, the overall electrochemical performance of PIBs was improved. An oxidation stability improvement from 4.0 to 5.9 V was realized, and the formation of dendrites and the dissolution of organic cathodes were inhibited. Consequently, the K||K cells continuously cycled over 3,700 h; K||Cu cells operated stably over 800 cycles with the Coulombic efficiency exceeding 99%; and K||graphite cells exhibited high-capacity retention over 74.7% after 1,500 cycles. Moreover, the 3,4,9,10-perylenetetracarboxylic diimide organic cathodes operated for more than 2,100 cycles and reached year-scale-cycling time. We fabricated a 2.18 Ah pouch cell with no significant capacity fading observed after 100 cycles. 

Trimming the Degrees of Freedom via a K+ Flux Rectifier for Safe and Long-Life Potassium-Ion Batteries

Abstract Aggressive chemistry involving Li metal anode (LMA) and high-voltage LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NCM811) cathode is deemed as a pragmatic approach to pursue the desperate 400 Wh kg −1 . Yet, their implementation is plagued by low Coulombic efficiency and inferior cycling stability. Herein, we propose an optimally fluorinated linear carboxylic ester (ethyl 3,3,3-trifluoropropanoate, FEP) paired with weakly solvating fluoroethylene carbonate and dissociated lithium salts (LiBF 4 and LiDFOB) to prepare a weakly solvating and dissociated electrolyte. An anion-enrichment interface prompts more anions’ decomposition in the inner Helmholtz plane and higher reduction potential of anions. Consequently, the anion-derived interface chemistry contributes to the compact and columnar-structure Li deposits with a high CE of 98.7% and stable cycling of 4.6 V NCM811 and LiCoO 2 cathode. Accordingly, industrial anode-free pouch cells under harsh testing conditions deliver a high energy of 442.5 Wh kg −1 with 80% capacity retention after 100 cycles. 

/pdf/anion-enrichment-interface-enables-high-voltage-anode-free-1g1vzc36.pdf

Anion-enrichment interface enables high-voltage anode-free lithium metal batteries

Single-function electronic (carbon) and ionic (electrolyte) conductors result in unbalanced ionic–electronic charge transport in conventional 3D porous electrodes due to a complex heterogeneous interface and flexural ionic–electronic transport pathways. Herein, an all-in-one ionic–electronic transport network wherein Li ions and electrons migrate in the same channel is proposed in an all-electrochemically active all-solid-state electrode using dual-carrier conductors (DCC). As a result, the tortuosity factor in the DCC all-solid-state electrode is significantly reduced to 1–4 (close to the value of 1.5–10 of existing commercial liquid batteries), and the polarization is significantly smaller than that of the triple-phase electrode. Our proposed all-in-one ionic–electronic DCC conducting mechanism is expected to offer a new feasible way to achieve high-mass-loading all-solid-state cathodes in practical applications. 

All-in-One Ionic–Electronic Dual-Carrier Conducting Framework Thickening All-Solid-State Electrode

Wearable pressure sensors have attracted significant consideration due to their wide use in healthcare, intelligent robotics, and electronic skin. In this article, a dielectric material composed of Sn-based nanofibers containing SnOx/SnCl2 ( ${x} =$ 1 and 2) was proposed for the first time to enhance the performance of pressure sensors. Compared with most of the reported nanofiber-based film pressure sensors, our tissue-like nanocomposite sensors achieve optimized sensitivity and working range and are particularly suitable for wearable applications. In contrast to most current research, electrospun nanofiber mats were oxidized without further pyrolysis at 100 °C, 200 °C, and 300 °C. Especially after annealing at 200 °C, the assembled tissue-like pressure sensor presents remarkable performance with a working range of up to 50 kPa and a sensor sensitivity of 11.6 kPa−1 (0–1 kPa). In addition, this sensor exhibits excellent cycling stability, permeability, and washability. Therefore, polyvinylpyrrolidone (PVP)/SnCl2 tissue-like nanocomposite sensors can be utilized in a wide variety of flexible and wearable electronic device applications in the future.

A Washable, Permeable, and Ultrasensitive Sn-Based Textile Pressure Sensor for Health Monitoring

Wadsley-Roth Phase Niobium-Based Oxide Anode Promising High Power and Energy Density Aqueous Li-Ion Batteries

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Anion-enrichment interface enables high-voltage anode-free lithium metal batteries

All-in-One Ionic–Electronic Dual-Carrier Conducting Framework Thickening All-Solid-State Electrode

A Washable, Permeable, and Ultrasensitive Sn-Based Textile Pressure Sensor for Health Monitoring

Wadsley-Roth Phase Niobium-Based Oxide Anode Promising High Power and Energy Density Aqueous Li-Ion Batteries