Formation Of Electrolyte Research Articles

Mechanistic Study on Oxygen Reduction Reaction in High-Concentrated Electrolytes for Aprotic Lithium-Oxygen Batteries.

Highly concentrated electrolytes (HCEs) have energized the development of high-energy-density lithium metal batteries by facilitating the formation of robust inorganic-derived solid electrolyte interfaces on the lithium anode. However, the oxygen reduction reaction (ORR) occurring on the cathode side remains ambiguous in HCE-based lithium-oxygen (Li-O2) batteries. Herein, we investigate the ORR mechanism in a highly concentrated LiTFSI-CH3CN electrolyte using ultra-microelectrode voltammetry coupled with in situ spectroscopies. It is found that, compared to the dilute electrolyte, the HCE prolongs the lifespan of superoxide intermediates and decelerates their migration rate to the bulk solution, resulting in a change in growth mode for the discharge product of Li2O2 from traditional two-dimensional film growth to surface three-dimensional expansion growth. This alteration reduces the cathode passivation and thus delivers the enhanced discharge capacity. Additionally, the HCE also increases the reaction energy barrier between superoxide and solvent molecules, thereby minimizing parasitic reactions and improving the cycle performance of Li-O2 batteries. Our study reveals the intricate interplay between electrolytes and oxygen intermediates and provides important insights into electrolyte chemistries for better Li-O2 batteries.

Metal-organic frameworks Derived frustrated Lewis acid-base pairs accelerate ion dynamics to dendrite-free solid-state lithium batteries

The Poly(ethylene oxide) (PEO)-based polymer electrolytes exhibit the drawbacks of high crystallinity and low ionic conductivity (<10−5 S m−1), which significantly restrict their application in solid-state lithium metal batteries. This study presents the bismuth metal-organic frameworks (MOFs) as a PEO-based electrolyte filler, incorporating frustrated Lewis acid-base pairs, which is formed in-situ through the coordination of ellagic acid (EA) and bismuth ions (Bi3+). The simultaneous presence of Lewis acids (unsaturated Bi3+) and bases (free nitrate, NO3−) in the MOFs, which effectively transfers and transports the lithium ions through the synergistic interaction based on the polymer matrix and the lithium salts, resulting in the high durable solid-state lithium batteries. Meanwhile, NO3− can further promote the dissociation of lithium ion (Li+) and the formation of inorganic solid electrolyte interfaces (SEIs) with lithium metal, which is conducive to the dynamic repair of SEIs. Characterizations and calculations show that Bi-MOFs promote the increase of composite ionic conductivity (6.4 × 10−4 S cm−1, 60 °C) and lithium transference number (0.52, 60 °C). At a current density of 0.4 mA cm−2, the assembled Li–Li symmetric battery can be continuously cycled for more than 500 h. This strategy opens a new window for improvement of solid-state electrolyte performance.

Multifunctional nitrile additives for inducing pseudo-concentration gel-polymer electrolyte: Enabling stable high-voltage lithium metal batteries

High-voltage lithium metal batteries (LMBs) are promising for next-generation high-energy storage systems. Unfortunately, their implementation has been severely plagued by the interfacial instability between the high-voltage cathodes/lithium metal (LM) anodes and electrolytes. To tackle these challenges, a novel nitrile additive, 1,4-dicyanobenzene (DCB) (Synonyms: terephthalonitrile), is added to the in situ polymerized pentaerythritol tetraacrylate-based gel polymer electrolyte (GPE). The DCB additive, as demonstrated both theoretically and experimentally, plays a crucial role in altering the Li+ coordinated solvation structure within the GPE. This alteration leads to the formation of a pseudo-concentrated electrolyte with a tightly packed Li+ cluster, expanding the electrochemical stability window of the electrolyte. Moreover, the DCB-included GPE significantly improves its compatibility with both LM anode and high-voltage cathode, attributed to the modified solvation structure and the generated LiF-rich electrolyte/electrode interphases. Accordingly, the GPE enables stable cyclic performance of LMBs based on a 4.9 V LiNi0.5Mn1.5O4 cathode at a low relative negative/positive ratio of 4, achieving a high reversible capacity of 123.8 mAh g−1 with a capacity retention of 87.7 % over 500 cycles at 0.5 C. This work provides new insights into enhancing the cyclability of high-voltage LMBs via the synergistic effect of additives and GPE.

Stabilizing electrode-electrolyte interface via crown ether-containing selective coating for dendrite-free Na-K anode-based solid-state sodium batteries

Sodium-potassium (Na-K) alloy is considered a promising anode material due to its liquid characteristics at room temperature. However, unstable interfaces and disastrous ion exchange between Na-K alloy anodes and solid-state Na electrolytes (SSNEs) have hindered further applications of solid-state Na batteries (SSNBs) based on Na-K anodes. In this work, a specially designed Na+/K+ selective gel coating with 15-crown 5-ether (15C5) is constructed on the beta-alumina solid electrolyte (BASE) to achieve a good match with Na-K anodes. The coordination of 15C5 with Na+ forms Na+-permeable complexes and affects the electrolyte solvation structure in the gel coating, resulting in the formation of solid electrolyte interfaces (SEIs) that lack K+ channels and are organically rich, which effectively inhibit the ion exchange and stabilize the interface. Benefitting from the selective coating, the cycling lifetime of the Na-K|Gel-BASE-Gel|Na-K symmetric cell reaches over 1000 h, and the Na-K|Gel-BASE-Gel|Na3V2(PO4)3 full cell exhibits great long-cycle stability and excellent rate performance at room temperature. This work extends the application of Na-K anodes and provides a suggestion for achieving high-performance SSNBs at room temperature.

Origin of O2 Generation in Sulfide-Based All-Solid-State Batteries and its Impact on High Energy Density.

The cathode surface of sulfide-based all-solid-state batteries (SBs) is commonly coated with amorphous-LiNbO3 in order to stabilize charge-discharge reactions. However, high-voltage charging diminishes the advantages, which is caused by problems with the amorphous-LiNbO3 coating layer. This study has investigated the degradation of amorphous-LiNbO3 coating layer directly during the high-voltage charging of SBs. O2 generation via Li extraction from the amorphous-LiNbO3 coating layer is observed using electrochemical gas analysis and electrochemical X-ray photoelectron spectroscopy. This O2 leads to the formation of an oxidative solid electrolyte (SE) around the coating layer and degrades the battery performance. On the other hand, elemental substitution (i.e., amorphous-LiNbxP1- xO3) reduces O2 release, leading to stable high-voltage charge-discharge reactions of SBs. The results have emphasized that the suppression of O2 generation is a key factor in improving the energy density of SBs.

Enabling stable high lithium storage of Si anode via synergistic effects of nanosized Fe3C and partially graphitized porous carbon

Si is considered as a promising anode for high-energy lithium-ion batteries (LIBs) because of its ultrahigh theoretical specific capacity and desired working potential. However, the main problems of Si as an anode are still faced with low conductivity and inevitable structure damage caused by large volume change during cycle. Although design of Si/C composites effectively mitigates the above problems, their preparation usually involves complex methods. This work demonstrates a very simple ball milling and subsequent carbonization approach for the preparation of high-performance Si NPs@Fe3C@PC anode, which integrates partially hollow Fe3C nanoparticles (Fe3C) and partially graphitized porous carbon (PC) into Si nanoparticles (Si NPs)-based composite. It is found that Fe3C with catalysis is favorable not only to formation of a graphitized porous carbon during material preparation but also to formation of a stable solid electrolyte interfaces (SEI) on electrode surface during cycle. With Fe3C, the Si NPs@Fe3C@PC shows smaller Li+ adsorption energy, lower activation energy, higher electric conductivity, larger Li+ diffusion coefficient and a thinner SEI film than Si NPs and Si NPs@PC counterparts. The findings verify that the synergistic effects of the Fe3C and PC provide fast kinetics, high capacitive contribution, improved structure stability and a stable LiF-rich SEI film for Si NPs@Fe3C@PC during cycle. Therefore, Si NPs@Fe3C@PC shows excellent electrochemical performance, gaining 1786, 1211.4 and 411.5 mAh/g after 210, 650 and 840 cycles at 100, 1000 and 5000 mA g−1, respectively. Finally, this contribution proposes a simple and effective strategy for improving Si NPs performance and hence obtaining a high-performance of Si-based anode for LIBs.

TiH2-based anode: In situ formation of solid electrolyte for high volumetric energy density with minimal content of conducting agent

Herein, we report the fabrication of an electrode composite with an ultra-high active material content (90 wt%). This composite was possible because of the utilization of TiH2 as an anode active material that forms a solid electrolyte (LiH) in situ and functions as an electronic conductor, enabling a substantial reduction of the amount of conductor additive in the electrodes. The electrochemical performance of the TiH2-based electrodes with a high active material content was comparable to that of electrode composites that include a solid electrolyte because of sufficient Li+-ion conduction pathways provided by the LiH formed in situ. To further increase the capacity of the TiH2-based electrode, MgH2 (theoretical capacity: 2036 mAh/g) was mixed with TiH2 to function as an active material. TiH2, which is known to exhibit high electron conductivity and a high density, is expected to be used as a partial substitute for low-density carbon additives to increase the volumetric energy density of batteries and their active material content. Hence, the xMgH2-(1 − x)TiH2-AB (AB: acetylene black) electrode composite exhibited a high active material content (90 wt%) and improved volumetric energy density (1687 Wh/L, based on the anode) compared with a MgH2-AB (70:30 wt%) electrode composite (1157 Wh/L), even when the AB content of the xMgH2-(1 − x)TiH2-AB composite was 10 wt%. In addition, a MgH2-TiH2-VGCF (VGCF: vapor-grown carbon fiber) based electrode composite exhibited the highest volumetric and gravimetric energy density (2154 Wh/L, 1888 Wh/kg) among the investigated composites, facilitated by sufficient electron pathways provided by VGCF.

In-situ formation of quasi-solid polymer electrolyte for wide-temperature applicable Li-metal batteries

As next-generation rechargeable batteries, the development of solid-state lithium-metal batteries (LMBs) in a multitude of applications is confronted with a trade-off between high energy density, safety, and wide-temperature tolerance. Especially in cold climates, their applications are challenged by insufficient dynamics in bulk electrolyte and at electrode/electrolyte interface. Herein, a flexible, highly ionic conductive, and low-temperature applicable quasi-solid polymer electrolyte (QSPE) is designed and fabricated, which achieves a stable Li-metal anode over a wide-temperature range (−20 ∼ 60 °C). The QSPEs prepared via in-situ polymerization of polyethylene glycol (PEO)-based monomers in low-melting solvent (1,3-dioxolane (DOL) or ethyl difluoroacetate (EDFA)) endow low-temperature tolerance, prominent ionic conductivity (4.5 × 10−4 S cm−1 at −20 °C) and exceptional electrochemical performance over a wide-temperature range. Consequently, with the DOL-based QSPE (D-QSPE), the Li/D-QSPE/LiFePO4 cell presents stable, long-term cycling at −20 °C (minimal capacity degradation over 550 cycles) and excellent fast-charging capacity (capacity retention of 81 % over 1300 cycles at 5 C). Even utilizing a thin lithium foil (25 μm) and a high mass loading LiFePO4 cathode (2.5 mAh cm−2), the assembled Li/LFP cell with a N/P ratio of 1.96 still exhibits good cycling performance at −20 °C. Additionally, the EDFA-based QSPE (E-QSPE) allows LMBs with NCM811 cathodes cycling over 140 cycles (capacity retention > 95 %) at −20 °C. With the capability of circumventing sluggish ion transport kinetics of quasi-solid polymer LMBs in cold climates, the developed polymer electrolyte provides new pathways for safe, high-capability, and wide-temperature operable batteries.

(Invited) A Sustainable and Reliable Electrolyte Toward Safe Zn-MnO2 Alkaline Rechargeable Batteries

Zinc-Manganese Dioxide (Zn-MnO2) rechargeable batteries has spurred interest due to lower cost, high specific capacity, increased safety while using in small electronic devices and wearable technology. Zn-MnO2 alkaline batteries form inactive compounds during charging and discharging that hinder their ability to be utilized in rechargeable settings. Design and development of functional electrolyte to replace traditional electrolyte have become an effective way to inhibit irreversible compound formations and Zn dendrite growth, avoid leakage issues and metallic packaging. However, many challenges such as reliable and reproducible ionic conductivity and ion transference number of free-standing electrolyte films at lower thickness (150 µm), and interfacial contact resistance between electrolyte and electrode layer still exist. Our assumption is producing reliable and consistent ionic conductivity and ion transference number of electrolytes at lower thickness (150 µm) will help in providing the faster redox reaction kinetics at electrolyte-electrode interface. Moreover, by reducing the interfacial contact resistance between electrolyte and electrode interface will help in reducing the charge transfer resistance and zincate ion movements and results in improving the reversible life cycle of batteries. Many electrolytes fabricated utilize two different solutions that are mixed separately, forming either a liquid or a solid electrolyte after curing. Due to separate mixing, both solutions are never fully incorporated into one another, causing discrepancies in the consistency of the electrolyte. Here, we propose to use sustainable chitosan, which utilized 5:1 ratio of naturally occurring Chitosan (Chi) and Polyvinyl Alcohol (PVA) respectively. The Chi and PVA solution were premixed using ultrasonic bath and vacuum suction was used to remove extra bubbles formation due to mixing of Chi and PVA. This new process of electrolyte formation was compared between different thickness (120 µm, 150 µm, and 250µm), and the best electrolyte was then compared to the old process of mixing the solutions separately for electrolyte formation. The different thickness electrolytes were soaked into Potassium Hydroxide (KOH) and compared on their Ionic Conductivity, Ionic Conductance, Ion Transference Number, PH, and Swelling Ratio. To reduce the interfacial contact resistance between electrolyte and electrode, free standing electrolyte layer will be dipped into Chi solution and then put in contact with electrodes. These electrolytes were then used in the fabrication of Zn-MnO2 batteries and measure their performance using cyclic voltammetry and galvanostatic charge-discharge.

Solid Electrolyte Coated NCM523 for Composite Cathode in All-Solid-State Batteries

All-solid-state battery using sulfide solid electrolyte has advantages such as high lithium ionic conductivity and wide electrochemical stability window. Although it is attracting great attention in that it is capable of high power and high energy density, there are problems to be improved.Organic liquid electrolytes in conventional lithium ion batteries have excellent wettability and can form uniform lithium ion transfer channels in electrodes. However, in the case of all-solid-state battery, the formation of a solid-solid interface is limited due to the solid characteristics. In addition, the degradation of the interfacial contact between the active material and solid electrolyte in the composite electrode due to the volume change of the active material with (de)-intercalation of lithium ion during cycling causes loss of the lithium ionic pathway and deterioration of cell performance. This study focuses on improving battery performance by coating the surface of active material with solid electrolyte to maintain an even lithium ion transfer path in the composite electrode. The solid electrolyte coating of the active material has a decisive effect on the electrochemical behavior of the cell because it affects the formation of smooth lithium ionic pathway and suppression of voids in the composite electrode. Therefore, the focus of this study is to confirm the formation of uniform solid electrolyte coating layer according to the size of the solid electrolyte.Therefore, the particle size of the solid electrolyte was diversified using a liquid-phase process and a dispersant, and the solid electrolyte coating was performed using a dispersion process. It was confirmed that an even solid electrolyte coating layer was formed as the particles size of the solid electrolyte decreased, and the electrochemical performance was improved due to the solid electrolyte coating layer. In addition, it was confirmed that the lithium ionic pathway was maintained even after long cycling with the solid electrolyte coating layer, and also the side reactions occurred less according to the homogeneous electrochemical reaction.

Polarization Reduction of a Novel Cell Configuration Based on Thin-Film Electrolyte on Porous Oxide Framework for Solid State Batteries Application

In early 1990s, rechargeable Li batteries using inorganic ionic conductors as solid electrolytes have been proposed. Because of their improved safety features, solid state batteries have received great attention recently. Although using Li metal as an ideal high-capacity anode has been a long-term goal, the critical issues remaining to be solved are the polarization contributed from the solid electrolyte and the electrode/electrolyte interface. Thus, to form a Li-conducting thin film with good adhesion with an adequate conducting and porous oxide framework in between Li anode and thin electrolyte may be a solution for the reduction of above-mentioned polarization observed in the solid state batteries. Thus, the main objective of this study is to (i) calculate/estimate the polarization reduction in a solid state cell using thin-film inorganic electrolyte and metallic Li as anode, (ii) to complete the experimental design for in-situ formation of thin electrolyte based on sol-gel deposition of an oxides precursor on a porous and conducting oxide framework followed by heat-treatment at temperatures > 700°C. The verification of polarization reduction contributed from the proposed thin-film electrolyte as well as the porous/conducting framework will be carried out in the near future.

Advancements in Prelithiation Technology: Transforming Batteries from Li‐Shortage to Li‐Rich Systems

AbstractThe sufficient and reversible active lithium is the cornerstone for the operation of high‐energy lithium‐ion batteries. However, active lithium is inevitably depleted due to the formation of a solid electrolyte and the presence of irreversible side reactions. The shortage of lithium in optimally designed batteries not only leads to a depreciation of energy density but also deteriorates the electrode structure resulting in degradation of cycle life. Inspiringly, prelithiation technology that additionally compensates for lithium has been proposed and is playing an increasingly significant role in enhancing battery energy density and prolonging cycle life. Herein, guided by the factors that initiate lithium loss, the action mechanism and the effectiveness of prelithiation are scrutinized. Moreover, the emerging advanced prelithiation technologies based on anode/cathode materials, the key barriers, and the applicability at scale are systematically summarized and compared. Integrating the challenges and development trends aspires to provide a comprehensive prelithiated hybrid lithium replenishment and storage technology as a reference in the scale‐up of prelithiation technologies.

Ceramic Fillers for Improved Lithium-Sulfur Batteries

With the decarbonization of transportation, the demand for electric vehicles (EVs) and batteries that can power these EVs has been increasing. Lithium-ion-based batteries are already well-established and are considered the main chemistries to power current EVs. However, limited specific energy (< 300 Wh/kg) prevents these batteries from having high mileage vehicles. Lithium-sulfur batteries are considered the most promising next-generation energy storage system as they high theoretical capacity (~1675 mAhg-1), low cathode materials cost, and cell energy densities that can exceed 700 Wh/kg [1,2]. However, some major drawbacks prevent the Li-S battery system from being applicable in energy devices and hinder its commercialization, that include low power density and rapid capacity degradation during their cycling life. In addition, the lithium metal anode in Li-S batteries bring various issues to the forefront such as continuous solid electrolyte interface growth, dendrite formation, and loss of active lithium and electrolyte. These issues are further exacerbated at high C-rates which increases the possibility of an internal short-circuit and sudden cell failure [3]. In order to promote longer life cycles and prevent sudden cell failure, a thorough understanding of the cell’s electrochemical behavior is crucial for the development of a stable and practical Li-S battery system. The introduction of oxide fillers such TiO2, Al2O3, SiO2, etc. has been previously studied in various lithium-ion systems and has been shown to improve the cell’s lithium-ion transport properties, which in turn improve the performance of Li-S cells [4]. When used as interlayers they can also trap soluble polysulfides diffusing out of the cathode and reduce their crossover to the anode which helps reduce the shuttle effect of said polysulfides.In the present study, the use of a polysulfide immobilizing system to reduce sulfur loss and improve capacity retention has been demonstrated. The galvanostatic charge-discharge cycling study shows that cells retain higher capacity during the course of cycling. The initial capacity for Li-S cells with the filler average 1300+ mAh/g (C/10) while the capacity stabilizes around 1000 mAh/g after 3 cycles (C/5). The capacity retention at C/5 after 75 cycles was approximately 875 mAh/g which represents a rate 0.17% drop per cycle. When compared to control cells, the cells containing no fillers had lower initial capacity that averaged 1050 mAh/g and that rapidly declined to stabilize around 650 mAh/g. However, after this major drop, the cells remained stable no with measurable drop after 75 cycles. The behavior indicates that the cells with fillers delayed the effect of sulfur loss experienced in cells without fillers; however, the slow capacity drop that ensued, indicates that while polysulfide trapping was efficient it was unable to fully prevent it. The effect of fillers on the Coulombic efficiency (CE) also supports the polysulfide “trapping” mechanism and shows the ability of the cell to reduce the shuttle effect that contributes to lower CE values. Further electrochemical studies have been performed to understand the mechanisms of the improvement of the cell.

In situ Formation of Solid Electrolyte during Lithiation Process of MgCl2 Anode in an All‐Solid‐State Lithium Battery

AbstractAll‐solid‐state lithium batteries, which are free from the risk of liquid entanglement, are expected to have high energy densities and high safety. In this study, the omission of a solid electrolyte from the electrode and an increase in thickness of the electrode were investigated to improve the energy density of all‐solid‐state lithium batteries. We focused on MgCl2, which reversibly self‐generates a solid electrolyte during the lithiation process, as an anode material that can operate without a solid electrolyte incorporated into the electrode mixture. Indeed, the electrochemical properties of the MgCl2 electrode were approximately the same with or without a pre‐contained solid electrolyte, LiBH4. X‐ray diffraction and X‐ray absorption spectroscopy analyses showed that lithiation produced Mg and LiCl, which were recovered to MgCl2 by subsequent delithiation. The available electrode thickness was also investigated, and the thickness limit for the first lithiation was found to be ∼100 μm.

Prelithiated rigid polymer with high ionic conductivity as silicon-based anode binder for lithium-ion battery

Silicon-based electrodes suffer from rapid performance degradation derived from a severe volume expansion during cycling in lithium-ion batteries, and using elaborately designed polymer binders is deemed an efficient tactic to tackle the above thorny issues. In this study, a water-soluble rigid-rod poly(2,2′-disulfonyl-4,4′-benzidine terephthalamide) (PBDT) polymer is described and employed as the binder for Si-based electrodes for the first time. The nematic rigid PBDT bundles wrapped around the Si nanoparticles by hydrogen bonding effectively inhibit the volume expansion of the Si and promote the formation of stable solid electrolyte interfaces (SEI). Moreover, the prelithiated PBDT binder with high ionic conductivity (3.2 × 10−4 S cm−1) not only improves the Li-ions transportation behaviors in the electrode but can also partially compensate for the irreversible Li source consumption during SEI formation. Consequently, the cycling stability and initial coulombic efficiency of the Si-based electrodes with the PBDT binder are remarkably enhanced compared to that with the PVDF binder. This work demonstrates the molecular structure and prelithiation strategy of the polymer binder that play a crucial role in improving the performance of Si-based electrodes with high-volume expansion.

Solid Oxide Fuel Cells with Magnetron Sputtered Single-Layer SDC and Multilayer SDC/YSZ/SDC Electrolytes.

Samarium-doped ceria (SDC) is considered as an alternative electrolyte material for intermediate-temperature solid oxide fuel cells (IT-SOFCs) because its conductivity is higher than that of commonly used yttria-stabilized zirconia (YSZ). The paper compares the properties of anode-supported SOFCs with magnetron sputtered single-layer SDC and multilayer SDC/YSZ/SDC thin-film electrolyte, with the YSZ blocking layer 0.5, 1, and 1.5 μm thick. The thickness of the upper and lower SDC layers of the multilayer electrolyte are constant and amount to 3 and 1 μm, respectively. The thickness of single-layer SDC electrolyte is 5.5 μm. The SOFC performance is studied by measuring current-voltage characteristics and impedance spectra in the range of 500-800 °C. X-ray diffraction and scanning electron microscopy are used to investigate the structure of the deposited electrolyte and other fuel cell layers. SOFCs with the single-layer SDC electrolyte show the best performance at 650 °C. At this temperature, open circuit voltage and maximum power density are 0.8 V and 651 mW/cm2, respectively. The formation of the SDC electrolyte with the YSZ blocking layer improves the open circuit voltage up to 1.1 V and increases the maximum power density at the temperatures over 600 °C. It is shown that the optimal thickness of the YSZ blocking layer is 1 µm. The fuel cell with the multilayer SDC/YSZ/SDC electrolyte, with the layer thicknesses of 3/1/1 µm, has the maximum power density of 2263 and 1132 mW/cm2 at 800 and 650 °C, respectively.

Edge Graphitized Oxygen-Rich Carbon Based on Stainless Steel-Assisted High-energy Ball Milling for High-Capacity and Ultrafast Sodium Storage.

Oxygen doping is an effective strategy for constructing high-performance carbon anodes in Na ion batteries; however, current oxygen-doped carbons always exhibit low doping levels and high-defect surfaces, resulting in limited capacity improvement and low initial Coulombic efficiency (ICE). Herein, a stainless steel-assisted high-energy ball milling is exploited to achieve high-level oxygen doping (19.33%) in the carbon framework. The doped oxygen atoms exist dominantly in the form of carbon-oxygen double bonds, supplying sufficient Na storage sites through an addition reaction. More importantly, it is unexpected that the random carbon layers on the surface are reconstructed into a quasi-ordered arrangement by robust mechanical force, which is low-defect and favorable for suppressing the formation of thick solid electrolyte interfaces. As such, the obtained carbon presents a large reversible capacity of 363mAhg-1 with a high ICE up to 83.1%. In addition, owing to the surface-dominated capacity contribution, an ultrafast Na storage is achieved that the capacity remains 139mAhg-1 under a large current density of 100Ag-1 . Such good Na storage performance, especially outstanding rate capability, has rarely been achieved before.

Recent Achievements on the Liquid Electrolytes for Fast‐Charging Lithium Metal Batteries

Lithium metal batteries (LMBs) with fast‐charging capabilities can ease mileage anxiety, which is essential for the popularization of electric vehicles. However, the uncontrollable growth of Li dendrites and the repeated formation of electrode electrolyte interfaces lead to safety risks and low coulombic efficiency, which hinder the practical application of LMBs. Liquid electrolytes play an extremely important role in solving these problems. This review focuses on the recent achievements of liquid electrolytes for fast‐charging LMBs. The main factors limiting the fast transportation of Li ions are first introduced. The recent progress in electrolyte regulation for fast‐charging LMBs, including Li salts, electrolyte additives, and novel organic solvents, is summarized. Finally, a general conclusion and perspectives are proposed.

Lithium Phosphorus Sulfide Chloride-Polymer Composite via the Solution-Precipitation Process for Improving Stability toward Dendrite Formation of Li-Ion Solid Electrolyte.

Improving the mechanical strength of ceramic solid electrolytes such as lithium phosphorus sulfide families for pressure-driven dendrite blocking as well as reducing the electronic conductivity to prevent a dendrite formation inside the electrolytes are very important to extend the lifespan of all-solid-state lithium-metal batteries. Here, we propose a low-temperature solution-precipitation process to prepare polymer-solid electrolyte composites for a highly uniform polymer distribution in the electrolyte to enhance their mechanical strength and reduce their electronic conduction. The composites with up to 12 wt % of polymer are prepared, and the composites exhibit high ionic conductivities of up to 0.3 mS/cm. Furthermore, the electrochemical stability of the electrolyte composites on Li striping/plating cycles is investigated. We confirm that the proposed solution-precipitation process makes the composite much more stable than the bare solid electrolyte and causes them to outperform similar composites from the other existing preparation methods, such as mechanical mixing and solution dispersion.

Multifunctional electrolyte additive for realizing high-temperature and high-voltage lithium metal batteries.

Methyl 1H-1,2,4-triazole-3-carboxylate (MTC) was added into lithium metal batteries as an electrolyte additive, and not only did this addition lead to formation of solid electrolyte interfaces to protect both the anode and cathode, but the added MTC also served as a Lewis base in removing HF from the electrolyte to prevent the electrolyte from deteriorating. Therefore, the addition of MTC, in an appropriate amount, can be very effective at improving the electrochemical performance of lithium metal batteries.