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1.
    
Lithium-ion batteries have attracted much attention in the field like portable devices and electronic vehicles. Due to growing demands of energy storage systems, lithium metal batteries with higher energy density are promising candidates to replace lithium-ion batteries. However, using excess amounts of lithium can lower the energy density and cause safety risks. To solve these problems, it is crucial to use limited amount of lithium in lithium metal batteries to achieve higher utilization efficiency of lithium, higher energy density, and higher safety. The main reasons for the loss of active lithium are the side reactions between electrolyte and electrode, growth of lithium dendrites, and the volume change of electrode materials during the charge and discharge process. Based on these issues, much effort have been put to improve the utilization efficiency of lithium such as mitigating the side reactions, guiding the uniform lithium deposition, and increasing the adhesion between electrolyte and electrode. In this review, strategies for high utilization efficiency of lithium are presented. Moreover, the remaining challenges and the future perspectives on improving the utilization of lithium are also outlined.  相似文献   

2.
All-solid-state batteries (SSBs) represent one of the most promising avenues for surpassing the energy density limitations of conventional lithium-ion batteries. However, the unstable interfacial contact between the solid-state electrolyte and the electrode poses a critical challenge for practical applications. To tackle this issue, a hybrid system incorporating both liquid electrolytes (LEs) and sulfide solid-state electrolytes may serve as a viable alternative. In this hybrid system, the LE facilitates the in situ formation of a solid electrolyte interphase layer, thereby enhancing the physical interface contact. Consequently, the electrochemical lifetime of the hybrid all-SSBs is significantly improved, as evidenced by the stable lithium plating behavior observed through analytical techniques such as in situ X-ray imaging. Nonetheless, the hybrid system exhibits clear limitations, and several issues that need to be addressed for its practical implementation are identified. In conclusion, potential solutions that could be employed to overcome these challenges are proposed.  相似文献   

3.
    
Rechargeable Li-metal batteries (RLBs) can boost energy yet possess poor cycle stability and safety concerns when utilizing carbonate electrolytes. Countless effort has been invested in researching and developing electrolytes for RLBs to obtain stable and safe batteries. However, only few existing electrolytes meet the requirements for practical RLBs. In this perspective, the challenges of organic liquid electrolytes in the application in RLBs are summarized, and requirements for electrolytes for practical RLBs are proposed. This perspective briefly reviews the recent achievements of electrolytes (liquid- and solid-state) for RLBs and analyzes the corresponding drawbacks of each electrolyte. Further, possible solutions to the existing shortcomings of various electrolytes are proposed. In particular, this perspective outlines the development strategy of in situ gelation electrolytes, accompanied by a call for people using pouch cells to evaluate performance and paying more attention to battery safety research. This perspective aims to expound on the challenges and the possible research directions of RLBs electrolytes to promote practical RLBs better.  相似文献   

4.
    
All-solid-state batteries (ASSBs) are considered the ultimate next-generation rechargeable batteries due to their high safety and energy density. However, poor Li-ion kinetics caused by the inhomogeneous distribution of the solid electrolytes (SEs) and complex chemo-mechanical behaviors lead to poor electrochemical properties. In this study, LiNi0.8Co0.1Mn0.1O2 (NCM) (core) – Li6PS5Cl (LPSCl) SEs (shell) particles (NCM@LPSCl) are prepared by a facile mechano-fusion method to improve the electrochemical properties and increase the energy density of ASSBs. The conformally coated thin SEs layer on the surface of NCM enables homogeneous distribution of SEs in overall electrode and intimate physical contact with cathode material even under volume change of cathode material during cycling, which leads to the improvement in Li-ion kinetics without the increase in solid electrolyte content. As a result, an ASSBs employing NCM@LPSCl with 4 mAh cm−1 specific areal capacity exhibits robust electrochemical properties, including the improved reversible capacity (163.1 mAh g−1), cycle performance (90.0% after 100 cycles), and rate capability (discharge capacity of 152.69, 133.80, and 100.97 mAh g−1 at 0.1, 0.2, and 0.5 C). Notably, ASSBs employing NCM@LPSCl composite show reliable electrochemical properties with a high weight fraction of NCM (87.3 wt%) in the cathode.  相似文献   

5.
    
Current lithium (Li)-metal anodes are not sustainable for the mass production of future energy storage devices because they are inherently unsafe, expensive, and environmentally unfriendly. The anode-free concept, in which a current collector (CC) is directly used as the host to plate Li-metal, by using only the Li content coming from the positive electrode, could unlock the development of highly energy-dense and low-cost rechargeable batteries. Unfortunately, dead Li-metal forms during cycling, leading to a progressive and fast capacity loss. Therefore, the optimization of the CC/electrolyte interface and modifications of CC designs are key to producing highly efficient anode-free batteries with liquid and solid-state electrolytes. Lithiophilicity and electronic conductivity must be tuned to optimize the plating process of Li-metal. This review summarizes the recent progress and key findings in the CC design (e.g. 3D structures) and its interaction with electrolytes.  相似文献   

6.
    
Electrolytes play a pivotal role to determine the electrode performances in lithium-ion batteries (LIBs). However, understanding the function of electrolyte components at the molecular scale remains elusive (e.g., salts, solvents, and additives), particularly how they arrange themselves and affect properties of the bulk, liquid-solid interfaces, and electrolyte decomposition, rendering a bottleneck for improving the electrolytes. Herein, the function of electrolyte components is thoroughly studied, from Li+ solvation structure in the bulk electrolyte, Li+ (de-)solvation behaviors at the electrolyte-solid interfaces, until the formation of solid electrolyte interphase (i.e., SEI) layer on the electrodes. Furthermore, a detailed model by taking into account the effects of solvent, additive, lithium salt, and concentration on the electrochemical properties of the Li+-solvent-anion complex to elucidate the electrode performances are depicted. As the ultimate benefit of this study, a completely new non-flammable ether-based electrolyte and stabilizing the promising antimony (Sb) anodes can be designed. Remarkably, a high-performance Sb anode that is superior to previous reports is obtained. This study provides a graphical model to unravel interfacial and interphasial behaviors of electrolyte components in LIBs, which is also significant for developing other metal-ion batteries.  相似文献   

7.
    
Anatase TiO2 is considered as one of the promising anodes for sodium‐ion batteries because of its large sodium storage capacities with potentially low cost. However, the precise reaction mechanisms and the interplay between surface properties and electrochemical performance are still not elucidated. Using multimethod analyses, it is herein demonstrated that the TiO2 electrode undergoes amorphization during the first sodiation and the amorphous phase exhibits pseudocapacitive sodium storage behaviors in subsequent cycles. It is also shown that the pseudocapacitive sodium storage performance is sensitive to the nature of solid electrolyte interphase (SEI) layers. For the first time, it is found that ether‐based electrolytes enable the formation of thin (≈2.5 nm) and robust SEI layers, in contrast to the thick (≈10 nm) and growing SEI from conventional carbonate‐based electrolytes. First principle calculations suggest that the higher lowest unoccupied molecular orbital energies of ether solvents/ion complexes are responsible for the difference. TiO2 electrodes in ether‐based electrolyte present an impressive capacity of 192 mAh g?1 at 0.1 A g?1 after 500 cycles, much higher than that in carbonate‐based electrolyte. This work offers the clarified picture of electrochemical sodiation mechanisms of anatase TiO2 and guides on strategies about interfacial control for high performance anodes.  相似文献   

8.
    
The practical application of lithium (Li) metal battery is impeded by the Li dendrite growth and unstable solid electrolyte interphase (SEI) layer. Herein, an ultra-stretchable and ionic conducting chemically crosslinked pressure-sensitive adhesive (cPSA) synthesized via the copolymerization of 2-ethylhexyl acrylate and acrylic acid with poly(ethyleneglycol)dimethacrylate as crosslinker (short for 70cPSA), is developed as both artificial SEI layer and solid polymer electrolyte (SPE) for stable Li-metal electrode, enabling all-solid-state Li metal batteries with excellent cycling performance. As an artificial SEI layer, the 70cPSA-modified electrodes exhibit excellent electrochemical performance in Li|70cPSA@Cu half cells and 70cPSA@Li|70cPSA@Li symmetric cells. In full cells with LiFePO4 (LFP) as cathode, the 70cPSA@Li|LFP cell exhibits stable cycling performance over 250 cycles. Utilized as SPE, the all-solid-state Li|SPE|LFP cell delivers excellent cycling stability with a capacity retention of 86% over 500 cycles. With high-voltage LiNi0.8Mn0.1Co0.1O2 (NMC811) as cathode, the Li|SPE|NMC811 cell exhibits a discharge capacity of 124.3 mAh g−1 with a capacity retention of 71% after 200 cycles. The rational design of PSAs and investigation of their dual role for stable and safe Li-metal batteries may shed a light on adhesive polymers for battery applications.  相似文献   

9.
    
The surface chemistry of garnet electrolyte is sensitive to air exposure. The poor LLZO/Li interface caused by Li2CO3/LiOH contaminants on garnet electrolyte surface easily induces large interfacial resistance resulting in the growth of Li dendrites. Herein, a versatile modification strategy is designed to convert the contaminants on Li6.4La3Zr1.4Ta0.6O12 (LLZTO) surface into a LiF and Li2PO3F-rich lithiophilic interface by targeted chemical reactions at the interface between LiPO2F2 and Li2CO3/LiOH. The newly formed LiF-Li2PO3F interfacial layer not only facilitates the interface wettability between Li and LLZTO, but also helps to resist corrosion of the LLZTO surface by moisture in the air. The Li|LiF&Li2PO3F-LLZTO|Li symmetric cell exhibits a low interfacial resistance of 5.1 Ω cm2 and ultrastable galvanostatic cycling, over 1500 h at 0.6 mA cm−2 and over 70 h at 1.0 mA cm−2. In addition, LiCoO2|LiF&Li2PO3F-LLZTO|Li hybrid solid-state full cells display high initial specific capacity of 192 mAh g−1 at 0.1 C, and excellent cycling stability with a capacity retention over 76% even after 1000 cycles at 0.5 C at a high cut-off voltage of 4.5 V. This study provides a simple and practical strategy for the feasibility of the application of high-voltage cathodes in this modified garnet all-solid-state batteries.  相似文献   

10.
    
Potassium-ion batteries (KIBs) are considered as the potential energy storage devices due to the abundant reserves and low cost of potassium. In the past decade, research on KIBs has generally focused on electrode materials. However, since electrolytes also play a key role in determining the cell performance, this review summarizes recent advances in KIB electrolytes and design strategies. Specifically, the review includes five parts. First, the organic liquid electrolyte is the most widely used type for KIBs. Its two major components, salts and solvents, have a huge impact on the formation of the solid electrolyte interphase and the performance of KIBs. Changes in salts/solvents, the introduction of additives, and the concentration increase all have a positive effect on organic liquid electrolytes. Second, the design of water-in-salt electrolytes can effectively widen the narrow electrochemical stability window of aqueous electrolytes. Third, despite the appealing properties, the ionic liquid electrolytes have not been widely applied due to its high cost. Fourth, the solid-state electrolytes have drawn much attention due to high safety, and current research has been working on improving their ionic conductivity at room temperature. Lastly, perspectives are provided to support the future development of suitable electrolytes for high-performance KIBs.  相似文献   

11.
    
Poly(ethylene oxide) (PEO)-based solid polymer electrolyte promises interfacial compatibility with the high-capacity metallic anodes in all-solid-state batteries (ASSBs). However, the prototype construction is severely hindered by the parasitic ohmic resistance at the electrode-electrolyte interface, insufficient ionic pathway of the high loading cathode, as well as the PEO oxidation tendency at the high voltage. Herein, a laser-assisted strategy is presented toward ultra-efficient cathode modification (completes within 240 s) by constructing continuous, multi-scale artificial cathode/electrolyte interface (CEI). The tailorable, yet localized temperature gradient induced by the pulsed laser beam can customize the CEI species from the target precursor salts for the on-demand protection purpose. Derived from the tris(trimethylsilyl)phosphate, the proof-of-concept model achieves phosphorus-rich, ion-diffusion network across the high-mass-loading LiNi0.8Co0.1Mn0.1O2 cathode, which enables the high-rate operation of the ASSBs prototype as well as the extended shelf life at the oxidized idling state. Transmission-mode operando X-ray phase tracking unravels the electrochemical stability origin at the cathode/PEO interface due to the insulation of electron shuttling, where the layered to spinel phase transition and the lattice oxygen release are alleviated. This generic, readily tailorable, highly-efficient laser processing strategy thus provides unprecedented opportunities to secure the varieties of energy-dense, polymer-based ASSBs.  相似文献   

12.
Solid-state batteries (SSBs) with addition of liquid electrolytes are considered to possibly replace the current lithium-ion batteries (LIBs) because they combine the advantages of benign interfacial contact and strong barriers for unwanted redox shuttles. However, solid electrolyte and liquid electrolyte are generally (electro)-chemically incompatible and the resistance of the newly formed solid–liquid electrolyte interphase (SLEI) appears as an additional contribution to the overall battery resistance. Herein, a boron, fluorine-donating liquid electrolyte (B, F-LE) is introduced into the interface between the high-voltage cathode and ultrathin composite solid electrolyte (CSE), which is fabricated by adhering a high content of nanosized Li6.4La3Zr1.4Ta0.6O12 (LLZTO) with poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), to generate a low resistance and high stable SLEI in situ, giving a stable high-voltage output with a reinforced cathode|CSE interface. B, F-LE, consisting of a highly fluorinated electrolyte with a lithium bis(oxalato)borate additive, exhibits good chemical compatibility with CSE and enables rapid and uniform transportation of Li+, with its electrochemically and chemically stable interface for high-voltage cathode. Eventually, the B, F-LE assisted LiNi0.6Co0.2Mn0.2O2|Li battery displays the enhanced rate capability and high voltage cycling stability. The findings provide an interfacial engineering strategy to turn SLEI from a “real culprit” into the “savior” that may pave a brand-new way to manipulate SLEI chemistry in hybrid solid–liquid devices.  相似文献   

13.
    
Lithium metal batteries (LMBs) working at subzero temperatures are plagued by severe restrictions from the increased energy barrier of Li-ion migration and desolvation. Herein, a competitive coordination strategy based on the ternary-anion (TA) coupling of PF6, TFSI, and NO3 toward Li+ to achieve an anti-freezing electrolyte with rapid kinetics is proposed. Computational and spectroscopic analyses reveal that the repulsive interaction among three anions and the preponderant coordination of the Li+-NO3 further weaken the involvement degree of other anions in the Li+ solvation structure. As a result, the formulated TA electrolyte exhibits low binding energy of Li+-anions (−4.62 eV), Li+ desolvation energy (17.04 kJ mol−1), and high ionic conductivity (3.39 mS cm−1 at −60 °C), simultaneously promoting anion-derived solid electrolyte interphase on Li anode. Assembled Li||LiNi0.8Co0.1Mn0.1O2 cells employing the TA electrolyte exhibit robust capacity retention of 86.74% over 200 cycles at 25 °C and deliver a specific cathode capacity of 103.85 mAh g−1 at −60 °C. This study will enlighten the rational design of multi-anion electrolytes to tailor the Li+ solvation/desolvation for advanced low-temperature LMBs.  相似文献   

14.
    
Polymer blends based solid polymer electrolytes (SPEs), combining the advantages of multiple polymers, are promising for the utilization of 5 V-class cathodes (e.g., LiCoMnO4 (LCMO)) with enhanced safety. However, severe macro-phase separation with defects and voids in polymer blends restrict the electrochemical stability and ionic migration of SPEs. Herein, inorganic compatibilizer polyacrylonitrile grafted MXene (MXene-g-PAN) is exploited to improve the miscibility of the poly(vinylidene fluoride-co-hexafluoropropylene) (PVHF)/PAN blends and suppress the consolidation of phase particles. The resulting SPE exhibits a high anodic stability with an ionic conductivity of 2.17 × 10−4 S cm−1, enabling a stable and reversible Li platting/stripping (over 2500 h). The fabricated solid Li‖LCMO cell delivers a 5.1 V discharge voltage with a decent capacity (131 mAh g−1) and cycling performance. Subsequently, the solid all-in-one graphite‖LCMO battery is also constructed to extend the application of MXene based SPEs in flexible batteries. Benefiting from the interface-less design, outstanding mechanical flexibility and stability is achieved in the battery, which can endure various deformations with a low-capacity loss (< ≈10%). This study signifies a significant development on solid flexible lithium ion batteries with enhanced performance, stability, and reliability by investigating the miscibility of polymer blends, benefiting for the design of high-performance SPEs.  相似文献   

15.
    
Lithium metal (LM) is a promising anode material for next generation lithium ion based electrochemical energy storage devices. Critical issues of unstable solid electrolyte interphases (SEIs) and dendrite growth however still impede its practical applications. Herein, a composite gel polymer electrolyte (GPE), formed through in situ polymerization of pentaerythritol tetraacrylate with fumed silica fillers, is developed to achieve high performance lithium metal batteries (LMBs). As evidenced theoretically and experimentally, the presence of SiO2 not only accelerates Li+ transport but also regulates Li+ solvation sheath structures, thus facilitating fast kinetics and formation of stable LiF-rich interphase and achieving uniform Li depositions to suppress Li dendrite growth. The composite GPE-based Li||Cu half-cells and Li||Li symmetrical cells display high Coulombic efficiency (CE) of 90.3% after 450 cycles and maintain stability over 960 h at 3 mA cm−2 and 3 mAh cm−2, respectively. In addition, Li||LiFePO4 full-cells with a LM anode of limited Li supply of 4 mAh cm−2 achieve capacity retention of 68.5% after 700 cycles at 0.5 C (1 C = 170 mA g−1). Especially, when further applied in anode-free LMBs, the carbon cloth||LiFePO4 full-cell exhibits excellent cycling stability with an average CE of 99.94% and capacity retention of 90.3% at the 160th cycle at 0.5 C.  相似文献   

16.
    
On‐board vehicle applications dictate the need for improved low‐temperature power densities of rechargeable batteries. Integration of high‐permittivity artificial dielectric solid electrolyte interfaces (SEIs) into the lithium ion battery architecture is a promising path to satisfy this need. The relationship between the permittivity of various artificial dielectric SEIs and the resulting high‐rate capability at low temperatures is investigated. Room‐temperature studies reveal a weak relationship between these variables. However, at low temperatures, the correlation between the larger permittivity of the dielectric SEIs and the greater high‐rate capabilities of the cells is striking. The high‐rate capabilities for pulsed laser deposition‐synthesized cathode thin films with various BaTiO3 (BTO) SEIs covering configurations are evaluated. A remarkable improvement in the high‐rate capability is observed for LiCoO2 (LCO) modified with dot BTOs, while the rate capability for planar BTO (fully covered LCO) is weakened significantly. A series of experimental results prove that a large polarization, P, in the dielectric SEIs intensified with permittivity accelerates interfacial charge transfer near the dielectrics–LCO–electrolyte triple junction.  相似文献   

17.
    
Solid-state lithium metal batteries (SSLMBs) are a promising candidate for next-generation energy storage systems due to their intrinsic safety and high energy density. However, they still suffer from poor interfacial stability, which can incur high interfacial resistance and insufficient cycle lifespan. Herein, a novel poly(vinylidene fluoride‑hexafuoropropylene)-based polymer electrolyte (PPE) with LiBF4 and propylene carbonate plasticizer is developed, which has a high room-temperature ionic conductivity up to 1.15 × 10−3 S cm−1 and excellent interfacial stability. Benefitting from the stable interphase, the PPE-based symmetric cell can operate for over 1000 h. By virtue of cryogenic transmission electron microscopy (Cryo-TEM) characterization, the high interfacial compatibility between Li metal anode and PPE is revealed. The solid electrolyte interphase is made up of an amorphous outer layer that can keep intimate contact with PPE and an inner Li2O-dominated layer that can protect Li from continuous side reactions during battery cycling. A LiF-rich transition layer is also discovered in the region of PPE close to Li metal anode. The feasibility of investigating interphases in polymer-based solid-state batteries via Cryo-TEM techniques is demonstrated, which can be widely employed in future to rationalize the correlation between solid-state electrolytes and battery performance from ultrafine interfacial structures.  相似文献   

18.
    
Concerning the safety aspects of Li+ ion batteries, an epoxy-reinforced thin ceramic film (ERTCF) is prepared by firing and sintering a slurry-casted composite powder film. The ERTCF is composed of Li+ ion conduction channels and is made of high amounts of sintered ceramic Li1+xTi2-xAlx(PO4)3 (LATP) and epoxy polymer with enhanced mechanical properties for solid-state batteries. The 2D and 3D characterizations are conducted not only for showing continuous Li+ ion channels thorough LATP ceramic channels with over 10−4 S cm−1 of ionic conductivity but also to investigate small amounts of epoxy polymer with enhanced mechanical properties. Solid-state Li+ ion cells are fabricated using the ERTCF and they show initial charge–discharge capacities of 139/133 mAh g−1. Furthermore, the scope of the ERTCF is expanded to high-voltage (>8 V) solid-state Li+ ion batteries through a bipolar stacked cell design. Hence, it is expected that the present investigation will significantly contribute in the preparation of the next generation reinforced thin ceramic film electrolytes for high-voltage solid-state batteries.  相似文献   

19.
For a variety of purposes, solid electrolytes with high ionic conductivity are believed to be an alternative to widely used liquid electrolytes. Most of them are developed based on the exploration of crystalline or amorphous structures. As a very rare example of the beneficial influence of glass/ceramic interfaces, we report the conductivity of LiF films on SiO2. The LiF thin films are surprisingly found to be structurally disordered on the silica (0001) surface, leading to a remarkable enhancement of the Li‐ion conductivity (6 × 10?6 S cm?1 at 50 °C, with an activation energy of 0.55 eV) of three orders of magnitude. The resulting conductivity is not exceedingly high, but is comparable with that of the current, best thin‐film solid electrolyte (Li(3 + x)PO(4 ‐ x)Nx). The conductivity is highest if a significant density of glass/ceramic interfaces is achieved and percolation of the interfaces guaranteed.  相似文献   

20.
    
Aqueous zinc metal batteries are safe, economic, and environmentally friendly. However, the dendrite growth and inevitable corrosion issues under aqueous condition greatly restrict the development of long cycling life zinc metal batteries. To achieve the long‐term reversible zinc deposition/dissolution, a polyzwitterionic hydrogel electrolyte (PZHE) is constructed with record high room temperature ionic conductivity of 32.0 mS cm?1 and Zn2+ transference number of 0.656. The abundant hydrophilic and charged groups in the zwitterionic polymer can well immobilize water molecules in the polymer skeleton and reduce side reactions. The charged groups of the zwitterionic polymer can also homogenize the ion distribution and achieve uniform zinc deposition. Long cycling life of over 3500 h is achieved for the symmetric batteries with PZHE. Full cells with VS2 and MnO2 cathodes are also demonstrated to exhibit excellent cycling stability. With combined advantages of physical and chemical crosslinking gels, the PZHE enabled flexible quasi‐solid state zinc metal batteries with excellent processability, self‐healing property and safety, can operate even under various extreme conditions such as cutting, soaking, hammering, washing, burning, and freezing. It is believed that the PZHE can provide a promising opportunity and pave the way for other long‐life aqueous batteries.  相似文献   

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